An Integrated Vision of The Green Chemistry Evolution Along 25 Years Marques - Machado

Foundations of Chemistry (2021) 23:299–328
https://doi.org/10.1007/s10698-021-09396-6
An integrated vision of the Green Chemistry evolution

along 25 years
Carlos Alberto Marques1 · Adelio A. S. C. Machado2
Accepted: 12 January 2021 / Published online: 18 June 2021

© The Author(s), under exclusive licence to Springer Nature B.V. 2021
Abstract
The objective of the present review on the evolution of Green Chemistry (GC), since its
emergence until 2016 (25th anniversary), aimed an integrated vision of its progress along
the three phases of its development: emergence, divulgation and consolidation. The meth‑
odology involved the analysis of a selection of bibliography on the evolution of GC col‑
lected from issues of the ACS symposia series; editorials in specialized GC journals; and
commemorative birthday papers/editorials of these journals and of the GC itself. The anal‑
ysis allowed to identify and discuss the characteristics and conceptions of GC agents about
fundamental concepts and procedures, in order to visualize and better understand the state
of knowledge and the subject areas that make up the field. The main alterations identi‑
fied in the evolution of GC were: it acquired a better defined identity, with more participa‑
tion of academy and increased scope; was progressively framed in sustainability; has been
aspiring to a holistic frame (but it is still dominated by its original reductionism) and to a
change on the nature of the innovation for its implementation, from incremental to trans‑
formative. The analysis suggests that for supporting expansion and consolidation of GC
the following aspects deserve attention: full validation of chemical greenness by metrics;
better characterization of the frontiers of GC research areas/themes; increased integration
between academy and industry; and penetration in chemistry curricula. Its basic philoso‑
phy being the practice of a chemistry more focused on the environment preservation, GC
means a new stage in nature and in the history of Chemistry.
Keyword Green Chemistry · GC evolution · GC innovation nature · GC integrated vision ·

