Bioresource Technology 366 (2022) 128168

Contents lists available at ScienceDirect

Bioresource Technology
journal homepage: www.elsevier.com/locate/biortech

Review

Biohydrogen in a circular bioeconomy: A critical review

Aristotle T. Ubando a, b, c, Wei-Hsin Chen d, e, f, *, Dennis A. Hurt a, Ariel Conversion a, b,
Saravanan Rajendran g, Sheng-Lun Lin h
a
Department of Mechanical Engineering, De La Salle University, 2401 Taft Avenue, 0922 Manila, Philippines
b
Thermomechanical Laboratory, De La Salle University, Laguna Campus, LTI Spine Road, Laguna Blvd, Biñan, Laguna 4024, Philippines
c
Center for Engineering and Sustainable Development Research, De La Salle University, 2401 Taft Avenue, 0922 Manila, Philippines
d
Department of Aeronautics and Astronautics, National Cheng Kung University, Tainan 701, Taiwan
e
Research Center for Smart Sustainable Circular Economy, Tunghai University, Taichung 407, Taiwan
f
Department of Mechanical Engineering, National Chin-Yi University of Technology, Taichung, 411, Taiwan
g
Departamento de Ingeniería Mecánica, Facultad de Ingeniería, Universidad de Tarapacá, Avda. General Velásquez 1775, Arica, Chile
h
School of Mechanical Engineering, Beijing Institute of Technology, Beijing 100081, China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• The utilization of a circular bioeconomy

framework to produce biohydrogen is
reviewed.
• Waste valorization and biomass con­
version into biohydrogen are viable
pathways.
• Biorefinery presents a sustainable
approach to generating biohydrogen.
• Microalgae have continued to attract
considerable interest in making
biohydrogen.
• The sustainability assessment of bio­
hydrogen is essential for
commercialization.

A R T I C L E I N F O A B S T R A C T

Keywords: Hydrogen produced from biomass feedstocks is considered an effective solution in moving toward a decarbon­
Biohydrogen ized economy. Biohydrogen is a clean energy source that has gained global attention for adoption as it promises
Biofuel to mitigate climate change and human environmental damage. Through the circular economy framework, sus­
Circular economy
tainable biohydrogen production with other bioproducts while addressing issues such as waste management is
Valorization
Biorefinery
possible. This study presents a comprehensive review of the various biomass feedstocks and processing tech­
Sustainability nologies associated with biohydrogen generation, as well as the possible integration of existing industries into a
circular bioeconomy framework. The currently standing challenges and future perspectives are also discussed.

1. Introduction resources, sustainability has increasingly become a global concern. A

concept that attempts to address this growing issue is the utilization of a
With an ever-increasing understanding of the finiteness of natural circular economy (CE). The CE framework attempts to lower resource

* Corresponding author.
E-mail addresses: weihsinchen@gmail.com, chenwh@mail.ncku.edu.tw (W.-H. Chen).

https://doi.org/10.1016/j.biortech.2022.128168
Received 13 August 2022; Received in revised form 14 October 2022; Accepted 17 October 2022
Available online 22 October 2022
0960-8524/© 2022 Elsevier Ltd. All rights reserved.
A.T. Ubando et al.
consumption and overall environmental impacts by maximizing the
service of each resource input and increasing a material’s useful life
(Velvizhi et al., 2020). In reference to a circular bioeconomy (CBE), the
inputs are derived from renewable biological resources. This means that
the innovation of this framework is about optimizing the extraction of
these resources or identifying untapped resource pools (D’Amato et al.,
2017). The products extracted from various biomass feedstocks are then
repurposed for other applications such as nutriment, biochemicals, or
bioenergy.
One of the valuable resources that can be derived from biomass is
biohydrogen (H2). Biohydrogen is one of the most attractive energy
sources, as it yields the largest amount of energy per gram of any known
fuel while producing no pollutants (Akca et al., 2021). It can be pro­
duced biologically from various biomass materials, and when burned,
the only two products yielded are water and the subsequently released
energy. Another significant aspect of this fuel is that it can be derived
from different biomass feedstocks and wastes from various industries.
Numerous approaches were implemented for industrial wastewater that
was capable of generating biohydrogen fuel (Rajesh Banu et al., 2020).
Additionally, biohydrogen can be produced through anaerobic fermen­
tation from common food wastes such as fruit peels (El Barnossi et al.,
2021).
There have been numerous reviews that have previously examined
the concept of biohydrogen within a circular economy. (Sharma et al.,
2021) discussing the current valorization possibilities for food waste and
examining it as a feedstock for bio-based products such as biofuels in a
circular bioeconomy. The utilization of various biomass materials as
potential feedstocks within this framework has also been critically
reviewed. Sar et al. (2022) reviewed the fermentation-engineering
techniques for effectively using effluents from the dairy industry, for
example. Opportunities for the valorization of the solid waste generated
from the paper and pulp industry were examined, specifically by
considering the thermal and biochemical processes involved individu­
ally and when integrated into a biorefinery framework (Gottumukkala
et al., 2016). Ghayur and Verheyen (2018) simulated five biorefinery
models, utilizing waste from post-combustion CO2 capture plants as the
potential feedstock. Several reviews concern themselves with examining
methods of aiding the biological production of biohydrogen. Two other
articles discussed the enhancement of dark fermentation production, the
first of which by means of biomass retention through calcium the dosing
of calcium, the second of which through a positive linear correlation
between the carbohydrate content of the biomass and hydrogen yield
(Alibardi and Cossu, 2016; Blanco et al., 2017). Kars and Ceylan (2013)
reviewed H2 production by Rhodobacter sphaeroides, using waste barley
as a substrate. They determined that increased sugar content in the
growth media resulted in more accumulated hydrogen. Other articles,
such as those by De Bhowmick et al. (2019), attempted to analyze the
overall development of the biofuel sector and review strategies to utilize
wastewater in a biorefinery model. In a similar light, the large quantity
of biogenic waste generated in India was recognized as a potential
feedstock and was subsequently reviewed through the lens of a CBE
(Chatterjee and Mohan, 2020).
Hydrogen production via renewable energy sources, particularly
those derived from biomass feedstocks (biohydrogen), is considered an
important key solution in fulfilling a decarbonized economy (Oliveira
et al., 2021). Varvoutis et al. (2022) conducted a review of the recent
technologies and challenges in CO2 hydrogenation. An overview of the
advantages of CO2 utilization or valorization instead of permanent
storage through carbon capture storage (CCS) and the feasibility of
global-scale decarbonization by transforming to a hydrogen-based
economy was presented. Carbon dioxide valorization via hydrogena­
tion, transforming captured CO2 into high-valued chemicals or synthetic
fuels, can lead to several economic benefits and can eventually be
exploited for the market. Mathur et al. (2022) published a review to
address the significant role of natural gas, including hydrogen, in global
industrial decarbonization. They also assessed the current and projected
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Bioresource Technology 366 (2022) 128168
financial, infrastructural, geopolitical, and governance concerns. Fig. 1
illustrates the role of biohydrogen production in a circular economy via
waste valorization and in decarbonization. The biomass feedstocks from
residuals and waste materials are pretreated before biohydrogen pro­
duction. Hydrogen and carbon dioxide are the main outputs of the
production process, which are then separated. The hydrogen product is
transported for several applications in various sectors while the sepa­
rated CO2 is prepared for storage or for utilization (Full et al., 2021a;
Full et al., 2021b). Furthermore, using hydrogen as a fuel will
completely eliminate CO2 emissions, with the only combustion
byproduct simply water (Hemschemeier et al., 2009).
With this preexisting literature in mind, there appear to be no review
studies that attempt to analyze the biorefinery models concerning uti­
lizing waste as a feedstock, with biohydrogen being the desired yield in
the circular bioeconomy. A Scopus bibliometric analysis was conducted
on the topics of “biohydrogen/bio-hydrogen,” “biohydrogen/bio-
hydrogen and biorefinery/bio-refinery,” and “biohydrogen/bio-
hydrogen, biorefinery/bio-refinery, and waste.” These search combi­
nations resulted in total scientific journal publications (Article and Re­
view) of 4096, 179, and 86, respectively (August 5, 2022). A
comprehensive review of the standing of biohydrogen production in
terms of the available feedstocks and the industry’s sustainability ap­
pears to have not been conducted. This is the reason why this study
focuses on the field of biohydrogen in a circular bioeconomy.
2. Circular bioeconomy
2.1. Circular economy and circular bioeconomy concept
The CE is a recent sustainable development model that has gained
traction with the goal of greening various industries. Inherent flaws to a
linear economy, such as resource and production efficiency, the inability
to capitalize on slower material flows, and the requirement of high
resource extraction for viability, can be addressed by implementing a
CE. It essentially allows various materials, products, and components to
be used to their highest degree of utility and value (Ari and Yikmaz,
2019). Municipalities and cities that are posed with issues such as waste,
excess emissions, effects of climate change, and sustainability can be
aided by the CE, but there are certain steps likely need to be taken to aid
its development. Public procurement of the philosophy depends on the
focus on the reuse, remanufacturing, and refurbishment of products and
materials, the integration of sustainability and CE issues in policy, and
attention to the working life of the products (Husgafvel et al., 2022).
The term bioeconomy references the production, use, and general
economic activity around biological processes and products (Brizga
et al., 2019). The convergence of bioeconomy agendas with those of a CE
with a ranging emphasis on biotechnology is referred to as a circular
bioeconomy. Both CE and CBE frameworks independently gained in­
terest in academic literature and policy after their popularization in the
1990s and 2000s. It is claimed that the trajectory of CBE is impeded by
narrow problem and solution framing and a finite number of advocates,
which lead to a more specific but less sustainable path (Hadley Kershaw
et al., 2021). Previous quantitative assessments of the development of
CBE have been tracked through specific social and economic indicators.
Kardung and Drabik (2021) overviewed several indicators to analyze the
development of EU countries’ CBE, whether they are progressing or
regressing from 2006 to 2016. The countries were classified according to
some CBE considerations: importance to the economy, agricultural
intensification, geographical coverage across the EU, and availability of
coherent data. They also highlighted an analysis of the importance of a
bioeconomy within the general German economy from 2002 to 2010,
with gross value added and employment as primary indicators.
2.2. Biomass feedstocks and biorefinery
Biomass is defined as organic material that is derived from animal
A.T. Ubando et al.
Fig. 1. The role of biohydrogen in circular economy and decarbonization via waste valorization.
manure, plants, or algae. Wood-based waste comprises the most biomass
utilized with 64 %, followed by municipal solid waste, agricultural
waste, and landfill gasses at 24 %, 5 %, and 5 %, respectively (Dha­
modharan et al., 2020). Biorefineries have been proposed to be a solu­
tion for optimizing the production of marketable bio-products by
increasing their energetic, technical, and economic efficiency. Rather
than processing biomass through stand-alone facilities with a low return
on investment, biorefineries allow for the simultaneous production of
multiple value-added products from a single source (Holm-Nielsen and
Ehimen, 2014). A prevalent hurdle in biorefineries is becoming
commercialized. This is due to its economic viability, which begins with
policy support and the logistics of procuring the necessary biomass and
competing with pre-established petrochemical products. In reference to
recent technological discussions of feasible biomass feedstocks, the
classifications of algal, lignocellulosic, and general waste appeared to be
the most prominent. Table 1 lists various categories and subsequent
biomass feedstocks that can produce biohydrogen, along with their
compositional and elemental makeup. Aside from the properties pre­
sented in the table, Luo et al. (2011a) mentioned the lower calorific
value of 15.5 GJ/t for biohydrogen derived from Rapeseed straw. And
compared to other biofuels, Hydrogen has the highest low heating value
(LHV) of 120 MJ/kg (Masilela and Pradhan, 2022).
2.2.1. Algal biomass
Algal biomass is a particularly promising substrate for producing
biofuel. Its fundamental components, such as proteins, lipids, and
starches, vary greatly depending on the strain. Algal biomass contains
three categories of microalgae, macroalgae, and cyanobacteria. Micro­
algal strains vary widely in their chemical composition, with 6–70 %
protein, 4–64 % carbohydrates, 2–50 % lipids, and 1–6 % nucleic acid
(De Bhowmick et al., 2019). Different synthesizing processes are
required depending on the algal strain and desired biofuel. Among them,
pyrolysis producing methane and biohydrogen is the most frequently
discussed endothermically thermal conversion process (Dhamodharan
et al., 2020). Microalgae have continued to attract considerable interest
in making biohydrogen, resulting from their high photosynthetic effi­
ciency and rapid growth rates (Sarkar et al., 2015). It is cultivated
widely through two primary reactor types; open ponds and closed
photobioreactor systems, whose appropriateness can vary depending on
the specific application (De Bhowmick et al., 2019).
2.2.2. Lignocellulosic biomass
Lignocellulosic biomass was traditionally used as a composting
bulking agent but has more recently found applications as a feedstock
for H2 production. It usually takes the form of a plant-based material
such as agricultural or forestry waste, energy crops, and yard trimmings.
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Bioresource Technology 366 (2022) 128168
In 2012, 340 million metric tons of lignocellulosic biomass were
accessible for use (Xu and Li, 2017). The initial challenge of processing
this form of biomass is developing an efficient method to separate its
primary components of cellulose, hemicellulose, and lignin (Merklein
et al., 2016). The production of useful biofuels such as H2 from ligno­
cellulosic biomass traditionally requires three steps: pretreatment,
enzymatic or acid hydrolysis, and fermentation (De Bhowmick et al.,
2019). Physical, chemical, or biological pretreatment is an essential step
as it plays a prominent role in the ultimate yield from biomass, and it is
frequently demonstrated that biohydrogen production from non-
pretreated substrates is substantially lower. The overall benefits of this
feedstock are its high cellulose and hemicellulose contents, renew­
ability, availability, and low cost. But it lacks competition for use in
other industries, such as animal feed or food production (Zhu et al.,
2021).
2.2.3. Waste biomass
Another primary biomass utilized in a CBE is general waste, specif­
ically biogenic waste and non-edible feedstocks. Using waste streams as
feedstock provides a significant advantage in reference to lowering
greenhouse gas emissions, production costs, and waste valorization
(Akca et al., 2021). Municipal waste is frequently discussed as an
attractive option for bioenergy production as it is produced in contin­
uous large amounts globally and is generally low cost. Organic waste is
traditionally processed through anaerobic digestion to generate value-
added products like methane and can be subjected to dark fermenta­
tion for biohydrogen production. Dark fermentation also allows for
secondary products with growing market value, such as volatile fatty
acids, carboxylic acids, and alcohols (Cesaro et al., 2020). Sar et al.
(2022) discussed dairy industry wastes and their subsequent byproducts
as a potential CBE feedstock for biohydrogen production. They stated
that the technical feasibility, the potential of techno-economic analysis,
and life-cycle assessments should be considered.
Among the three biomass feedstocks, waste was considered to have
the most advantages in expanding the boundaries of biorefinery in a
circular economy due to its availability and lower production cost
(Ubando et al., 2020). However, there are still numerous recent studies
and emerging technologies on the valorization of lignocellulosic and
algal feedstocks because of their greater advantages in terms of envi­
ronmental and social aspects and their vital roles in rapid decarbon­
ization (Yadav and Mondal, 2021).
2.3. Valorization
Valorization is defined as the enhancement of a component’s value,
status, or price. It takes place when the higher cost s of energy resources
A.T. Ubando et al. Bioresource Technology 366 (2022) 128168