Systemic science · Sustainability
* Carlos Alberto Marques

carlos.marques@ufsc.br
Adelio A. S. C. Machado
amachado@fc.up.pt
1
Departamento de Metodologia de Ensino and Programa de Pós‑Graduação em Educação Científica
e Tecnológica, Universidade Federal de Santa Catarina, Florianópolis, SC, Brazil
2
Departamento de Química e Bioquímica, Faculdade de Ciências da Universidade do Porto, Porto,
Portugal
13
Vol.:(0123456789)
300 C. A. Marques, A. A. S. C. Machado
Introduction
The emergence of Green Chemistry1 (GC) is a landmark for Chemistry in the context of
progress towards environmental sustainability (Clark 2003; Grassian and Meyer 2007;
Anastas 2011; Logar 2011; IUPAC 2017) and represents a proactive response to the nega‑
tive image of Chemistry, strongly stressed in the Brundtland Report (WCED 1987). GC is
an increasing field of academic and industrial research and innovation, with strong empha‑
sis in environmental prevention, where Chemistry can find solutions for problems caused
by the manufacturing processes and use of chemical products. Therefore, GC express ethi‑
cal and political compromises with the environment and sustainability. These are subjected
to increasing emphasis at present and involve not only the Chemistry but also other basic
sciences as well as technologies.
From the birth of GC at the early nineties of last century, the adhesion of chemists and
the reports mentioning a greener or cleaner chemistry from academy and industry have
increased, GC bringing new knowledge with traditional Chemistry as a departure point.
An increasing number of publications in journals, both new journals specialized in GC
and more traditional journals of different areas of chemistry, as well as interactions in con‑
gresses and networks, prompts already an increasing acknowledgment of an international
community of green chemists.
Since GC inception, along its 25 years commemorated in 2016, the initial ideas formu‑
lated by its precursors, general principles and main subjects have been evolving through
different stages. Therefore, the characterization (concept and identity) of GC has been
changing with its growth. Reviews from several institutions and members of the commu‑
nity, performed at different moments and with different scopes, have dealt with this theme
(Amato 1993; Collins 1997; Poliakoff and Anastas 2001; Thornton 2001; Winterton 2003;
Warner et al. 2004; Woodhouse and Breyman 2005; Kidwai and Mohan 2005; Poliakoff
and Licence 2007; Dichiarante et al. 2010; Linthorst 2010; Logar 2011). This literature
suggests that GC: (a) is a research field within Chemistry, searching for innovative solutions
for negative impacts in the environmental crises context; (b) has incorporated scientific
productions from different traditional areas of Chemistry; (c) has acquired progressively a
worldwide comprehensiveness, with increasing numbers of journals and specialized pub‑
lications, as well as of professional chemists involved; (d) has been expressed as an inter‑
disciplinary field, focussed on environmental prevention; and (e) should be developed with
a systems thinking mindset, as suggested by Graedel (2001). Having this in mind, as well
as the growing of its academic production, GC activity requires a deeper and permanent
monitoring to allow the identification and mapping of its features and its agent’s ideas on
fundamental concepts and procedures for comprehension of the state of knowledge and
definition of areas. This is complex and requires a more systemic and rational treatment,
therefore less disperse, than in fragmented scope analysis. This situation prompted the
more global treatment presented in this study, which is addressed to the GC community—
and other partners interested in its discussion, practice and teaching.
Therefore, the broad objective of the present study is to examine the tendencies of GC
evolution using available bibliography on the moments and phases that mark its devel‑
opment, specifically: several issues of the ACS Symposium Series (ACS SS), the scarce
1
Anastas and Warner (1998, p. 11) defined GC as: “… the utilization of a set of principles that reduces
or eliminates the use or generation of hazardous substances in the design, manufacture and application of
chemical products”.
13
An integrated vision of the Green Chemistry evolution along 25 years 301
papers published in the first few years after the concept emerged, editorials in specialized
GC journals, and commemorative birthday papers/editorials of these journals and of the
GC itself. More precisely, our objectives were: (a) to find the main lines of GC develop‑
ment, detecting and commenting recurrences of basic ideas, as well as absences, difficulties
and challenges to the GC implementation; (b) to search for evidence on connections with
the theme of sustainability; (c) to follow the adoption of a holistic view (systems thinking)
for GC practice; and (d) to discuss the importance given in the literature on the validation
of the GC green efficacy. In summary, to offer a more integrated and holistic vision of the
GC evolution.
Our research used the method of documental analysis, with inventorial and exploratory
characteristics, based on study of the contents of the texts—especially texts with academic
origin and those of GC precursors—along a historical pathway. Therefore, their read‑
ing was included in the analytical treatment and provided support to the discussions and
conclusions about the theme. In some stages, searches of “signal-words” (Chen and Xiao
2016) in the texts were used for obtaining trails of the presence of significant contents/con‑
cepts (for instance, the signal-word sustainability).
With respect to the different periods or phases of GC, Linthorst (2010) used the follow‑
ing division: the first period referred to the origins of GC within US EPA until 1993; the
second (1993–1998), to the activity focussed on Pollution Prevention (P2) in the expanding
network around EPA, ending with the publication of the Twelve Principles in the anchor
book of GC (Anastas e Warner 1998, in this text abbreviated to A&W, 1998); finally, the
third (1999–2008) meant GC steady growth, shown by the increase of the number of jour‑
nals/papers (Linthorst 2010, Fig. 2, p. 63). In the present study, we merged the Linthorst
two first periods, both centered in EPA activities, in a unique phase (Emergence phase),
that closes with the publication of the Twelve Principles. The second phase (Divulgation
phase) started with the launching of the journal Green Chemistry (GCJ) (Clark 1999a) and
includes near the end the launching of the second journal with a stated connection to GC
in the title, Green Chemistry Letters and Reviews (GCL&R) (Warner 2007; Anastas 2007).
The third phase (Consolidation2 phase) starts with the commemoration by the CGJ of its
ten years, with an editorial (Poliakoff and Leitner 2008) as well as a set of reviews on dif‑
ferent themes. Some of these were important for our work, because they constituted first
efforts of analysis of the evolution of GC themes, therefore supporting the purpose of the
present text. This phase extends to the present, with emphasis to the commemoration of the
25 years of GC. This division is presented in Fig. 1 (see below).
The structure of the paper is as follows: (1) This introduction; (2) Emergence phase; (3)
Divulgation phase; (4) Consolidation phase; (5) Discussion; and 6) Conclusions. Figure 1
shows the route of our study, providing a panorama of the emergence and evolution of GC.
The line of the figure is the time-line, the dotted line referring to the time range where
the control legislation on environmental impacts and chemical studies on pollution, envi‑
ronment, etc. provided the base for emergence of GC (Machado 2011). This range ended
with the US Pollution Prevention Act (PPA) (US 1990). To the right the Emergence,
Divulgation and Consolidation phases of GC evolution, as discussed below, are shown.
The arrow BbDCh refers to the initial period before the name “Green Chemistry” was
coined. The arrows GC-SD indicate the acknowledgement of the integration of GC to SD.
The transitions between phases, represented by ellipses, are respectively: publication of the
2
The word consolidation is not used here meaning stability or mature science, but rather acknowledgement
by the whole area of Chemistry (Howard-Grenville et al. 2017).
13
Fig. 1 GC evolution: from emergence to 25 yearsPPA/US: Pollution Prevention Act (USA 1990); BbDCh:
benign by design chemistry
Fig. 2 Evolution of GC and
challenges and limitations (in the
cloud) along its first 25 years
Twelve Principles and the launching of GCJ; the launching of GCL&R and commemora‑
tion of the tenth birthday of GCJ. The publication times of the ACS SS addressed to GC
are also included. Further details of the figure are discussed along the text.
The Emergence phase
To acquire information on the initial development of the field, then not yet called GC, we
reviewed the scarce bibliography on its presentation constituted mainly by some books of
proceedings published in the ACS SS.
The PPA (US 1990) was crucial for the GC emergence. This legislation meant an impor‑
tant change on the way environmental problems were dealt with in the North American
context. The PPA involved a new paradigm for supporting the minimization of chemical
wastes by proactive prevention of their formation which replaced the end-of-life reactive
13
treatment and elimination of wastes (based on the risk paradigm). PPA required suitable
design of syntheses or processes but involved no regulatory legislation, allowing overall
changes in the processes to improve their technical and economic performance in parallel
with the waste elimination—an indispensable item to attract the entrepreneurs. This new
paradigm meant a new ethics for P2 and since then acquired a dominant role in shaping the
North American environmental policy on pollution, followed by environmentalists, indus‑
trialists, legislators, policy makers, academics and the public at large (Breen and Dellarco
1992; Browner 1993), as recently reaffirmed (US EPA 2015, p. 1). P2 was the driving force
of several ACS symposia on GC, which influenced its initial development and route until
the presentation of the Twelve Principles (A&W 1998).
The report ACS SS 577, titled “Benign by Design: Alternative Synthetic Design for
Pollution Prevention” (Anastas and Farris 1994), constituted the formal presentation of GC
in the published literature—it reported a new style of synthetic chemistry designed to pro‑
duce non-hazardous (or less hazardous) compounds. This was a new challenge begging for
the development of alternative synthetic pathways with production of less residues—a pro‑
phylactic type of chemistry, similar to the preventive medicine (idem, Preface, p. ix). The
designation “Green Chemistry” was not used in this report, except in an “In Memoriam”
dedicated to Kenneth G. Hancock included ad hoc in the introduction (p. xi). In Chapter 1,
Anastas presented an overall view of Benign by Design Chemistry (BbDCh), stressing the
importance of new synthetic methodologies for the resolution of the residues pollution
included) problem. The design of novel synthetic procedures for the purpose of minimiz‑
ing residues involved three factors: efficiency, economic viability and environmental benig‑
nity (p. 10). A non-exhaustive list of themes dealt with in different BbDCh research lines
was included (pp. 19–20). In Chapter 2, Hancock e Cavanaugh discussed the importance
of this new way of practicing chemistry in the broader context of economic development
and environmental sustainability. These texts included no clear characterization of GC or
green synthesis as a field, although all the chapters discussed different aspects of synthetic
benignity. With reference to the designation, if the term “benign by design chemistry” is
substituted by “Green Chemistry” in the texts of both chapters their meaning is not altered,
thus it can be inferred that the now intensively used term “Green Chemistry” was shaped
in period.
In ACS SS 626 (Anastas and Williamson 1996, p. 1), the designation GC was used
prominently, although in Chapter 1 Anastas mentioned several other alternatives relating
chemistry and environment (Environmentally Benign Chemistry, Clean Chemistry, Atom
Economy and BbDCh). “General principles” of a greener chemistry were mentioned with
no details, although interestingly Atom Economy (Trost 1991) was presented as a gen‑
eral base for the principles (p. 13). Like in the previous ACS SS 577, all other chapters
described research on synthesis.
In ACC SS 640 (DeVitto and Garrett 1996), which complemented the previous report,
the editors referred that beside benign synthetic routes, the design of benign chemical sub‑
stances was important in BbDCh as a “sister concept” of benign routes. Thus, the design
of molecules of new compounds aiming the proactive elimination of the toxicity was
contemplated in this volume (p. vii). In Chapter 1 (p. 2), Garrett discussed more clearly
the connection among PPA, GC and the Design of Safe Chemicals. After presenting the
context in which PPA emerged and the hierarchisation of P2 activities (source prevention,
source reduction, recycling, treatment and deposition), source prevention was pointed as
the “supreme aim” of P2 (p. 5). This concept served as departure point of several pro‑
grams developed by EPA addressed to “the reduction or elimination of the toxic chemicals
through fundamental changes in the field of chemistry” (p. 5). Thus, the purpose and broad
13
dimension of GC was presented more clearly, giving full emphases to the importance of
reformulation of synthetic pathways, which required basic research and amplification of
knowledge.
In this Emergence phase, only a reduced number of papers addressed to analysis of GC
was found. Anastas and Breen (1997), when discussing the connection between Industrial
Ecology and GC, stressed the importance of the design in GC, as well as of the adoption
of a systemic mindset. To establish a bridge between GC and the Design for Environmen‑
tal (DfE) for the implementation of Industrial Ecology, GC was considered a "technologic
pull” and DfE a “technologic push”. In Industrial Ecology, DfE and GC are “the heart and
soul of the emerging sustainability science” (as expressed in Fig. 1 of the paper, p. 97).
However, subsequently, this type of analogy and the GC-DfE bridge were never mentioned
again by the authors. On the other hand, the Industrial Ecology analysis ignores the differ‑
ence between objects in general and chemical products in particular. A substantial part of
chemicals is used destructively and/or dispersedly and therefore lost in the environment,
which prevents recycling as prescribed by Industrial Ecology. In summary, the bridge
between DfE and GC involves limitations.
Along another line, Amato (1993) and Collins (1995, 1997) presented a more systemic
vision of the features of the rising GC. In a divulgation paper with some new points of
view on the field, Amato (1993) used the name GC for the first time in scientific jour‑
nals. This use may have influenced the change of name from benign chemistry to GC men‑
tioned above. Sustainable development (SD) was pointed as one of the driving forces of
GC (p. 1539) and the increasing efforts of the Chemical Industry in the implementation
of processes for preventive protection of environment, which required large investments,
were also acknowledged (p. 1539, box). Moreover, the role of recycling in reducing wastes
and the consumption of natural resources was mentioned—this meant a connection of GC
with Industrial Ecology, although no express mention to such connection was included.
The diversification of Environmental Chemistry, primitively only analytical chemistry of
pollution, as a consequence of the recognition by chemists of the impact of chemistry on
environment, was also discussed (p. 1540). However, the term “slow birth” in the title sug‑
gests that the author felt the existence of barriers to GC development. On the other hand,
Amato reaffirmed the contents of ACS SS 577 and 626 on several items: launching of GC
in EPA; industrial residues as a strong economic driving force that pressed the P2 emer‑
gence; importance of the design to reshape industrial syntheses; and relevance of the elimi‑
nation of toxicity in industrial products and reagents used in their manufacture (p. 1541,
box). Globally, Amato´s view of the rising GC seems to contain a more systemic approach
than that in the ACS SS books.
In what was the first paper on GC published in the Journal of Chemical Education,
Collins (1995) described a university GC course at introductory level. Interestingly, GC
was presented as a hypothesis because chemical processes with negative impacts may be
replaced by non-pollutant alternatives, as already verified in several important cases (p.
965), but is not always feasible. The strength of ethical and political components contained
in the GC idea for dealing with environmental problems was stressed. GC principles were
mentioned generically without detailing, but expressing the opinion that their materializa‑
tion requires a long term effort (see Discussion below). The connection of GC to Chemis‑
try was considered important because the scientific base of chemistry has to be preserved
and the functions of chemical compounds in their utilization cannot be jeopardized by GC.
In another paper (Collins 1997), in which texts in ACS SS 577 626 were revisited, the
connection between GC and SD was mentioned (p. 691). Interestingly, principles that may
serve as GC fundaments were specified, three examples of generic nature and broad scope
13
being presented: (1) Genuine GC is designed to eliminate pollution at source, therefore its
objective”is never to imperil beneficial life forms” (p. 693); (2) The production of chemical
knowledge is obtained from different fields, which requires more attention to training of
green chemists; moreover, because environment is a complex chemical system involving
multidisciplinary knowledge, GC requires collaboration between different specialties, par‑
ticularly between academic and industrial partners, requiring flexibility in both fields; (3)
In GC research projects it is necessary to pay attention to the time scale, because environ‑
ment complexity requires long-term instead of short term views, implying modifications in
the strategy and the evaluation criteria of the projects. In summary, Collins (1997) intro‑
duced a different vision of GC, including awareness of its limitations, which contrasts with
the more idealistic GC suggested by the Twelve Principles presented a year later (A&W
1998).
The analysis of texts published in this period of genesis of the Twelve Principles aimed
the identification of elements that allowed the GC characterization and the definition of
items in its content, with the purpose of their systemization. Therefore, absences and/or
recurrences in this Emergence phase of elements that later deserved attention and were
integrated in GC were searched. For this purpose, the following “signal-words” were used:
principle(s), sustain(ability)/sustainable development, metric(s), life(cycle), molecular
design, product/process design, innovat(ion), prevent(ion)/P2, cohes(ive) and system.3
However, the diffuse nature of some of these elements and the variability of language used
for their naming in this Emergence phase may affect the scope and robustness of this pro‑
cedure in some situations.
The results of this analysis showed that only the concepts of design (of product or pro‑
cess) and of prevention/P2 were clearly present in the Emergence phase. Molecular design
and life-cycle were rarely found, while only generic and weak references were found to
sustainability/SD, innovation and general principles of GC (without specification and/
or enunciation). Finally, no reference at all of a holistic view of GC was found (“signal-
words”: cohesive and system).
The final landmark of the Emergence phase was the publication of the anchor book of
GC (A&W 1998) with the Twelve Principles (in Chapter 4)—a body of ethical values for
guiding scientific procedures and lines in the implementation of a benign chemistry, which
acquired a strong and long lasting importance in GC diffusion. The focus of the text was
on industrial wastes, as in the previous ACS SS 577 and 626, stressing the importance
of reshaping synthetic chemistry towards BbDCh for intentional elimination of wastes
(pp. 9–10). On GC limitations and barriers, the authors referred mainly those involving
the toxicity of substances (pp. 16–19). However, at present, the lacunas on toxicological
data remain about the same (REACH, on-line), which shows how much the knowledge
on the subject requires improvement. On the other hand, the text ignored thermodynamics
as a limitation to GC, it being implicitly referred only about the nature of sustainable vs
exhaustible materials in the context of Principle 7 (A&W 1998, pp. 45 and 68)—however
the inexorable limits imposed by Second Law on the scope of sustainability can’t be for‑
gotten (Marques and Machado 2014). In summary, no clear connection between GC and
sustainability was presented until later (see below, p. 7).
In the final chapter, A&W stated that the future of Chemistry is “difficult of predict
or summarize”, being based on “continual improvement, discovery and innovation” (p.
3
In brackets the parts of the words eliminated in searches are presented.
13
115) towards the aim of environmental benignity. The chapter included a list of promising
research areas, for instance: oxidation reagents and catalysts; biomimetic, multifunctional
reagents; combinatorial GC; chemistry that both prevents problems and solves current pol‑
lution problems; proliferation of solventless reactions; energy focus and non-covalent deri‑
vatization. However, in a companion book reviewing the current state of GC, a different list
of areas was included (Anastas and Williamson 1998, pp.12–15): selection of feedstocks;
selection of reagents; choosing synthetic transformations; selection of solvents and reac‑
tion conditions; selection of products and the design of safer chemicals. The differences of
items in these two lists show the difficulties in fixing the domains of activity of GC, con‑
firmed by comparisons with other lists of areas, for instance those included in the ACS SS
577 and 626 (see above). This is probably a consequence of the diversity and complexity of
Chemistry which prevent or difficult the fixation of basic criteria for domain characteriza‑
tion (see also Discussion below, p. 17).
Soon after the end of the Emergence phase of GC, some works that help to visualize
its development were published and were analysed. One of these reports the activity of
the working-party of IUPAC on “Synthetic Pathways and Processes in Green Chemistry”
(Tundo et al. 2000), two items deserving attention. The first is on the field terminology,
green vs. sustainable chemistry. Green was considered more evocative but assuming a
political connotation, although not intentional, while sustainable (paraphrasing “chemistry
for a sustainable environment”) was perceived as less focused and incisive as referring to
the format of a discipline—the party chose green, therefore GC. The second item referred
to the areas that conform GC, categorized as: alternative feedstocks; benign reagents/syn‑
thetic pathways; synthetic transformations; solvents/reaction conditions; products/design of
safer chemicals; minimization of energy consumption. This list shows a relative similarity
to those included in the books mentioned above (A&W 1998; Anastas e Williamson 1998).
The party also stressed that the complexity of the environment requires an interdiscipli‑
nary approach to GC and that therefore the scientific community must promote educational
opportunities that allow the understanding of its principles and methodologies.
Beside the IUPAC report, four ACS SS books on GC were published. In ACS SS 767
(Anastas et al. 2000, cap. 1), the authors continued to frame GC in P2, placing more
emphasis in the manipulation and control of compounds at molecular level. GS started to
be characterized as not having narrow disciplinary limits, its frontiers broadening due the
many ways it can be implemented. In later chapters several themes were explored: design‑
ing safer chemicals, green chemical synthesis, biocatalysis and biosynthesis, environmen‑
tally benign catalysis and green solvent systems (pp. 3–5). In a sister volume reporting the
same conference, ACS SS 766 (Anastas et al. 2001), further examples of research areas
were included, showing the importance of the chemical engineering field for sustainability:
green processing, green applications of carbon dioxide, environmentally benign catalysis
and separations.
In ACS SS 819 (Anastas 2002, cap. 1) the important role of solvents for improving
chemistry greenness was stressed. Solvents were already an active area of green develop‑
ment and innovation (design), where several studies on traditional and alternative solvents
had been developed with the purpose of increasing greenness (Alder et al. 2016, and ref‑
erences therein). The traditional performance criteria of solvents were discussed and the
reduction of hazards was proposed as a further performance criterion, to be applied along
the whole lifecycle of the synthesis of compounds, in which solvents often play an impor‑
tant role. New research areas on green alternative solvents were mentioned: aqueous;
fluorous; immobilized; supercritical or dense phase fluids; ionic liquids; solventless condi‑
tions; reduced hazard organic solvents (p. 6).
13
In ACS SS 823 (Anastas and Lankey 2002) GC was clearly connected to SD and sus‑
tainability, stressing both the urgency of developing this connection to approach sustain‑
ability and the importance of GC education for this purpose (p. 10). The role that GC plays
in the resolution of a lot of basic environmental problems in agriculture, food, climatic
change, energy, natural resources depletion, toxics in the environment, etc., was empha‑
sized. A comment on Industrial Ecology (p. 7) mentioned the importance of adopting a
systemic mindset. On this aspect, it had been already considered that although the Twelve
Principles were not something totally new, their parallel use in group was revolutionary
(Poliakoff e Anastas 2001). However, this statement does not mean necessarily a sys‑
temic approach, as the interconnections among the principles were ignored. These authors
stressed that GC decreases costs and improves the efficiency of elimination of the toxicity
of residues, but also the challenges to its implementation. However, a sentence highlighted
in a box “… young people are beginning to perceive chemistry as a key to saving our envi‑
ronment rather than a tool for its destruction…” (p. 257) suggested a “salvationist” per‑
spective of science and technology.
In summary, this Emergence phase of GC brought proposals for attitudinal changes
from a chemistry insensible to the environment to a new chemistry committed preventively
with its preservation, developed in the context of P2 and expressed by BbDCh, the com‑
mitment to synthesis benignity being crafted in the Twelve Principles. However, it seems
that aspects like research areas and the connection between GC and sustainability, although
mentioned, did not deserve enough attention by the main precursors of the new field.
The divulgation phase
The important role of scientific communication in science development is well recognized