Table 1
Biomass feedstocks used in biohydrogen production with the corresponding compositional and material properties.
Classification Feedstock Compositional Analysis Elemental Analysis References

Waste Waste activated sludge (WAS) pH (6.9 ± 0.2)

Excess Sludge
Fruits-and-vegetable waste
Corn stover
Waste barley
Cellulose based municipal waste
Cheese whey
Food scraps and woody-based
fraction
Tangerine peel waste
Pomegranate peel waste
Banana peel waste
Naresh Kumar and Venkata Mohan (2018)
Carbohydrates (162 ± 0.6 mg/l)
SCOD (1240 ± 0.4 mg/l)
TSS (28.4 ± 0.2 g/kg)
VSS (22.4 ± 0.3 g/kg)
pH (7.1 ± 0.3)
Zhang et al. (2022)
SCOD (345.6 ± 10.7 mg/L)
TSS (25460 ± 420 mg/L)
VSS (18660 ± 178 mg/L)
TCOD (27570 ± 27570 mg/L)
Total protein (12300 ± 275 mg/L)
Total polysaccharides (5160
± 489 mg/L)
pH (5.52) Carbon (51.69 %) Rodríguez-Valderrama et al. (2020a,
TS (10.19 %) Hydrogen (3.43 %) 2020b)
VS (87.66 %) Oxygen (42.69 %)
Ashes (12.34 %) Nitrogen (2.19 %)
Cellulose (12.8 %)
Hemicellulose (23.4 %)
Lignin (10.26 %)
Protein (12.63 %)
Extractives (38.1 %)
pH (7.54) Carbon (43.84 %) Rodríguez-Valderrama et al. (2020a,
TS (94.59 %) Hydrogen (15.74 %) 2020b)
VS (89.78 %) Oxygen (39.98 %)
Ashes (10.22 %) Nitrogen (0.44 %)
Cellulose (33.25 %)
Hemicellulose (24.35 %)
Lignin (24.74 %)
Protein (3.25 %)
Extractives (10.19 %)
Protein (11.19 ± 0.46 %)
Kars and Ceylan (2013)
Fat (2.45 ± 0.035 %)
Starch (37.5 ± 0.49 %)
Carbon (29.93 %) Agarwal et al. (2013)
Hydrogen (4.18 %)
Oxygen (1.96 %)
Nitrogen (0.12 %)
Sulfur (63.81 %)
pH (6.42)
Dessì et al. (2020)
TS (69.98± 1.94 %)
VS (64.04 ± 1.76 %)
TSS (1.18 ±0.11 %)
VSS (1.17 ± 0.05 %)
pH (6.4 ± 0.3)
Cesaro et al. (2020)
TS (78.5 ± 2.3 %)
VS (22.8 ± 0.7 %)
SCOD (33.1 ± 7.7 g/L)
Carbohydrates (18.8 ± 1.9 %)
Protein (11.9 ± 3.1 %)
pH (4.27)
El Barnossi et al. (2021)
Moisture (2.50 ± 0.10 %)
Proteins (8.55 %)
Lipids (2.97 %)
Crude fibers (12.80 %)
Ash (2.88 %)
Carbohydrates (18.03 %)
pH (4.83)
El Barnossi et al. (2021)
Moisture (7.06 ± 0.07 %)
Proteins (3.26±0.14 %)
Crude fibers (34.0 %)
Ash (3.31± 0.05 %)
Carbohydrates (86.52± 0.18 %)
pH (6.23)
El Barnossi et al. (2021)
Moisture (9.80 %)
Proteins (5.13± 0.14 %)
Lipids (1.70 ±0.10 %)
Crude fibers (31.70± 0.25 %)
Ash (5.01 %)
Carbohydrates (59.0± 1.36 %)

Lignocellulosic Rapeseed straw TS (92.6 ± 0.02 %)

Luo et al. (2011a, 2011b)
VS (89 ± 0.02 %)
Proteins (10.5 ± 0.19 g/L)
(continued on next page)

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A.T. Ubando et al. Bioresource Technology 366 (2022) 128168

Table 1 (continued )
Classification Feedstock Compositional Analysis Elemental Analysis References

Lipids (1.6 ± 0.01 g/L)

Xylose (20.2 ± 0.3 %)
Glucose (44.4 ± 0.1 %)
Lignin (25.8 ± 0.1 %)
Dairy manure Carbon (50.51 %) Zhu et al. (2021)
Nitrogen (3.03 %)
Phosphorus (0.810 %)
Calcium (2.41 %)
Potassium (1.24 %)
Magnesium (0.966 %)
Cassava wastewater pH (3.6–6.2) Nitrogen (2.3 g/L) Zhang et al. (2016)
TS (4.5 – 38.2 g/L) Phosphorous (70–780 mg/
VS (2.4 – 33 g/L) L)
TCOD (8.0 – 66.2 g/L)
SCOD (14.2 – 34.5 g/L)
Carbohydrates (9.6–37.5 g/L)
Oil and grease (0.6 g/L)
Protein (2.3 g/L)
Cassava bagasse Starch (40.1–75.1 %) Zhang et al. (2016)
Crude fiber (14.9 – 50.6 %)
Cellulose (4.1 – 11.4 %)
Hemicellulose (4.2 – 8.3 %)
Lignin (1.2 %)
Total ash (0.7–11.9 %)
Crude fat (0.5 – 1.1 %)
Crude protein (0.3 – 1.6 %)
Barley straw Cellulose (36 – 43 %) De Bhowmick et al. (2019)
Hemicellulose (24 – 45.6 %)
Lignin (6.3 – 9.8 %)
Corn cob Cellulose (32.3 – 45.6 %)
Hemicellulose (39.8 %)
Lignin (6.7 – 13.9 %)
Corn stover Cellulose (35.1 – 39.5 %)
Hemicellulose (20.7 – 24.6 %)
Lignin (11 – 19.1 %)
Rice straw Cellulose (29.2 – 34.7 %)
Hemicellulose (23 – 25.9 %)
Lignin (17–19 %)
Rice husk Cellulose (28.7 – 35.6 %)
Hemicellulose (11.96 – 29.3 %)
Lignin (15. 4–20 %)
Wheat straw Cellulose (35–39 %)
Hemicellulose (22–30 %)
Lignin (12–16 %)
Sugarcane bagasse Cellulose (25–45 %)
Hemicellulose (28–32 %)
Lignin (15 – 25 %)
Switchgrass Cellulose (35 – 40 %)
Hemicellulose (25 – 30 %)
Lignin (15 – 20 %)
Oat straw Cellulose (31 – 35 %)
Hemicellulose (24 – 27 %)
Lignin (10 – 15 %)
Sorghum straw Cellulose (32 – 35 %)
Hemicellulose (24 – 27 %)
Lignin (10 – 15 %)
Hardwood stems Cellulose (40 – 55 %)
Hemicellulose (24 – 40 %)
Lignin (18 – 25 %)
Softwood stems Cellulose (45 – 50 %)
Hemicellulose (25 – 35 %)
Lignin (25 – 35 %)
Nut shells Cellulose (25 – 30 %)
Hemicellulose (25 – 30 %)
Lignin (30 – 40 %)
Miscanthus Cellulose (10 %)
Hemicellulose (12.5 %)
Lignin (16 %)

are compensated by even higher perceived and paid worth of energy
products (Krozer, 2017). In the case of biomass valorization, value is
added to various types of plants and residues, such as those discussed in
the previous three sections. The conversion process to value-added
products is conducted through biological or thermochemical conver­
sion processes, each of which has its own defined drawbacks. Biological
processes are usually associated with a lack of stability, low product
yield, and long processing time, whereas thermochemical processes
frequently generate products that are difficult to dispose of (Okolie
et al., 2022). Several biohydrogen production studies on valorization
processes of various biomass are listed in Table 3, in which the common
byproducts are also listed, which can be further marketed. In addition,