and this was confirmed by the launching, in 1999, of the Green Chemistry Journal (GCJ),
which contributed strongly to the divulgation of academic research in GC and boosted
its development. Only almost ten years later, in 2007, close to the tenth birthday of GCJ,
another journal, the Green Chemistry Letters and Reviews (GCL&R), started publication.
Next, we discuss editorials of these journals selected to show elements that characterize
different and successive comprehensions of GC with respect to its aims and components of
evolution along this second phase.
Editorials of the Green Chemistry journal
In the editorial of the GCJ first issue, in 1999 (Clark 1999a), GC was described as aiming
the elimination or minimization the production and use of hazardous substances (and haz‑
ardous wastes) through the utilization of the Twelve Principles in the design and synthesis
of chemical products. Two driving forces of GC were mentioned: first, the rising interest of
the Chemical Industry in the importance of the concepts of waste minimization and atom
utilization in synthesis design; second, the growing governmental attention to the produc‑
tion and deposition of residues, expressed in legislation of increasing strictness and com‑
plexity. However, no mentions of the concepts of sustainability, innovation or system were
included. A list of examples of themes acceptable for publication in the journal provided a
glimpse of its scope. In summary, the GC global view in this editorial was similar to that
presented in A&W (1998), being more reactive to the production of residues than to the
13
proactive implementation of sustainability. Other editorials by Clark in later issues of the

first year of GCJ referred several other aspects of GC implementation.
The first editorial was accompanied by a review of the same author on Green Chemis-
try: challenges and opportunities (Clark 1999b) where it was acknowledged that SD was
then accepted by governments, industry and society; as well as the poor image of chem‑
istry. It was remarked that the reduction of wastes in processes and in the use of prod‑
ucts decrease the global costs of residues and improve industrial competitiveness. The
ideal synthesis aiming the protection of the environment, health and safety and economy,
was considered a source of challenges to CG, therefore the “environeconomics” should
be the driving force for the development of new products and processes. Two important
lines for GC development—acid catalysis and partial oxidations—were discussed to show
how to deal with environmental unacceptability that results from the low atom economy
of improper synthetic pathways. In summary, the review reinforced the BbDCh concepts
(Anastas and Ferris 1994) about the role and nature of GC, underscoring that this involves
innovation, application and education. However, no mention of the Twelve Principles was
included, although the fundamental ideas of some of these were mentioned.
In the first issue of the second year of publication of GCJ, Sheldon (2000) mentioned
that the journal is the ideal forum for broad discussion of GC, including technological
and social aspects. The meaning and use of the term green was discussed once more—the
industry preferred sustainability or DS instead of “green”, because of the political associa‑
tions of the word in several countries, but the word “green” was more broadly accepted by
the general public. However, the association of the two terms was considered appropriate:
sustainability as a goal and GC as the way towards it. Moreover, the definition of what is
or is not “green” is not always sharp, chemical greenness being a relative concept. Shel‑
don stressed also that GC involves two fundamental components: the efficient utilization of
resources, through waste elimination; and safety in the manufacture of chemicals. The aim
of GC is the elimination of residues at source, i.e. primary P2, but the end-of-line waste
treatment is not GC. In summary, this editorial showed that at this stage, the discussion
included the main finality and connection of GC to sustainability—something mentioned
above (p. 7, on Anastas and Lankey 2002, cap. 1). In a later editorial, Clark (2000a, p.
G33) considered that GC “is a concept that should influence Chemistry at all levels”—
education, research and industry. Awards and honours awarded in the field of GC in sev‑
eral countries showed its world expansion, although depending on the level of development
(Clark 2000b). The broad perspective required to deal with GC (multidisciplinarity, cataly‑
sis, workup, etc.) was also pointed in another editorial (Macquarrie 2000).
In the editorial of the first issue of the following year, Clark (2001) mentioned the grow‑
ing of the GCJ (number, variety and quality of submitted papers, etc.) and the continued
development of GC (congresses, acceptation by industry, etc.), as a result of the economic,
environmental and social achievements it may provide.
In 2002, Clark (2002), after mentioning new GC emerging areas (green products,
sources of alternative energies, separation and purification technologies, etc.), called atten‑
tion to the importance of greenness metrics for the progress of GC, which should be used
in the whole lifecycle for energy, resources consumption and the end-of-life of the product;
and remarked that the end-of-life requires attention to design, for example of recyclability.
Bashkin (2002) considered that the diversity of GC is a problem for the communication
among its practitioners and that incremental innovation is important for improving chemi‑
cal greenness.
In 2003, Raston (2003) referred the existence of a GC community and the importance
of innovation for its implementation and placed GC under the umbrella of sustainability,
13
which means that chemists should develop GC to support sustainable technologies as