5
A.T. Ubando et al.
Table 2
The different methodologies for assessing the sustainability of biohydrogen production.
Classification Sustainability Performance Index Methodology
Algae Green house gas emissions, Economic assessment
energy demands, climate change
Waste (tangerine, Recovery of valuable products Environmental and social
pomegranate, and from waste, environmental sustainability assessment
banana peels) impact, human health
Waste (fruits-and- Production costs, cost to revenue Techno-economic
vegetable waste and ratio, fossil fuel depletion, assessment, profitability
corn stover) climate change. analysis
Lignocellulosic (Cassava Renewable resource demand, Techno-economic
waste) mitigating waste production, analysis
food insecurity.
Table 4 comments on the valorization processes and circular bio­
economy. It is a common theme that the valorization of biomass feed­
stocks, for example, in Gottumukkala et al. (2016) with paper sludge,
required the integration of multiple bioprocesses in the form of a CE or
biorefinery concept. The potential negative impact on human health and
the environment results from the inappropriate valorization of wastes.
Soil organisms may undergo organic amendments, and the accumula­
tion of pollutants can occur with an excessive application of lower-
quality composts, affecting living microbes in the soil and piling heavy
metals (El Barnossi et al., 2021). Though part of these wastes, such as
from tangerine, pomegranate, and banana fruits, are used directly as
animal feed or organic soil fertilizers, most of them are just disposed of
in landfills which pose serious environmental hazards (Krčmar et al.,
2018; Tenodi et al., 2020). As a result, these landfills can have a number
of detrimental effects on human health either by direct or indirect
contact with the polluted soil, contaminated air, ground, or surface
water (Tenodi et al., 2020). If the disposed of wastes are inadequately
valorized, the negative effects on human health include birth defects,
low birth weight, neurological related diseases, nausea and vomiting
(Liu et al., 2015), respiratory diseases (Heaney et al., 2011), and
increased risk of cancer (Mattiello et al., 2013; Porta et al., 2009).
2.4. Dark fermentation
Fig. 2 shows the different biohydrogen production processes. One
option for the biological production of H2 is dark fermentation (DF), as
shown in Fig. 1. It is a process carried out by obligate and facultative
anaerobes in the absence of oxygen and light (Kamran, 2021). The
substrate required for this process are the biomass feedstocks discussed
previously, where the efficiency of the dark fermentation is significantly
dependent on their pretreatment, sugar content, and the microorgan­
isms involved (Ghimire et al., 2015). Facultative or obligate anaerobic
bacteria such as Escherichia coli, Citrobacter intermedius, Enterobacter
cloacae, Bacillus species, and Clostridium beijerinckii, are few common
examples of microorganisms that are involved in DF (Cheonh et al.,
2022; Koutra et al., 2020; Singh and Sarma, 2022). The resulting
breakdown of the feedstock during DF are the production of hydrogen,
organic acids and alcohol (Rizwan et al., 2019), which can be further
processed and marketed as high-valued products. DF has become
particularly promising in producing H2 as it may be applied to a wide
array of organic wastes in both solid and liquid forms (Koutra et al.,
2020). It does not require luminous energy, can be conducted in non-
sterile environments, and has a relatively high hydrogen production
rate (Ghimire et al., 2015; Rodríguez-Valderrama et al., 2020a; Zhu
et al., 2021) that makes DF an effective and cost-efficient approach
(Singh and Sarma, 2022) with production cost that is estimated to be
6
Bioresource Technology 366 (2022) 128168
Circular Bioeconomy Comments References
Costs can be reduced through utilizing a closed circular De Bhowmick
bioeconomy, in which microalgae cultivated using wastewater et al. (2019)
allowed for CO2 mitigation and production of high value
products
Research is required to alter perceptions of fruit peels as waste El Barnossi et al.
to that of a valuable resource for implementation in the (2021)
bioeconomy
Co-digestion of biomass aid in the development of biorefinery Rodríguez-
models through means such as improving supply chain Valderrama et al.
management, avoiding seasonality and lack of nutrients. (2020)
Adoption of a biorefinery concept for cassava-based waste Zhang et al. (2016)
mitigate the need for specific dedication of land to bioenergy
crops.
340 times lower than the other photosynthetic methods (Antonopoulou
et al., 2011). In addition, building blocks such as volatile fatty acids are
generated and can be used in downstream applications (Dessì et al.,
2020).
The common feedstocks listed in Table 3 that involved dark
fermentation are waste products and lignocellulose, which normally
require inoculation and pretreatment processes. Some of the existing
pretreatment processes are listed in the table. Among these are hydro­
lysis (Rodríguez-Valderrama et al., 2020a), sterilization (Marone et al.,
2015), steam-heated pretreatment (Cheng et al., 2015), and dry-bath
heat pretreatment (Dessì et al., 2020). Pretreatment of biomass is typi­
cally carried out prior to the fermentation process to enhance the di­
gestibility of the biomass and increase its biohydrogen yield as well as
the subsequent biofuel yields (Cheng et al., 2015). The operational
conditions during dark fermentation are commonly either mesophilic
(37 ± 2 ◦ C) or thermophilic condition (55 ± 2 ◦ C). Zhang et al. (2015)
performed a test on dark fermentation of corn stover hydrolysate at
extreme thermophilic conditions (70 ◦ C), but the biohydrogen yield was
lower than that of thermophilic conditions. Moreover, the common
byproducts of biohydrogen production are acetic acid, butyric acid,
volatile fatty acids (VFA), lactic acid, and propionic acid.
2.5. Pyrolysis
The chemical decomposition of organic materials by the application
of heat in the absence of oxygen is referred to as pyrolysis and is another
method for producing biohydrogen (Vallero, 2008). A variety of biomass
feedstocks can be used in this process, with the final quality of the
product and the distribution being dependent on the pyrolytic temper­
ature, residence time, heating rate, and the type of feedstock and reactor
used (Sarkar et al., 2015). In most instances, various processes, such as
transesterification, gasification, lipid extraction, and anaerobic diges­
tion, are combined with pyrolysis to be more economical (Kumar et al.,
2020).
2.6. Sustainability assessment
A broad definition of a sustainability assessment translates to direct
decision-making in a process towards achieving development that is
sustainable, with an alternative definition being the consideration of
local and global proportions with long- and short-term perspectives to
integrate natural and societal systems (Hou and O’Connor, 2020). An
application of this assessment providing an insight into the feasibility of
the process is examined in terms of environmental, economic, and social
aspects. De Bhowmick et al. (2019) attempted to view the sustainability
of algal feedstocks in a biorefinery concept through four categories of
A.T. Ubando et al. Bioresource Technology 366 (2022) 128168

Table 3
Biohydrogen production and byproducts with corresponding conversion technologies and operational conditions.
Feedstock Inoculum Conversion Temperature Hydraulic H2 Production Byproducts References
Technologies (◦ C) retention Yield
time

Municipal waste (60 % Activated Semi-continuous 55 21 days 1.641 mmol H2/ Acetic acid and butyric acid (Escamilla-
food waste, 40 % sludge hydrogenogenic g-VS Alvarado et al.,
waste office paper) fermentation 2013)

Corn stover Activated Dark fermentation 55 2h 6.08 mmol-H2/g Furan derivatives and (Zhang et al., 2015)
hydrolyzate: sludge Dark fermentation 55 utilized sugar phenolic compounds
Anaerobic 7.74 mmol-H2/g
granular sludge utilized sugar

Agro-industrial waste: Anaerobic Anaerobic digestion 37 3 days 0.54 mol H2/ Volatile fatty acids, lactic (Dareioti and
olive mill wastewater digested sludge mol acids, alcohols Kornaros, 2014);
(55 %), cheese whey carbohydrates Naresh Kumar and
(40 %), liquid cow Venkata Mohan
manure (5 %) (2018)

Agro-industrial waste: Anaerobic Anaerobic digestion 37 18 h 0.64 mol H2/ Volatile fatty acids, lactic (Dareioti et al.,
olive mill wastewater digested sludge mol glucose acids, acetic and butyric 2014)
(55 %), cheese whey acid, and ethanol
(40 %), liquid cow
manure (5 %)

Cassava wastewater Facultative Dark fermentation 28 2h 1.91 mol H2/ Ethanol, acetic acid, butyric (Amorim et al.,
pond sludge mol glucose acid, and propionic acid 2014)

Fruits-and-vegetables Anaerobic Hydrolysis 35 30 days 1.91 mol H2/ Furfural, 5-hydroxymethyl- (Rodríguez-
waste and corn stover digested sludge pretreatment and mol glucose furfural (HMF), formic acid, Valderrama et al.,
dark fermentation acetic acid, propionic acid, 2020a)
succinic acid, and lactic
acid

Buffalo slurry Lagoon Sterilization and 37 15 min 117 mL H2/g vS Butyric acid, acetic acid, (Marone et al.,
sediments dark fermentation of substrate formic acid, propionic acid, 2015)
and lactic acid

Cheese whey and Anaerobic Dark fermentation 55 8 days 152 mL H2/g vS Lactic acid, acetic acid, (Ghimire et al.,
Buffalo manure digested sludge of substrate propionic acid, and butyric 2017)
acid

Cassava residues Hydrogen Steam-heated 35 120 h 106.2 mL H2/g Methane, acetate and (Cheng et al., 2015)
producing pretreatment and VS butyrate
bacteria (HPB) dark fermentation

Cheese whey Local cheese Anaerobic packed 30 24 h 1.1 mol H2/mol Acetic acid, lactic acid, and (Perna et al., 2013)
production bed reactor lactose butyric acid
factory

Cheese whey Activated or Dry-bath heat 35 24 h 0.9 mol H2/mol Volatile fatty acids, high- Dessì et al. (2020)
digested sludge pretreatment and glucose purity butyric acid, ethanol
from dairy dark fermentation
indsutry

Algal (Heterotrophically _ Solar drying (SL), 800 3h 110.5 mL H2/g Fatty acid methyl ester Sarkar et al. (2015)
cultivated from mixed lipid extraction (SL)
consortia) (LEMA) and pyrolysis 100 mL H2/g
(LEMA)

*Note: Volatile solids (VS); Without sand additive or sand less (SL); Lipid extracted microalge (LEMA).

sustainability, hurdles in technological development, economic affairs,
and environmental concerns. Table 2 lists some of the sustainability
assessment methodologies of previous studies for biohydrogen
production.
2.6.1. Life cycle assessment
One technique for assessing the environmental aspects of a product
over its usable period is a life cycle assessment (LCA). There are four
stages of an LCA study, determining the goal and scope, inventory
analysis which describes material and energy flows concerning the
environment, impact assessment, and critical review. This method al­
lows for determining the available life cycles with the least environ­
mental impact, the priorities of industry and public organizations, and
important indicators (Muralikrishna and Manickam, 2017). There
currently appear to be very few LCAs of biohydrogen in a circular
economy; however, it is frequently recommended that it be conducted to

7
 A.T. Ubando et al.
Table 4
Case studies of biohydrogen production in a circular bioeconomy.
Classification Biomass Strategic Technology Valorization Location Circular Bioeconomy Comments References

Algal Microalgae (deoiled algal Hydrothermal acid treatment and Wastewater treatment with simultaneous H2 and India Generation of value-added products under Venkata Subhash and
cake) acidogenic fermentation biodiesel production and extraction of volatile biorefinery approach. Venkata Mohan (2014)
fatty acids.

Algal Microalgae Pyrolysis Domestic wastewater recovered for biogas, bio- n.d. Environmental sustainability in biorefinery Sarkar et al. (2015)
(heterotrophically oil, and bio-char. framework displayed in integration of thermos-
cultivated) chemical and microalgae cultivation processes.

Algal Microalgae (multiple) Pretreatment and saccharification, Biodiesel, biohydrogen, and biofertilizer n.d. Coupling of multiple processes allows for more Kumar et al. (2020)
fermentation, gasification, pyrolysis, production form algal biomass. economical production.
hydrothermal liquefaction, and
anaerobic digestion

Algal/ Algal, lignocellulosic, and Pretreatment, hydrolysis, fermentation, Production of value-added products. n.d. Co-production of multiple biofuels as well as De Bhowmick et al.
Lignocellulosic/ general waste anaerobic digestion. other value-added products lead to more (2019)
Waste sustainable approach.

Lignocellulosic Fruits-and-vegetables Dilute acid hydrolysis pretreatment, dark Biohydrogen production from waste. Mexico Co-processing of multiple feedstocks in Rodríguez-Valderrama
wastes and corn stover fermentation biorefinery model. et al. (2020a, 2020b)

Lignocellulosic Cotton-seed cake Alkaline pretreatment, enzymatic Biodiesel and biohydrogen production from Greece Biodiesel can potentially be served in addition Panagiotopoulos et al.
hydrolysis, fermentation. cotton waste. to production of biohydrogen in biorefinery (2013)
concept.
8

Lignocellulosic/ Waste barley Acid hydrolysis, photo fermentative Biohydrogen production from waste with n.d. Effective use of feedstocks in economical Kars and Ceylan (2013)
Waste hydrogen production via non-sulfur simultaneous production of 5-aminolevulinic process can be optimized through an integrated
bacteria acid biorefinery concept.

Lignocellulosic/ Rapeseed plant Alkaline peroxide pretreatment, Bioethanol production with byproducts of Denmark Producing multiple products takes advantage of Luo et al. (2011a,
Waste enzymatic hydrolysis and fermentation rapeseed cake, glycerol, hydrolysate, and stillage maximizing value derived from biomass. 2011b)
used for hydrogen and methane production

Lignocellulosic/ Waste sawdust Dark and photo fermentation Solid waste reduced by converting to lignin and Australia Industrial ecosystem of post-combustion CO2 Ghayur and Verheyen
Waste biohydrogen capture plant with hydrogen biorefinery (2018)
maximizes value of biomass.

Lignocellulosic/ Dairy manure Acid pretreatment, dark fermentation. Pollutant utilized as feedstock for multiple n.d. Utilizing renewable biomass in biorefinery Zhu et al. (2021)

Bioresource Technology 366 (2022) 128168

Waste bioproducts and acids. technology may offer sustainable solution for
energy crisis.

Waste Waste activated sludge Alkaline-catalyzed physiochemical Waste treatment with additional production of n.d. Significant growth in biobased economy can be Naresh Kumar and
pretreatment, acidogenic fermentation biohydrogen and short chain carboxylic acids. achieved by utilizing existing biological Venkata Mohan (2018)
wastewater treatment in biorefinery
framework.