a moral obligation. The inclusion of toxicity studies in GC was also commented. In
a similar line of thought, Collins (2003) discussed the importance for chemistry of
sustainability ethics and ecotoxicology, to allow full contribution of GC to SD. In a
last editorial, Clark (2003) referred to the fifth birthday of GCJ and commented the
internationalization of GC (conferences, networks, etc.), its multidisciplinarity and the
strengthening of its connection with sustainability, highlighting that “the race towards a
sustainable future is a marathon not a sprint”—it requires a long-time effort. In conclu‑
sion, all these editorials mention the connection between GC and sustainability, show‑
ing increasing acceptation of this theme.
Several 2004 editorials discussed the GC progresses along different dimensions, some
of which recurrent. In the first issue, Leitner (2004a) referred the increase of the number of
papers on GC (1700 in December 2003, SciFinder) and the RSC decision of starting publi‑
cation of twelve issues of the GCJ per year. Metzger (2004), in a commentary on an edito‑
rial discussed above (Collins 2003), called the attention to the importance of some chapters
of Agenda 21 for the restructuration of chemistry towards sustainability, for this purpose
defending changes in chemistry teaching and research. Warner (2004) referred again the
importance of toxicology teaching for GC and stressed its difficulty because the toxic risks
and the functions of substances are not always closely connected. Finally, Leitner (2004b)
commented on the importance of education for GC advancement, highlighting the role of
experiments for motivation of students.
In 2005, two editorials discussed innovatory themes. Raston (2005) dealt with the
importance of biomass residues as raw materials for manufacture of chemicals and the
challenges this involves in several research areas. Leitner (2005) reported on a meeting
on green solvents where several emerging themes for synthesis implementation were pre‑
sented, like new concepts on phases/solutions for increasing reactivity and selectivity;
reaction and workup integration; and multidisciplinary research studies in the molecular
science/reaction engineering interface.
In 2006, several editorials brought to discussion some interesting aspects about GC evo‑
lution that improved its understanding and/or brought novel ideas for pressing its progress.
Welton (2006), under the title “All solutions have a solvent”, discussed briefly the contents
of the term solvent-free or solventless, often used uncritically, as only solid (and dry) phase
reactions and reactions that involve a liquid without any solute are solventless. This unsuit‑
able use of the term prevents a correct vision of the complex nature of the implementation
of chemistry, but the discussion opens the door for research on new solvents (see below, p.
18). Leitner (2006), in a reflection on the GC progress in the previous year, highlighted that
revisions of chemical processes may not imply greenness improvement, suggesting that this
purpose should be included as an intentional aim in such tasks—however, the importance
of green metrics for this purpose was not mentioned. Clark (2006), revisiting his ideas on
GC (Clark 1999b), referred that the problems with wastes were considered increasingly
more important by society, implying changes in legislation and pressing progresses in GC
towards the three components of sustainability. In addition, the text highlighted the strong
connection between the lifecycle of products and sustainability, as shown in diagrams that
involve GC in all lifecycle stages (extraction of raw materials, manufacturing and use of
the product), suggesting that a systemic approach is required for greenness assessment.
This means a broader scope of GC, previously based in P2 and BbDCh, as already previ‑
ously recognized by Anastas and Lankey (2000). The importance of REACH (REACH on-
line) for GC, especially for dealing with the toxicity of substances and its impacts, and the
necessity of research in this field, were also remarked.
13
Editorials of the Green Chemistry letters and reviews
In a first editorial in the launching issue of GCL&R, in 2007, Warner (2007) discussed
the evolution and progress of GC, this being presented as a “cohesive area of endeavour”
expanded along three lines: breadth, depth and geography. Breadth refers to the increasing
number and diversification of themes dealt with success, both in the academy and in the
chemical industry. Depth results from the work of an increasing number of research groups
in specific fields, forming communities settled in diversified institutions. With respect to
geography, the number of industrialized countries where GC is practiced covers the whole
world. However, the concepts of sustainability and system deserved no attention, while the
importance for GC of innovation, both in the design of benign products and processes and
for providing increased economic advantages to industrial firms, was mentioned.
The title of a second editorial (Anastas 2007) included the words design, innovation and
system (more precisely cohesive system). GC was described as chemistry of sustainabil-
ity, with capacity to support simultaneously environmental, economic and societal benefits.
With reference to the evolution of GC it was mentioned that, from the emergence, it pen‑
etrated successive new research areas, allowing more deepness and diversity and requiring
interdisciplinary research with integration of several sub-disciplines of chemistry. In this
context, four fundamental elements were highlighted: (1) Design: addressed with intention
to products and processes in a framework where aims that involve criteria both for func‑
tional and environmental performance are required; (2) Innovation: addressed to the proac‑
tive conception of new products and synthetic pathways without environmental impacts—
bringing no problems to be resolved reactively; (3) Solutions: focused on the resolution
of environmental and sustainability problems through the design of a new generation of
substances, processes, etc.; (4) Cohesive system: integrated implementation of the Twelve
Principles within a systemic mindset for allowing both the optimization of compromises
among them and synergic advances of transformative nature, instead of the incremental
progress resulting from the isolated application of the Principles. These four elements
meant a change of attitude to a systemic framework (not the reductionist prevalent in the
GC emergence!) allowing better exploration of the breadth and depth of GC to increase its
scope towards supporting the SD. In summary, both these two separate editorials from the
authors of the basic book of GC (A&W 1998) suggest an evolution to a different, more sys‑
temic view of GC, although this is better explained in Anastas´s text.
In conclusion, in this Divulgation phase, some editorials show evolution of GC in sev‑
eral different aspects: connection of GC to sustainability; acknowledgement of its systemic
nature; attraction of new practitioners; and progressive internationalization.
The consolidation phase
In this section a set of GCJ editorials that commemorate the tenth and fifteenth anniver‑
saries of the journal and the twenty fifth GC anniversary are discussed. No similar edi‑
torials were found in GCL&R. The journal ACS Sustainable Chemistry and Engineering
published a commemorative issue of the twenty fifth anniversary (November 2016), with
an editorial discussing the progresses of GC and Green Engineering in supporting sustain‑
ability, followed by papers about the evolution of several themes, p. ex., solvents, nanotech‑
nology and education (see section Discussion, p. 17, on Haack and Hutchinson 2016).
13
The Green Chemistry Journal 10th anniversary
In the first editorial, Poliakoff et al. (2008) stressed the growing of the impact factor of
GCJ (4192 in 2006) and announced the publication of a series of reviews of several GC
areas along the year. Li (2008) considered that the increase of efficiency (of several types,
p. ex. material, energetic and functional efficiency) is a central GC concept and highlighted
the importance of research on solvents, mentioning the use of water as a green solvent
for preventing side-reactions in free radicals reactions and therefore improving the atom
efficiency (economy), as discussed in a review paper in the same issue. Sheldon (2008),
connecting GC to the industry and academy, discussed GC as a dual field, “Green and
Sustainable chemistry”; referring that GC preconizes the “design of greener and more
sustainable processes and products” (p. 359), defended the existence of several shades of
green and degrees of sustainability, therefore reaffirming the idea of the relativity of chemi‑
cal greenness (see p. 8 above, on Sheldon 2000). For Sheldon, GC involves two compo‑
nents: first, the efficient use of (preferably) renewable materials—for elimination of wastes;
second, the prevention of the use of toxic and dangerous solvents and chemicals—in the
whole lifecycle; in summary, the GC concept comprises multiple dimensions. Welton
(2008), in an analysis of catalysis in ionic liquids, pointed the greenness limitation of these
compounds and presented for the first time a specified version of the Twelve Principles—
addressed to evaluating the design of chemical processes involving ionic liquids. Anastas
(2008) referred that GC should evolve towards an interdisciplinary and integrated model;
and defended the multidisciplinarity of design, which means complexity in its implemen‑
tation but allows improving the performance and preventing undesirable consequences in
innovations. Leitner and Poliakoff (2008), on using supercritical fluids as solvents, pointed
that they not only allow replacing VOCs by more benign solvents, but also may provide
the implementation of new practices for manufacture of materials—these requires innova‑
tive design for processes. Varma (2008a, b) discussed a review in the same issue on the
introduction of new activation techniques in green synthesis, like mechanochemical mix‑
ing, microwaves and ultrasounds, which allow savings of material and energetic resources.
Finally, Green (2008), after adverting that the use of petrochemicals will go on in the near
future, referred that attention should be paid to the design of new installations with clean
technologies for Fischer–Tropsch refineries, used in the manufacture of transport fuels and
chemicals from synthesis gas obtained from coal.
In summary, this set of commemorative editorials addressed to specific themes, in
which the importance of design was again highlighted, suggests that the comprehension of
the nature of GC moved to a more systemic vision, although with limited progresses.
The Green Chemistry journal 15th anniversary editorial
This editorial included five texts authored by scientific editors and chairpersons of the Edi‑
torial Board of the GCJ.
Clark (Clark et al. 2014, p. 18) remembered the first years of the publication of the
journal, when he had to persuade colleagues that the new journal was the adequate place
to publish their best work, as often they saw no relevance to GC in their papers; in con‑
trast, fifteen years later, the situation had changed, with many papers published as GC in
different journals. Therefore, he deemed necessary to clarify what is GC, without “regu‑
lating the research or standardizing its output” (p. 18). The growing of GCJ showed that
13
this has to be developed continuously to include new themes, for instance, chemicals from
renewables, catalysts, life-cycle assessments and green solvents, confirming the validity of
a journal with the word green in the title. However, the text suggests wrongly that the ideal
of absolute greenness is reachable, with the Twelve Principles covering all chemical activ‑
ity (see Discussion below, p. 19); on the contrary, greenness is a relative concept of great
complexity, being context dependent.
In the second text, Sheldon (in Clark et al. 2014, p. 19) remarked that the two compo‑
nents of GC he had considered before—efficient use of resources and prevention of haz‑
ards, especially toxicity, see above (Sheldon 2008, p.359)—mean that a paradigm change
occurred with the GC emergence in the nineties, which allowed later its evolution and
development, as shown by the different pattern of publications in the GCJ. For instance,
while in its first year of publication most articles were addressed to only two themes (cata‑
lytic processes and alternative reaction media), the analysis of later years shows a broaden‑
ing of scope to subjects addressing GC and sustainability, for instance, on biomass use as
a resource for production of fuels and chemicals (bio-economy) and on bio-catalyses. The
importance of metrics for assessment of the different shades of greenness was also stressed,
as well as the increasing acceptance of GC by industry. Finally, Sheldon concluded that
GCJ is “firmly established as a top-raking journal publishing excellent science”, contribut‑
ing to the recognition of GC as a “sustainable concept”, good for both business and envi‑
ronment (p. 19).
The following text, by Raston (in Clark et al. 2014, p. 20), discussed the role of GCJ as
a scientific base for the development of sustainable technologies that serve the community
at large, both in chemistry and in other fields (nanotechnology, energy, etc.) —highlighting
the importance of GC as a bridge between chemical sciences and engineering. As an exam‑
ple, continuous flow processes were considered a promising field in this interface, with
several topics requiring exploration in the field of reactor technology for process intensifi‑
cation (decrease of size of installations), aiming to reduce the footprints of production of
energy and residues. These and other aspects, like scale and sustainability metrics, should
be included in the design of new reactors for the manufacture of products by kinetics vs
thermodynamics controlled processes.
Next, Poliakoff (see Clark et al. 2014, p. 21) discussed the importance of toxicity eval‑
uation, as highlighted by the Twelve Principles, but pointed that it is difficult to design
greenness metrics for this component. After stressing the general importance of metrics,
he proposed the Function Factor (F-Factor) as a new metric for evaluating the amount of
substance required for obtaining a certain level of its function. This metric assesses the
efficiency of the function, internalizing the concept of matter utility (vs. energy utility
and utility in economy), to be used in parallel with other greenness metrics in the design
and manufacture of chemicals—to obtain more efficiency with respect to both function
and benignity. For instance, the increase of potency of the active pharmaceutical products
allows the decrease of doses, lowering malefic side effects on patient health. However, it is
expectable that the generalization of the use of the F-Factor will be problematic, due to the
difficulties in its calculation. The scope of the F-Factor is similar to the engineer’s attitude
of prescribing the use of the minimum amount of a material to accomplish a certain effect.
Finally, Leitner (in Clark et al. 2014, p. 22), after registering the success of the GCJ,
commented several interesting items. About the connection GC-sustainability, he sagely
remarked that “sustainability is not an absolute goal that can be reached (…)—it will
remain utopia” and that to move on to the ideal goal, successful systems have to be
adaptative by design (p. 23). In this context, some GC research topics amenable to con‑
tinuous evolution were indicated: toxicity and ecotoxicity of intermediates and products;
13
diversification of raw materials; replacement of noble by abundant metals in catalysts.