Waste Excess Sludge Anthraquinone-2-sulfonate additive, Biohydrogen derived from waste China Traditional wastewater treatment processes are Zhang et al. (2022)
dark fermentation. a burden to operators.
(continued on next page)
 A.T. Ubando et al.
Table 4 (continued )
Classification Biomass Strategic Technology Valorization Location Circular Bioeconomy Comments References

Waste Food waste Anaerobic membrane reactor, Biohydrogen and volatile fatty acids derived Turkey Commercialization of biohydrogen production Akca et al. (2021)
fermentation. from waste can be improved through co-production of
VFAs.

Waste – Anaerobic structured-bed reactor, dark Biohydrogen derived from waste n.d. Efficient hydrogen production levels can be Blanco et al. (2017)
fermentation achieved through coupling H2 production to
wastewater management.

Waste Kitchen based vegetable Pyrolysis Multiple energy outputs from single waste India Utility of municipal waste for pyrolysis is viable Agarwal et al. (2013)
waste biomass for the addressing of multiple energy needs.

Waste Cheese whey Dark fermentation Biohydrogen generation with simultaneous n.d. The European union adopted an updated Dessì et al. (2020)
generation and extraction of volatile fatty acids bioeconomy strategy to achieve sustainable
growth and environmental goals.

Waste Organic solid waste (food Formic acid pretreatment, dark Bioenergy, biochemicals, and value-added n.d. Novel waste management strategy perfectly fits Cesaro et al. (2020)
scraps and woody-based fermentation. products generated from municipal solid waste. circular economy principles via waste to
reside) bioproduct supply chain.

Waste Dairy waste Anaerobic treatment, fermentation. Traditionally disposed waste can be recovered as n.d. Contributions to the bioeconomy can be made Sar et al. (2022)
microbial products for bioproduct generation. by integrating wastes into biorefinery.
9

Waste Residual fermented solid Dark fermentation Biodiesel byproducts used to generate H2, with n.d. Circular economy concepts encourage Buback dos Santos et al.
(enzymatic biodiesel H2 byproducts utilized for methane obtainment. researchers to optimize use of raw materials (2021)
byproduct) with low waste generation and multiple
product obtainment.

Waste Food waste Acidogenic fermentation Biohydrogen production from waste with n.d. Integrated multistage process may optimize Amulya et al. (2015)
polyhydroxyalkanoates production for VFA simultaneous waste remediation and value-
byproducts. added product generation.

Waste Cassava waste Anaerobic digestion Bioconversion into value-added products. n.d. Adoption of biorefinery concept simultaneously Zhang et al. (2016)
reduce food insecurity and need for land
expansion.

Waste Nitrogen and phosphorous Application of microalgae-bacteria Dual goals of bioenergy production and nutrients n.d. Downstream process used for producing Zhang et al. (2021)
wastewater consortia removal from wastewater. bioenergy.

Bioresource Technology 366 (2022) 128168

Waste Hydrogen production Dark fermentation Recovery of value-added products from n.d. Biomass is used as alternative to petroleum raw Sarma et al. (2015)
liquid waste hydrogen production effluents. materials in biorefinery concept.

Waste Industrial wastewater Microbe application and dark Biohydrogen and value-added products derived n.d. Coupling process considered most appropriate Rajesh Banu et al.
fermentation from wastewater. biorefinery route for H2 production. (2020)

Waste Municipal wastewater Microbial electrolysis cells and dark Biohydrogen, biofuels, and value-added products n.d. Viable approach for efficient H2 production Lu and Ren (2016)
fermentation. derived from wastewater with system integration.

(continued on next page)

A.T. Ubando et al. Bioresource Technology 366 (2022) 128168

validate economic feasibility (Rajesh Banu et al., 2020). Cvetković et al.

El Barnossi et al. (2021)

(2021); Wang et al. (2022) presented an analysis of the energy flows in

Kumar Awasthi et al.

Sharma et al. (2021)

Chandrasekhar et al.
Gottumukkala et al.
the life cycle of biogas as used for biohydrogen production. It was found

Chia et al. (2020)

that the process of producing hydrogen using biogas steam reforming
has a negative balance and is not energy-sustainable. Wang et al. (2022)
References

discovered through their LCA study that the subsequent generations of

(2016)

(2022)

(2020)
byproducts from biohydrogen production have an impact on the life-
cycle implications. They suggested that there would be further recov­
ery systems of byproducts to make the biohydrogen production from

Diverse H2 production processes integrated can

into bioeconomy concept to utilize all fractions.

upon the use of potential technologies for food

valorization may improve carbon conversion.

Circular bioeconomy can only be sustainable

There is further need to innovate biorefinery lignocellulosic biomass more environmentally sustainable.
increases sustainability and environmental

become an efficient contributor to circular

Production of bioenergy and bioproducts
simultaneous with wastewater treatment

conversion into value-added products

2.6.2. Techno-economic analysis

Biorefinery is promising approach to

Biorefinery context for paper sludge

The intersection of economic evaluation with engineering and pro­

Circular Bioeconomy Comments

cess modeling is referred to as a techno-economic evaluation or techno-

economic analysis (TEA). This tool helps provide the appropriate di­
rection for the development, investment, research, and policy, along
waste valorization.

with assessing the overall economic viability of the examined process.

Few articles conduct a TEA relating to the production of H2. Gottu­

bioeconomy.
mukkala et al. (2016) investigated a paper sludge biorefinery’s energy
and economic efficiency, specifically utilizing simulation software such
impact.

as WinGEMS to analyze anaerobic digestion implementation. Indicators

such as payback period and internal rate of return aided in conveying
which of several tested processes is the optimal solution. Nouwe Edou
Malaysia
Location

and Onwudili (2022) utilized ASPEN Process Economic Analyzer soft­

n.d.

n.d.

n.d.

n.d.

n.d.

ware to present techno-economic modeling of four thermochemical

technologies, which include fluidized bed (FB) gasification, fast
pyrolysis-FB gasification, fast pyrolysis-steam reforming, and steam
Bio-based products, biofuels, and bioproducts
Bioproducts and valuable acids derived from
Bioenergy and value-added products derived

resulting effluents contributing to additional

reforming of biogas from anaerobic digestion (AD). The produced

Bioethanol, biogas, and biohydrogen from

Biohydrogen production from waste with

hydrogen was for over 2000 public transport buses in West Midlands
region, UK. Mahmod et al. (2021) used SuperPro Designer to perform a
techno-economic analysis on the proposed two-stage anaerobic system
to convey its viability in producing BioH2 and biomethane from a palm
Biofuel derived from waste.

biofuels and biochemicals.

oil mill effluent that is obtained locally. Moreover, Rajendran and Han
(2022) conducted a techno-economic analysis of integrated poly­
derived from waste

hydroxyalkanoates (PHAs) and biofuels, including biohydrogen from

valorized peels.

food waste.
Valorization

from waste.

In Table 2, the comments on the circular economy, particularly on

techno-economic analysis for algae, waste, and lignocellulosic biomass,
waste.

are summarized. Judd et al. (2017) concluded and as cited in De

Bhowmick et al. (2019), that costs have been reduced by 35–86 % as a
result of microalgae cultivation using wastewater nutrients and reducing
Anaerobic digestion and fermentation

CO2 emissions while producing biofuels and high-value products,

Fermentation, pyrolysis, anaerobic

Ultrasonic and microwave assisted

including biohydrogen, in a closed circular biorefinery. For waste,

Rodríguez-Valderrama et al. (2020a) commented that production prof­
Dark fermentation, pyrolysis
Acid pretreatment and dark

itability can be increased if byproducts from dark fermentation, such as

organic acids and solvents, are further processed or sold. Moreover, for
Strategic Technology

Dark fermentation

lignocellulosic biomass, Zhang et al. (2016), emphasized the need for

adopting a biorefinery concept for cassava-based industries to produce
fermentation.

high-value bioproducts while reducing possible food insecurity.

extraction
digestion.