Finally, Leitner remarked that there is a large difference between the initial themes dealt
with by GC and those researched in 2014. This statement stresses the difficulties in the
characterization of GC areas, as we remarked in the two previous sections.
In the introduction of this editorial (Clark et al. 2014, p. 21), the publication in the GCJ
of a virtual issue of reviews on themes dealt with in papers that reached a large number of
citations was announced, their objective being to provide a comparative analysis of their
evolution by the same authors (see: rsc.li/gc-15-years). In a review on the use of biomass
for the manufacture of chemicals, Sheldon (2014) rose its status, considering that biomass
is a third basic component of GC, together with waste minimization and toxicity elimina‑
tion—however GC ignores the economy, one of the three pillars of sustainability. For over‑
coming this gap, a set of metrics of sustainability addressed to full evaluation of the use
of biomass were proposed: material and energy efficiencies (GC); land use (environment);
and process costs (economy). Varma (2014) reviewed the progresses on obtaining greener
synthetic processes with more benign reaction media and alternate techniques to energize
the reaction. Advantages and disadvantages are discussed, for instance, microwaves as an
energy source allow a decrease of reaction time and an increase of selectivity in organic
reactions, but these improvements depend on the efficacy of the solvent to absorb the radia‑
tion. Willes and Watts (2014), in a discussion based on the Twelve Principles, reviewed
continuous flow processes as tools for sustainability, identifying potential gains in safety,
efficiency, costs and scale—and highlighting barriers to their adoption, including those of
regulatory nature found in pharmaceutical industry. Cevasco e Chiappe (2014) reviewed
the potential of ionic liquids as adequate solvents for a variety of processes that are of dif‑
ficult or even impossible implementation in traditional media, but refer the problems of
increasing the scale for large levels of production. The contents of the remaining reviews
(Song, Dunn, Pfaltzgraff, Climent, Chatel and Behr; see: rsc.li/gc-15-years) were mainly
technical, with limited information on global progresses in their fields (ionic liquids, bio‑
mass and renewables, and pharma regulation). In conclusion, our analysis shows that most
of these reviews report the advantages of the new ways that GC provides for performing
benign chemistry and point to the limitations and barriers that are often found—demon‑
strating how relative chemical greenness is.
The Green Chemistry 25th anniversary editorials in the Green Chemistry journal
In 2016, the GCJ published a series of editorials commemorating the 25 years of the emer‑
gence of GC that provide useful information for understanding its evolution.
In the first issue, Anastas et al. (2016) pondered over generic aspects of the evolution
of GC, mentioning that it is not correct to consider GC as mature, because it is only more
mature than at its beginning and more ready to contribute to sustainability—considering
that “if sustainability is the goal, GC will show the way!” (p. 12). With reference to the
nature of GC, the authors maintained previous ideas (Anastas 2007), stressing again the
importance of innovation and design to combine environmental, economic and human
wellbeing benefits, as required to persecute the goal of sustainability. However, on the
global goal of decreasing the negative impacts of industrial chemicals, the vision of the
authors seems to be now less conclusive about the degree of real achievements of GC than
in the Emergence phase, albeit the frequent successes achieved.
After highlighting that the formulation of the Twelve Principles played an important
role on the perception of GC by the community, the authors recognized that they are
13
“guidelines rather than rules” (p. 12), being useful as a motivation only and intending no
restriction on chemistry development. Therefore, they constitute no checklist for obtaining
automatically a greener reaction or process—they were not conceived as problem-solvers,
rather as a tool for analysis of potential improvements of chemical greenness. The authors
commented also that knowledge in well-established areas were integrated in the Princi‑
ples, in parallel with new knowledge then emerging. Indeed, at the time of their formula‑
tion, many concepts of several types had already been proposed: atom economy or atom
utilization; the search of biodegradability, waste minimization and clean reactions; use of
renewable resources, catalysis for lower energy consumption and improved selectivity, and
safety for prevention of accidents. In summary, the authors seem to acknowledge that a lot
of ideas incorporated in the Principles were already practiced in industry and academy to
incentivize chemical benignity, but provide no information on the integration of the set of
Principles as a structure.
The systemic nature of the Principles, not mentioned at their formulation (A&W 1998),
but only later, when referred as a cohesive system by Anastas (2007), was reaffirmed as a
change of thinking style, important to implement “a transformation of GC from a way of
getting rid of bad things (inefficient syntheses, toxic reagents, needless waste, etc.) into an
approach that is used as a way to generate better things (in essence a tool for innovation to
generate new performance, function, and efficiencies)” (Anastas et al. 2016, p. 13). This
requires design, being reaffirmed that “design does not happen by accident, but rather is
an indication of intention” (p. 13). In summary, only recently the systemic nature was con‑
sidered an important characteristic of the Principles, as its simultaneous use is essential for
obtaining synergic compromises addressed to obtain better global chemical greenness.
The following issues included invited editorials that dealt individually with the Twelve
Principles. An exception is the text by Li (2016) that developed a philosophical analysis on
GC development, with a Daoist insight of the Principles that provides an alternative per‑
spective for implementation of green synthesis. The “Wu Wei” principle (ado or do noth-
ing) should be applied to the different components of the synthetic route, for instance: on
natural resources, to do without using depleting starting materials; on solvents, the better
is the absence of solvent; on energy, use no heat; in separation, use no conventional tech‑
niques, very demanding on solvents and energy; and on reaction design, minimum number
of steps. These prescriptions mean a redefinition of synthetic elegance, considered a goal
of GC by Anastas (1994, p. 10).
With reference to each of the editorials addressed to individual Principles (P1, P2, …,
P12), the ideas, arguments and main examples are presented next, together with occasional
brief commentaries. The text follows the numeration of the Principles, not the sequence of
publication (no editorial on P 8 was published).
Peters and von der Assen (2016) defended the amplification of the scope of P 1—waste
prevention. The usual way of its application is the alteration of synthetic pathways, for
instance by decreasing the number of steps to decrease the amount of wastes (examples:
ibuprofen, sertline and propylene oxide), but prevention of wastes is considered a broader
concept. For example, on one hand, it can be implemented through other Principles, by
increasing atom economy (P2 and P9), by decreasing auxiliary substances (P5) or the pol‑
lution derived from energy production (P6). On the other, the situation should be viewed
more holistically, paying attention to the multidimensional nature of environmental impacts
and to the frontiers of the global system. In this context, it is necessary to consider both the
quality of the wastes and the product functionality, and not only the wastes/product ratio of
masses; and also to the possibility of recycling and/or use of wastes as starting materials.
In summary, when considering the problems of wastes (inevitability of their formation and
13
implications on the environment), the utility of the product (function) should not be forgot‑
ten and lifecycle treatments are required.
Sheldon (2016) highlighted the importance of P 2—resource efficiency, both to the effi‑
ciency of utilization of resources and the minimization of wastes (p. 3180), as well as the
relevance of the atom economy (AE) and E-factor metrics in this context. The principle is
vital for the circular (bio)economy and concomitant resolution of environmental problems,
but will require design addressed to the efficient use of resources. In this situation, catalysis
for minimization of residues, use of renewable resources and valorisation of waste biomass
were considered important for supporting sustainability. However, Sheldon’s discussions
appear to be more reductionist than the previous discussion on P1.
As a postulate of P3—less hazardous synthesis, Wakaki et al. (2016) discussed the
importance of replacement of stoichiometric reactions by catalytic reactions for eliminat‑
ing hazardous substances in synthetic pathways that yield toxic residues. In a more sys‑
temic approach, they pointed as manageable alternatives for these eliminations the design
of processes in which toxic intermediates are retained at low concentrations in the reac‑
tional system, with recycling and reuse (example: alcohol oxidations).
Although without referring P 4—design safer chemicals, Jackson et al. (2016) seemed to
insert the formulation of the Twelve Principles in the historic chemical problem of getting
away of toxicity, started by alchemy and developed along the progress of chemistry, and
placed confidence in GC towards developing procedures for the production of chemicals
with low toxicity, but high functional efficacy.
On P5—safer auxiliary substances, Jessop (2016) referred two aspects about using aux‑
iliary substances. First, these are important in product formulation, including those for
public consumption, and not only in synthetic processes (rarely mentioned before!). Sec‑
ond, attention should be paid to substances that are not solvents, i.e., all auxiliary sub‑
stances should be eliminated whenever possible and, when required, should be innocu‑
ous. Moreover, two strategies were suggested for reducing the environmental impact of
solvents: reduction of use or replacement by greener solvents. Decisions should be based
on lifecycle assessments, for instance in the choice of agents for paint removal, adhesives
and aerosols. However, the nature of the text is descriptive and the future evolution of an
efficient implementation of the Principle is not discussed.
Quadrelli (2016) discussed the numerous “exciting lines of investigations” around P 6—
design for energy efficiency (p. 330), where GC is important for obtaining new materials of
several types to be used along energy chains (production, transportation, storing and con‑
version) in renewable energy systems. The importance of metrics for a realistic evaluation
of the environmental benignity of the production of renewable energies (“green electrons”)
was mentioned. Also the production of ammonia, which requires a high consumption of
energy, was presented as a successful example of saving energy by incremental improve‑
ments of the process along the time. This appears to contrast with Anastas´s idea that GC
should be transformative (see below, p. 16), but it should be remarked that in the ammonia
synthesis the diminution of the energy consumption was not achieved by the prescription
of low temperature and pressures in P 6.
On P7—renewable feedstocks, Llevot and Meier (2016) commented that the renew‑
ability of feedstocks is important in a global vision of sustainability, remarking that the
replacement of exhaustible by renewable materials should be implemented “whenever
technically and economically practicable” (p. 4800), but with internalization of all costs:
environmental, economic and social. Renewability alone does not imply sustainability, as
a process based on renewable feedstocks has to be evaluated comparatively with the no
renewable alternative by assessments covering the whole carbon cycle, to be confirmed
13
as the more sustainable solution. On the other hand, with reference to toxicity, the benig‑
nity of products derived from biomass is not guaranteed by its natural origin. However,
the authors considered the increased use of biomass as inevitable as the deposits of fossil
combustibles are not re-generable, as the geological time of their formation in the crust is
unrepeatable. On the other hand, the continued use of vegetal biomass has to be compatible
with its regeneration time. In summary, this discussion suggests that P 7 is one of the most
difficult Principles with reference to scope and implementation: the advantages of the use
of biomass have been well advertised, but the attention given to the disadvantages has been
scarce (p. ex., the variety of functional groups in biomass and the stability of lignin), as
well as the compatibility with the multiple traditional uses of biomass.
Delilovich and Palkovits (2016) discussed catalysis (P9—preference for catalytic reac‑
tions) as a key technology for obtaining synthetic benignity, presenting examples of cata‑
lytic versus stoichiometric processes (acid catalysis). Beyond waste reduction, the cataly‑
sis may provide decrease of energy requirements of processes. Searching opportunities of
catalysis in the manufacture of products that integrate the carbon cycle, allowing its closure
(C/CO2 neutral products), are presented as a way towards “sustainable processes and future
circular economy” (p. 593). In conclusion, the importance and role of catalysis in GC is
once more confirmed by this review.
10—design for degrada‑
In an incisive analysis of the potentialities and limitations of P
tion, Scott and Lee (2016) stressed that this task requires a systemic treatment for dealing
with the problems along the whole lifecycle. The detailed analysis of the scope of bio‑
degradation and its consequences on chemical greenness suggests that the products of
degradations may bring complexity to the environment when it receives anthropogenic
components. Similarly, searching for complete degradation may produce the design of
products inadequate for the intended function and/or that prevent an efficient recycling,
thus subverting the implementation of a circular economy. For example, in the manufac‑
ture of polymers, the embedment of lifetime in the design of molecules and materials is
important: it allows a suitable balance between polymer durability—required for utiliza‑
tion—and monomer robustness—required for its maintenance in closed circles. In other
cases, like surfactants, a dispersion in the environments is intrinsic to the use and recycling
is not possible, therefore the design should include total degradation to innocuous products
that are fully integrable in the nutrients biologic cycles. These situations require a holistic
mindset towards lifecycles, which is complex. In summary, the Principle can be used as a
valid guide, but provides no warranty of chemical greenness for materials with origin in
biomass.
In a review on P11—real-time analysis for pollution prevention, MacFarlane et al.
(2016) referred the importance of developing new analytical techniques to support GC.
For instance, in industrial processes, the use of sensors of different types (electrochemi‑
cal, spectroscopic, etc.) can provide direct determinations in real time of several species
in parallel, allowing increase of the process efficiency, improvement of the product quality
and prevention of pollution. However, the barriers to broadening the implementation of
the mentioned analytical technologies in industrial practice are numerous and difficult to
overcome.
The multiple aspects of accidents and hazards (p. ex., of substances, losses, explosions
and fires) are discussed by Sneddon (2016) in his review of P12—safer chemistry for inci‑
dent prevention. Control measures for these hazards obey a hierarchy, its top level being
the elimination/removal of the dangerous agent, with substitution by a viable alternative
(with reference to cost and function) as second level. Indeed, these are intrinsic features
of GC that prescribes the inherent safety of the first level and, if this is impossible, adopts
13
hazard reduction by substitution. The publication of guides (of solvents, reagents and reac‑
tions, see Discussion, p. 19) and other tools that push safety into chemical tasks by pro‑
viding alternatives means progress in this direction. All chemists should consider safety
a fundamental ingredient for the chemical activity and a component of environmental
sustainability.
These editorials mean an effort of analysis and synthesis of the research activities that
have been promoted by each of the Principles, providing a demonstration of their potenti‑
alities for application in further situations. The present discussion evidences the different
challenges and barriers to be overcome for the implementation of most of them, among
other aspects, in the next section.
Discussion
GC emerged in the context of PPA (USA 1990), aiming at the elimination or decrease of
the use of hazardous substances, through modifications in the industrial synthetic pro‑
cesses. In the Emergence phase, previously to the publication of the Twelve Principles,
several successive ACS symposia (577, 626 and 640) played an important role in the divul‑
gation of the GC purpose and of the research work in the field. Along this stage, the idea of
preventing by design the use and formation of toxic substances in synthetic routes emerged,
in parallel with the elimination of residues at source, the supreme goal of P2 (as detailed
in ACS SS 640). The term GC was also crafted, but principles were only generically men‑
tioned (ACS SS 626, p. 6), atom economy being referred (p. 13) as one of the fundamen‑
tals of such principles. This suggests that the Twelve Principles were under slow gestation,
but no mention of this process was included in the ACS reports—indeed, no remarks about
the incubation of the Principles were also included in their publication (A&W 1998). It
would be interesting to know details on how the Principles were formulated: choices of
their individual goals and their ordering, whether hierarchisation and interdependence were
though about, etc.
In the next stage of evolution, GC progressively acquired independence of P2, larger
scope, and more interest from academy, with increased participation of researchers. As a
consequence, other areas beyond alternative benign synthetic routes (BbDCh) deserved
attention, from toxicology and biodegradability of substances to the formulation of green
products. The publication of the Twelve Principles demarked the recognition of the new
field and started a second phase in the GC evolution—the Divulgation phase—supported
by the launching of GCJ in 1999. Along this evolution, the adhesion of a crescent number
of chemists allowed the constitution and consolidation of a diversified community engaged
in the GC principles and practices (Howard-Grenville et al. 2017).
In its initial stage, GC aimed at improving environmental protection by chemical indus‑
try, only very occasionally being related with SD. Only later, in ACS 823 (2002), it started
to be inserted in the sustainability context. However, about ten years later, in the Interna‑
tional Year of Chemistry, Anastas (2011) highlighted the parallel growing and increased
interrelationship of GC and sustainability (p. 62), but still provided no discussion on
the nature, ways and complexity of the interactions. This suggests that, in practice, little
strengthening of causal vincula occurred, albeit the omnipresence of both terms in Chemis‑
try at present. This situation is still remaining nowadays—probably owing to the broadness
and complexity of both concepts.
13
The systemic nature of GC deserved little mention along the Emergence phase.
Only a paper, in 1997, discussed the importance of a systemic mindset for dealing with
the problems of the emergent GC (Anastas e Breen 1997), opinion later endorsed by
Graedel (2001). However, in the conception of the Twelve Principles, the interrelations
among them and the importance of their parallel application were not mentioned, sug‑
gesting that their formulation was developed in a reductionist mindset, although they
conveyed a huge ethic strength to support GC. Only ten years later, the proponents of
the Principles recognized that these should be used as a “cohesive system” (Warner
2007, p. 1; Anastas 2007, p. 3), in parallel, allowing simultaneous contributions of all of
them to obtain or improve chemical greenness. Later, in a comment of the evolution of
GC along its twenty years, Anastas (2011, pp. 62–65) reaffirmed the importance of the
holistic approach for using the principles.
When the cohesive system concept was introduced, no suggestions were presented
on characterizing the structure (interconnections among Principles) and its implication
on handling the system of Principles in practical situations. The connections impose
conditions in the use of the Principles as an innovation tool for obtaining or optimizing
greenness and performance as a whole. The lack of completness of the set of Principles
for covering all the dimensions of chemical greenness and its role as a base for the
conception of greenness metrics were also ignored (Machado 2014, 2015). Similarly,
the Second Twelve Principles (Winterton 2001), albeit their importance for achieving
greenness in the laboratory easily transferable to industrial syntheses, were not consid‑
ered. Again, when Welton (2008) applied the Twelve Principles to the catalysis in ionic
liquids, their interdependences were ignored—the adaptation dealt with the Principles
individually. Later, Anastas et al. (2016) reaffirmed that the Twelve Principles should
be considered as a guide, not a set of rules for providing automatically greenness, rather
serving as a motivation (p. 12), but referred no significant progress on their systemic
application. Indeed, a certain mitigation of Anastas’s enthusiasm on the support that
Principles provide to GC seems to be present in this text. On the other hand, in the set
of editorials commemorating the twenty-five years of GC only two (Wakaki 2016; Scott
and Lee 2016) refer the importance of the systemic mindset in for GC implementation.
Different views have been advanced for the nature of innovation in GC. In the Emer‑
gence phase, Anastas mentioned that innovation of incremental nature applied to less
benign steps of lifecycle could support the development of the new GC (Anastas and
Williamson 1996, p. 3). Later, when presenting the Principles as a cohesive system, he
stated that their use in parallel would provide transformative advances (Anastas 2007,
p. 3), especially in the design of products and processes for obtaining simultaneously
good performance and pro-active prevention of adverse impacts. Although recogniz‑
ing the progresses implemented by small increments of efficiency, toxicity reduction,
etc., he stressed that innovation should be transformative rather than incremental (Ana‑
stas 2011, p. 64). Later, Anastas (2015) reaffirmed this idea more strongly (in the title
“Green Chemistry next: moving from Moving from Evolutionary to Revolutionary”),
stating that only the revolutionary way can provide economic value (p. 3). However,
other authors gave more importance to incremental innovation (Raston 2003; Quad‑
relli 2016). In summary, considering the diversity of situations found in the practice
of chemistry, both ways seem useful, incremental innovation being more easily imple‑
mented—most chemical systems are complex and the transformative way requires their
design from scratch. Anyway, this item is controversial and we suggest that further anal‑
ysis is required, but in both ways GC validation is indispensable and for this purpose
greenness metrics are important tools.
13
The first mass metric, the E-factor, was conceived before the emergence of GC (Sheldon
1992), as well as the concept of atom economy (Trost 1991), that later was used as the
base of the AE metric. Although this concept was pointed as a fundament of GC principles
(Anastas and Williamson 1996), mass metrics deserved little or no attention in the Emer‑
gence phase, probably because they were conceived outside the GC movement. Greenness
metrification acquired importance only at the beginning of the present century, especially
in the pharmaceutical industry, which started using these two and other mass metrics
(Curtzons et al. 2001; Constable et al. 2001, 2002). Meanwhile, the chemical industry had
initiated using environmental metrics previously conceived in lifecycle assessments (Aza‑
pagic 1999). Later, in the Divulgation phase, further metrics were proposed (see review by
Calvo-Flores 2009) and interest in metrification increased. Manley et al. (2008) referred
the importance of greenness metrics for the incorporation of GC in education, industry,
research and regulation. Sheldon has also repeatedly stressed the relevance of metrics
(Sheldon et al. 2014; Sheldon 2016). However, in the set of the thirteen GCJ (2016) edito‑
rials commemorating the twenty-five years of GC, less than a half mentioned metrics and
only Sheldon´s contribution included a specific discussion on the subject. The E-factor was
examined in this editorial and in another (Delilovich 2016). AE and lifecycles were men‑
tioned in one editorial each (Sheldon 2016; Scott and Lee 2016, respectively). Albeit these
mentions to the importance of metrics and their increasing application, their use is not still
generalized—this situation suggests that greenness evaluation continues to be a secondary
concern for most chemists, perhaps as consequence of their long-time adherence to the tra‑
ditional yield and selectivity calculations.
In this context, GC requires more attention to the assessment of greenness to be able
to affirm itself as green—to show the claimed benignity it is expected to provide. For
instance, prudence is required in generalizations of “green behaviour” for classes of reac‑
tions—generalizations are an inheritance of the habitual reductionist vision of chemists.
Anastas (2015) stressed that the multidimensional nature of GC implies the simultaneous
use of several metrics for assessment of the greenness. Moreover, the increasing connec‑
tion between GC and sustainability involves, for instance, more integration of GC with
green engineering and incorporation of knowledge from biology, especially toxicology.
All these changes increase the complexity of the practice of Chemistry, requiring multiple
parallel evaluations in studies of different types: molecular design, benignity/toxicity and
prevention, fate and effects of chemicals in the environment, lifecycle assessments, etc. In
summary, green metrics are an important challenge for GC.
Research areas have been listed by different authors along GC evolution (Anastas and
Farris 1994, pp. 19–20; Anastas et al. 2000, pp. 3–5; Anastas et al. 2001, pp. 1–5; Abra‑
ham and Moens 2002, pp. 1–9; A&W 1998, pp. 21–27 and 115–119; Anastas and Wil‑
liamson 1998, pp. 12–15; Anastas et al. 2016, p. 12), but these lists show recurrences and
amplifications and we found difficult to define and classify the GC research areas and their
evolution. This is understandable because the field is new and kept aggregating new part‑
ners from different specialties of Chemistry that brought with them increasingly diversi‑
fied interests. The difficulty of characterizing areas is a result of the complex nature of
chemistry—for example, the increase of complexity of synthetic routes with the number
of intermediates and steps (Anastas e Lankey 2000, Fig. 2, p. 290, referring Hendrick‑
son 1966). All these aspects suggest that rigid frontiers between areas/specialties can‑
not be established. This diffusiveness is connected to the GC identity problem—whether
GC be considered a separate discipline, a meta- or a sub-discipline (A&W 1998, p. 29;
Tundo et al. 2000) and the definition of its frontiers, as highlighted by Clark: “we need to
be more clear on what deserves to be classified as GC… [but]… cannot regulate research
13
or standardize its outputs” (Clark et al. 2014, p. 18). On the other hand, as an activity of
the ACS GCI GC Institute Pharmaceutical Roundtable (ACS GCI PR), the pharmaceuti‑
cal industry has been trying to define its priority research areas with pragmatism, through
decisions involving researchers as representatives of the companies (Constable et al. 2007;