The goal of much research is also to produce biohydrogen at prices

that are commercially competitive. By ensuring the inexpensive avail­
ability of biomass, circular bioeconomy approaches improve the prof­
itability of biohydrogen production (Pathy et al., 2022). Fig. 3 shows the
Tangerine, pomegranate,

biohydrogen production cost and selling price as mentioned in the

Palm oil mill effluent

published studies with techno-economic analysis. The production cost

and selling price of biohydrogen vary with the conversion process
Organic waste
banana peels
Paper sludge

involved. From the techno-economic model of Nouwe Edou and

Dairy waste

Food waste

Onwudili (2022), with wood pellets as the feedstock, the selling prices of
Biomass

bioH2 from FB gasification, pyrolysis gasification, and pyrolysis

reforming were USD 3.40/kg, USD 4.83/kg, and USD 7.30/kg, respec­
Table 4 (continued )

tively. Using food and agricultural wastes through AD-biogas reforming

process, the selling price of bioH2 was USD 4.20/kg. The prices are also
Classification

fluctuating due to the climate of fuel prices.

Waste

Waste

Waste

Waste

Waste

Waste

10
A.T. Ubando et al. Bioresource Technology 366 (2022) 128168

Fig. 2. The biohydrogen production processes.

Techno-economic studies:

Lee (2016)
Hosseinzadeh et al. (2022)
Lee (2016)
Dinesh et al. (2018)
Yun et al. (2018)
Nouwe Edou and Onwudili (2022)
Nouwe Edou and Onwudili (2022)
Nouwe Edou and Onwudili (2022)
Nouwe Edou and Onwudili (2022)
Qyyum et al. (2022)
Qyyum et al. (2022)
Rajendran and Han (2022)
Rajendran and Han (2022)

Fig. 3. The biohydrogen production cost and selling price from techno-economic studies. Techno-economic studies:, Lee (2016), Hosseinzadeh et al. (2022), Lee
(2016), Dinesh et al. (2018), Yun et al. (2018), Nouwe Edou and Onwudili (2022) , Nouwe Edou and Onwudili (2022), Nouwe Edou and Onwudili (2022), Nouwe
Edou and Onwudili (2022), Qyyum et al. (2022), Qyyum et al. (2022), Rajendran and Han (2022), Rajendran and Han (2022).

3. Circular economy on biohydrogen production case studies 3.1. Algal biomass

The relevant case studies are divided into classifications based on the
three types of feedstocks found throughout the various papers: algal,
lignocellulosic, and waste. Table 3 shows several biohydrogen produc­
tion data, including the different substrates and the inoculum source,
conversion technologies, operational conditions, the corresponding
biohydrogen yield, and the byproducts. Fig. 4a also shows the summary
of several biohydrogen production molar yields from various studies. It
can be observed that higher yields were achieved so far from sucrose and
lactose. There are several studies using glucose as substrate concentra­
tion, and the biohydrogen production yield has ranged only from 0.3 to
2.4 mol H2 since the year 2000. Moreover, Fig. 4b is the plot of bio­
hydrogen production yield per volatile solids of the substrate. Concetti
et al. (2013) were able to produce a very high yield of 170 mL H2/g vS
from buffalo manure. The specifics of the case studies and their contri­
butions to the insight into valorization and circular bioeconomy are
further displayed in Table 4.
Algae biomass shows biohydrogen production potential due to its
high photosynthetic efficiency and rapid growth rate. It has rarely been
the primary focus of advanced studies. There are numerous advantages
of algae and other cyanobacteria for biomass cultivation to be used in a
CBE. It allows for water to be used as an electron donor for oxygenic
photosynthesis. It provides high productivity of biomass per acre
compared to other common crops and does not require arable agricul­
tural land. It also is capable of growth in a multitude of water bodies,
and it can be utilized to generate a wide range of useful products. In
addition, it is not subjected to the frequently referenced food versus fuel
debate as it is a nonfood feedstock (Kumar et al., 2020). The efficiency
and overall feasibility of biofuel production from algal biomass depend
on the extraction process. Sarkar et al. (2015) displayed several other
factors that affected the H2 yield in an experiment using freshly har­
vested and lipid-extracted microalgae for pyrolysis. The biomass nature,
the use of sand additives, and the pyrolytic retention time and

11
A.T. Ubando et al.
Fig. 4. Biohydrogen production yield reported in various studies: (a) molar H2 yield, (b) volumetric production yield per gram of volatile solids (VS) of substrate.
(See above-mentioned references for further information.)
temperature influenced the final biohydrogen yield. The addition of
sand displayed a significant increase in H2. In reference to dark
fermentation, the specific pretreatment strategy of the algal biomass
appeared to optimize the overall biohydrogen yield. Pretreated biomass
displayed a higher rate of hydrogen production than non-pretreated,
with algal pretreated extract having a higher production rate, cumula­
tive hydrogen production, and specific hydrogen yield than other pre­
treatment conditions (Venkata Subhash and Venkata Mohan, 2014).
3.2. Lignocellulosic biomass
Lignocellulosic components appear to be a highly esteemed option
12
Bioresource Technology 366 (2022) 128168
for H2 production, resulting from their high abundance and potential for
bioprocessing. The barrier to commercialization, however, remains in
the required pretreatment which is estimated to constitute a third of the
total cost. Panagiotopoulos et al. (2013) selected alkaline pretreatment
for cotton-seed cake due to its high yield-to-cost ratio and concluded it to
be a suitable method for biohydrogen production. Co-digestion of
lignocellulosic biomass in dark fermentation has been investigated, with
the ratio of the utilized materials showing an effect on final H2 yield.
Fruits-and-vegetable waste was efficiently fermented with corn stover;
however, the concentration of sugars due to the specific acid pretreat­
ment had a significant influence (Rodríguez-Valderrama et al., 2020a).
Waste barley utilized as a substrate post-acid hydrolysis showed promise
A.T. Ubando et al.
for the simultaneous generation of biohydrogen and 5-aminolevulinic
acid through the implementation of rhodobacter sphaeroides O.U.001
(Kars and Ceylan, 2013). The co-production of hydrogen and methane
from whole rapeseed plants was displayed to be stable, with an increase
from 20 % to 60 % in energy recovery when utilized in a biorefinery
concept rather than conventional biodiesel processes (Luo et al., 2011a).
Five hydrogen biorefinery models were evaluated using sawdust as the
feedstock to determine the optimal process for maximizing the value of
the biomass (Ghayur and Verheyen, 2018). Dairy manure was deter­
mined to also be a suitable feedstock for a biorefinery following research
to overcome bottlenecks such as pretreatment (Zhu et al., 2021).
3.3. Waste biomass
The utilization of wastes and effluent streams for biohydrogen pro­
duction offers inherent benefits due to the necessity of their treatment
for environmental purposes. The valorization of the many forms of waste
is particularly attractive. However, similarly to the previously discussed
biomass, it hinges on the efficiency of the harvesting and treatment
required. The papers examined the general categories of waste: food,
agricultural, municipal, and industrial.
3.3.1. Food waste
Food waste constitutes a large portion of waste generated worldwide,
with traditional disposal techniques including landfilling and incinera­
tion. Due to the inherent environmental impacts of these strategies and a
loss of possible valorization, many technologies for biohydrogen pro­
duction using food waste biomass have been investigated. The co-
production of biohydrogen and volatile fatty acids (VFA) via dark
fermentation and anaerobic membrane bioreactors displays the most
efficient H2 and VFA generation through the butyric acid pathway (Akca
et al., 2021). Kitchen-based food waste for the application of pyrolysis
was examined in an Indian context, displaying it to be a significant
technology for sustainable development (Agarwal et al., 2013). A two-
step process of polyhydroxyalkanoates production with the initial step
of biohydrogen production utilizing food waste as the renewable feed­
stock was examined, displaying the potential for value-added product
generation with simultaneous waste remediation (Amulya et al., 2015).
Sharma et al. (2021) discussed the potential of developing a circular
economy around the valorization of food waste, focusing on the existing
extraction technologies such as ultrasound and microwave-assisted, and
enzyme immobilization assisted. Tangerine, pomegranate, and banana
peels were identified to have several valorization products such as bio­
ethanol, biogas, and biohydrogen; however, the mismanagement or
inappropriate valorization was highlighted to pose a risk to public
health and the environment (El Barnossi et al., 2021).
3.3.2. Agricultural waste
Various agricultural processes produce substantial amounts of waste
that have the potential for valorization in this context. The dairy in­
dustry appears to be a primary supplier of this category of biomass and is
identified as a particularly detrimental effluent in reference to the
environment and climate change. Sar et al. (2022) reviewed the
fermentation-engineering aspects concerning the effective utilization of
dairy industries’ byproducts for producing various microbial products,
including biogas. An additional review discussed the potential for dairy
waste to not only be valorized to produce biogas, biohydrogen, bio­
ethanol, and various useful acids but also the production of bio-oil and
biochar by subjecting the resulting effluents to pyrolysis (Kumar
Awasthi et al., 2022). Bioconversion processes for generating high-value
products from cassava industry waste displayed promise in terms of
providing environmental stability to cassava production (Zhang et al.,
2016). The palm oil industry produces a particularly environmentally
severe effluent that can be valorized. Regulations of discharge amounts
spurred the development of various bioreactors and bioremediation
methods that allow for simultaneous wastewater treatment and
13
Bioresource Technology 366 (2022) 128168
bioenergy production (Chia et al., 2020).
3.3.3. Municipal and industrial wastes
Due to the rapid urbanization in many locations, substantial amounts
of domestic waste have become an increasing concern due to its ne­
cessity for proper treatment. In addition to this form, many industrial
processes result in similarly harmful wastes that require attention. The
treatment of both waste streams often results in byproducts that are
potential candidates for valorization and, in some cases, the raw
wastewater itself. Waste-activated sludge is biomass from the biological
treatment of wastewater that is generated in massive quantities,
approximately 0.1 to 30.8 kg per person per year. Alkaline-catalyzed
physiochemical pretreatment followed by acidogenic fermentation
allowed for biohydrogen and short-chain carboxylic acid production as a
function of pH (Naresh Kumar and Venkata Mohan, 2018). The same
biomass, except excess waste, was fermented for H2 generation in a
similar study that displayed the potential for enhancement through the
addition of anthraquinone-2-sulfate in the process (Zhang et al., 2022).
Blanco et al. (2017) examined another possible enhancement process in
which it was found that calcium dosing of synthetic wastewater
increased biomass retention in an anaerobic structured-bed reactor.
Municipal wastewater was also observed to be a working feedstock for
the pyrolytic generation of multiple bioenergy products (Agarwal et al.,
2013).
Municipal solid waste (MSW) was also utilized in dark fermentation
post-formic acid pretreatment to generate biohydrogen and a wide range
of metabolites such as acetic and butyric acids and ethanol (Cesaro et al.,
2020). Traditional wastewater treatment methods through activated
sludge do not efficiently eliminate nitrogen and phosphorous; however,
the resulting harmful waste can be valorized for microalgal biomass
using microalgae-bacteria consortia (Zhang et al., 2021). Residual fer­
mented solid waste from enzymatic biodiesel production was displayed
for the first time by Buback dos Santos et al. (2021) to have the potential
for H2 and methane obtainment through dark fermentation and anaer­
obic digestion. Rajesh Banu et al. (2020) and Lu and Ren (2016) both
reviewed the current standing of biohydrogen production using micro­
bial technologies and the expected challenges and prospects. Liquid
waste generated from the H2 production process has been shown to have
the potential for valorization as well, with products such as ethanol,
propanediol, butyric acid, and polyhydroxyalkanoates being desirable
(Sarma et al., 2015).
4. Current challenges and future perspectives
Table 2 displays the assessment strategies that were found in the
relevant studies. It is generally concluded that biohydrogen holds a very
high standing in terms of its desirability as a clean energy source.
However, there are investment and commercialization challenges
identified. For policymakers, the overall cost of H2 production
frequently outweighs the benefits of utilizing this fuel source as an
environmentally friendly alternative. Reviewing the potential technol­
ogies and strategies that project an increased cost-to-benefit ratio is
essential.
Many of the current industry’s bottlenecks concern the difficulty and
price associated with harvesting the necessary biomass feedstocks. An
improvement of the technologies that allow for the generation of these
biomass feedstocks, as well as selecting sources that otherwise require a
more environmentally detrimental treatment process, makes it more
likely for policy and general social interest to be directed towards a
biohydrogen-biorefinery approach. Integrated approaches to H2 gener­
ation, meaning the utilization of multiple processes for multiple prod­
ucts, have been stated to improve overall economic viability
(Chandrasekhar et al., 2020). Profitability analyses of waste-to-energy
processes and technologies give important insights into the market
trends that allow the adoption of technologies (Sharma et al., 2021). A
review of the permissible levels of waste production and carbon
A.T. Ubando et al.
emissions in certain industries and the effect of a CBE on the cost of
meeting regulation provides more interest for technology adopters
(Kumar Awasthi et al., 2022). Furthermore, increasing public knowl­
edge on the use of hydrogen is crucial for reaching carbon neutrality
because it can significantly influence how people perceive energy
transitions. Therefore, Tasnim Sahrin et al. (2022) also suggested that it
is essential to strongly involve the public through educational initiatives
in order to ensure that hydrogen is accepted by a larger social group and
that it successfully enters the market.
5. Conclusion
Biohydrogen in a circular bioeconomy framework presents a sus­
tainable way to generate the needed bioenergy while addressing climate
change and environmental damage. In this study, various techniques for
the harvesting and valorization of several biomass feedstocks were
reviewed. The recent development of technologies used in previous
studies for converting different biomass feedstocks into biohydrogen
was also presented. Several industries, particularly those that generate
copious amounts of waste, appear to exist that could potentially benefit
from implementing a circular bioeconomy, contingent on the contin­
uous development of the relevant technologies and the proper assess­
ment of its sustainability.
CRediT authorship contribution statement
Aristotle T. Ubando: Conceptualization, Formal analysis, Method­
ology, Validation, Investigation, Visualization, Writing – original draft.
Wei-Hsin Chen: Formal analysis, Validation, Investigation, Funding
acquisition, Project administration, Resources, Writing – review &
editing. Dennis A. Hurt: Formal analysis, Methodology, Investigation,
Writing – review & editing. Ariel Conversion: Formal analysis, Meth­
odology, Investigation, Writing – review & editing. Saravanan Rajen­
dran: Methodology, Investigation, Writing – review & editing. Sheng-
Lun Lin: Methodology, Investigation, Writing – review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
Acknowledgments
The authors thank the National Science and Technology Council,
Taiwan, R.O.C.’s financial support under contracts MOST 109-2221-E-
006-040-MY3, MOST 110-2622-E-006-001-CC1, and MOST 110-3116-
F-006-003- for this research. This research is also partly supported by
the Higher Education Sprout Project, Ministry of Education to the
Headquarters of University Advancement at National Cheng Kung Uni­
versity (NCKU).
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