Jiménez-González et al. 2011). In summary, the difficulty of identifying and describing
the areas of GC remains and the evolution of these should deserve attention as it allows to
observe the evolution of GC itself and the configuration of recurrences in its domains and
fields of interest.
Education in GC was a theme often found in the literature analysed but, although impor‑
tant, was not extensively explored in the present study, due to its specificity and dimension.
However, ASC SS 1011 “Green Chemistry Education—Changing the Course of Chem‑
istry (Anastas et al. 2009) deserves mention, because it included several important items
(curricular innovations, integration with engineering teaching and successful examples of
GC teaching in US). Moreover, the subtitle means a challenge for chemical education as a
whole, p. ex. for preparing young chemists to support sustainability (p. xi). More recently,
Haack and Hutchinson (2016) summarized advances and needs of GC education, exam‑
ining strategies for the training of chemists and the incorporation of GC in curricula, in
pedagogic materials and in specific program/courses. The barriers to overcome were dis‑
cussed, as well as the advantages of establishing a roadmap for GC education (Voorhees
and Hutchinson 2015). An example of the barriers is the absence of evolution in chemistry
degrees, which have hardly changed since fifty years ago (Ritter 2016, p. 25), GC being an
opportunity to operate the required modernization. However, other studies show that no
global vision of the penetration of GC in Chemistry curricula is available (Zuin and Mam‑
mino 2015; Marques and Machado 2018). On the other hand, it is interesting to remark that
most of the reports that emphasize the importance of education in GC contain recommen‑
dations, but to be implemented by the readers—most of the authors provide no results of
their efforts to test their ideas.
The integrated nature of GC deserved little discussion along its evolution, although
Anastas (2007) and Warner (2007) mentioned this feature when they re-assessed the GC
Principles as a cohesive system (see above). More emphasis on the subject was provided in
several papers by Collins (1995, 1997, 2001, 2003, 2017). Collins (2001), in a discussion
on the connections between Chemistry and sustainability, reaffirming previous ideas (Col‑
lins 1995, 1997), mentioned the existence of general principles in GC, without specifying
the Twelve Principles. On sustainability, Collins (2003) highlighted the importance of both
ethics and ecotoxicology, advancing a set of questions and suggestions on how education
and research in chemistry may contribute to SD. Metzger (2004) replied to these ques‑
tion suggesting that was necessary to transfer the base of chemical education from fos‑
sil to renewable feedstocks (biomass)—for this purpose, education would require a change
of objectives for integrating GC/chemistry in the challenges of SD. However, oil and gas
will continue to be the basis of chemistry for some decades, therefore the timescale for the
changes should deserve attention, as well as the complexity of acquiring knowledge on the
design of efficient chemical processes based in biomass.
Recently, in a review on the evolution of a GC course he has been teaching since 1992,
Collins (2017) referred the challenge of transforming tertiary GC teaching towards sustain‑
ability and remarks that GC has to be the field in which the problems are addressed in a
way suitable to support ecologic and social sustainability—negative impacts to health and
environment have to be eliminated and simultaneously innovation is required for helping
society in the resolution of those problems. Interesting, Collins (2017) re-phrased more
directly the three generic principles (presented above, pp. 5–6) he had suggested long ago
13
(Collins 1997): (1) the purpose of CG is the protection of life; (2) GC has to be inter‑
disciplinary; and (3) being complex, has to be implemented at long notice. Collins now
considered that the Twelve Principles (A&W 1998) support “minor technical strategies for
achieving cleaner synthesis”, therefore being of limited scope—not an ample doctrine for
“advancing sustainable products and processes” (p. 97); and concluded that green sciences
like GC should be faithful to sustainability, as this is hierarchically superior, and prescribed
that GC should give priority to the preservation of life through due consideration of toxic‑
ity, evoking the four sustainability principles developed by Robèrts et al. (2013). In sum‑
mary, Collins (2017) presented an integrated vision of GC, with a close relationship with
respect to the ecological and social components of SD, which requires innovation, inter‑
disciplinarity and a continued effort along the time. An example of this last aspect is the
effort that the Pharmaceutical company GSK has placed since 1999 in successive revisions
of its guide of solvents for implementing the replacement of problematic by green solvents
(Alder et al. 2016, and reference therein).
Other dimension of the integrated nature of GC important to understand its develop‑
ment is the penetration in academy and industry. Only a few papers attempted the analy‑
sis of this aspect, although separately in the academy (Sjöstrom 2006) and in the pharma‑
ceutical industry (Constable et al. 2007; Veleva et al. 2018). This situation is probably a
consequence of the complexity of the GC expansion due to its numerous dimensions and
interconnections.
Our analysis revealed the absence or scarcity of treatment of the following themes,
which deserve mention because they are also important for GC development as they mean
challenges and barriers to its implementation.
Albeit the cohesive nature of the Twelve Principles (Anastas 2007), the traditional edu‑
cation of chemists in a rationalist mindset, that ignores the complexities of chemistry and
the search for sustainability, rises barriers to the progress of GC which require a systemic
vision to be overcome. This systemic attitude must include also aspects not present in the
Twelve Principles, for instance the context—the connections of chemistry with the envi‑
ronment in lato sensu. Indeed, beyond ignoring the Second Twelve Principles (Winterton
2001), Anastas rarely mentions his Twelve Principles of Green Engineering (Anastas and
Zimmerman 2003). In summary, the practice of the cohesiveness has not been emphasized.
Indeed, more recently, Gilbertson et al. (2015), in a review on green nanomaterials, pre‑
sented a holistic approach involving the multi-parametric nature of the Principles that is
required to support multidimensional decisions when greenness optimization is pursued.
However, in the repeated presentations of the Twelve Principles no attention has been
given to this requirement—the systemic attitude that is essential for the management of a
cohesive system.
As GC is increasingly considered as a science for supporting sustainability, it is impor‑
tant to remark the limitations imposed by the Second Law of thermodynamics, which con‑
ditions the solutions for the environmental problems capable of being done (Marques and
Machado 2014). Indeed, for instance, the contribution of energy to chemistry was insuf‑
ficiently considered in the development of GC. Quadrelli (2016) discussed the potential of
renewable energies (see above, p. 14), but these are still faraway of being fully green, given
their high voracity for fossil energy. The fossil sources are able to provide energy at high
concentrations obtained at large scale, essential for technology, this explaining the techno‑
logical progress and civilization development achieved by the “carbon society”. However,
thermodynamics limits the solutions for environmental problems (or even implies their
irresoluteness), which brings extra complexity to achieving sustainability—GC has to pay
attention to such limits.
13
The importance of the lifecycle for GC implementation was recognized very early. Ini‑
tially it was associated to benign-by-design (Anastas and Ferris 1994, p. 6), later it was
remarked that innovation should cover the whole lifecycle (Anastas and Lankey 2000) and
that metrics had to be employed in all its stages (Lankey and Anastas 2002). However,
given the complexity of following and assessing the lifecycle of a chemical to obtain envi‑
ronmental benignity and efficacy in function, its full scope and implementation is still an
open theme (Scott and Lee 2016).
Beside metrics, that in most cases are used a posteriori, other tools based in the techni‑
cal consolidation of GC are important for its practical implementation, for instance guides
for choosing: (1) green solvents (Aldrer et al. 2016); (2) green reagents for important syn‑
theses in pharmaceutical chemistry (Adams et al. 2013; Henderson et al 2015); and (3)
agents for derivation/protection (Tobiszewski et al. 2017). Tools of this type for a priori
application constitute a broad field with a large future, due to the importance of restrict‑
ing the practice of chemistry to greener reactions, reagents, techniques, etc. for the pro‑
gress of GC. Moreover, the use of utility criteria will increasingly determine the research
in the GC field, allowing the identification of priority problems addressed to supporting
sustainability.
Finally, a limitation we found in the present study was the characterization of biblio-
graphic items for constitution of the inventory for discussion, because of lack of consist‑
ence in the abstracts and key words provided in papers, albeit the advances of electronic
supports (Minhas 2003; Ruthven 2006). For the analysis of the development of the GC
domains and procedures the modern science of information is important, for instance the
adoption of a standard for bibliographic information (inclusion of standardized keywords
by the GC journals, etc.) should deserve more attention.
Conclusions
The aim of the present analysis was to provide an integrated vision of the GC evolu‑
tion, an important conclusion being that the number of researchers in different areas of
chemistry that pursue sustainability in the field of GC has been increasing. There is now
a self-denominated community of green chemists—or epistemic community (Epicoco
et al. 2014)—with relative cohesion of principles, albeit some differences between US
and Europe with reference to the initial approach to GC. Recently Howard-Grenville et al.
(2017) reported also that the emergence and growth of GC drove changes in the occupation
of chemists upon their adhesion to GC, given that it means: (1) a “normalizing frame” that
gives origin to general innovation in chemistry; (2) a “moralizing frame” (based on an ethic
imperative); (3) a “pragmatizing frame” (a tool for dealing with the problems chemists find
in their daily work). These two studies of different nature, respectively epistemology and
labour sociology, therefore with purposes different from ours, confirm the importance, the
changes and the strength of GC within the whole Chemistry.
The existence of lacunas of information and the scarcity of discussions difficult a holis‑
tic analyses of the evolution of GC along the twenty-five years of its life and limit studies
like the present one. Beside the two aspects included in the discussion above (research
areas and lack of uniformity of bibliography), two other important items deserve further
attention: (1) the difficulty of characterizing the advances in different research areas, conse‑
quently to define the domains of GC; and (2) the complex problem of greenness evaluation,
13
that limits the differentiation between GC and traditional chemistry—the use of green met‑
rics has been increasing, but is not a general practice yet.
Having in consideration that GC is still young and hardly started, rather is only ready for
full development (Anastas 2016, p. 12), we chose to rise two broad questions to conclude
our analysis: What has changed more intensively in GC during its short life? What has not
changed yet?
With reference to the first question, we list the more important changes we were able to
identify:
1. GC acquired identity, now better defined and acknowledged; its scope increased, includ‑
ing now further areas beyond synthesis, for instance the formulation of green products
and green analytical chemistry; and received also more interest and participation from
the academy.
2. GC was progressively framed in sustainability, after being born in the industrial activity,
focussed on P2, which involved no or little connections to SD and sustainability—such
a framing has influenced ways of thinking and practices of Chemistry.
3. More recently, GC has been “aspiring” (but moving slowly) to a systems thinking frame,
as still dominated by the reductionist mindset in which the Twelve Principles were for‑
mulated and are nowadays often applied, albeit later they were considered a cohesive
system.
4. Some of the precursors of GC changed their vision on the nature of the design in
its implementation—from incremental to transformative, to allow more innovation;
however, both ways allow its development, depending on the type and context of the
problems.
With reference to what has not changed yet or needs better implementation, we identi‑
fied the following items:
1. The important problem of the validation of chemical greenness remains: greenness met‑
rics are still insufficiently used, although the use of mass metrics has been increasing;
it is recommended to the editors of GC journals that they press the inclusion of metrics
by the authors of manuscripts when these claim greenness gains, following the recent
example of ACS Sustainable Chemistry and Engineering (Allen et al. 2015).
2. The frontiers of GC research areas/themes have not deserved enough attention, perhaps
due the GC youth and growth, beside the intrinsically complex nature of Chemistry; a
better—and as clear as possible—definition of the GC conformation would allow better
following of the dynamics of its growth, evolution and evaluation and would facilitate
synergic collaborations among areas, therefore strengthening the field.
3. A more integrated vision between academy and industry is required to allow better
understanding of GC global development (theory and practice).
4. GC education requires more penetration in chemistry curricula—that is important for
expansion and consolidation.
The route of GC along its evolution is summarized graphically in Fig. 2.

In conclusion, after twenty-five years, GC has been a movement towards generalization
and amplification of efforts for simultaneously decreasing the negative impacts of chem‑
istry on environment and increasing the efficacy of functions of chemical products, pro‑
viding a more intense and proactive engagement of chemists with the movement toward
13
sustainability—although its approach to sustainability requires more reflection on its limi‑

tations, for instance those due to the Second Law of thermodynamics. Thus, the emergence
and development of GC appears to endorse Chamizo (2011) when he remarked that Chem‑
istry lives a new period of change on the emphases of scientific researches and practices,
recognizing that this is “el momento de las culpas” (the “moment for blames”) in which the
responsibilities of Chemistry for environmental damages are assumed (p. 329), the chem‑
istry addressed to the environment, including GC, being the fifth revolution of Chemistry
(Chamizo 2017).
Acknowledgements CAM thanks support of CAPES Foundation (Coordenação de Aperfeiçoamento

de Pessoal de Nível Superior, Brasil) for a sabbatical leave (2017-2018) at the Department of Chem‑
istry and Biochemistry, Faculty of Sciences, University of Porto, Portugal (Estágio Sênior no Exterior
88881.119087/2016-01).
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An Integrated Vision of The Green Chemistry Evolution Along 25 Years Marques - Machado

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Foundations of Chemistry (2021) 23:299–328

An integrated vision of the Green Chemistry evolution

Accepted: 12 January 2021 / Published online: 18 June 2021

Keyword Green Chemistry · GC evolution · GC innovation nature · GC integrated vision ·

* Carlos Alberto Marques

The Emergence phase

The divulgation phase

The important role of scientific communication in science development is well recognized

Editorials of the Green Chemistry journal

proactive implementation of sustainability. Other editorials by Clark in later issues of the

which means that chemists should develop GC to support sustainable technologies as

Editorials of the Green Chemistry letters and reviews

The consolidation phase

The Green Chemistry Journal 10th anniversary

The Green Chemistry journal 15th anniversary editorial

diversification of raw materials; replacement of noble by abundant metals in catalysts.

The Green Chemistry 25th anniversary editorials in the Green Chemistry journal

The route of GC along its evolution is summarized graphically in Fig. 2.

sustainability—although its approach to sustainability requires more reflection on its limi‑

Acknowledgements CAM thanks support of CAPES Foundation (Coordenação de Aperfeiçoamento

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