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Electrocatalysis Goes Nuts

Andrew R. Akbashev*
Cite This: ACS Catal. 2022, 12, 4296−4301 Read Online

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ABSTRACT: While searching for new nanoelectrocatalysts with outstanding performance, researchers often disregard the
complexity and true usability of such materials. Here, it is argued that the chemical and structural complexity of electrocatalytic
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materials and electrodes reported in numerous studies significantly exceeds the quality of their characterization, making meaningful
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interpretation of the data impossible and providing little (or no) scientific insight as a result. It is suggested that the experiments
should be designed with the aim of obtaining an interpretable electrochemical response by minimizing the complexity of electrode
materials. A greater recognition of the worrisome state of the field will help improve the quality of research in electrocatalysis.

■ INTRODUCTION
An industry-scale implementation of (photo)electrocatalysis is
inherently highly active electrocatalysts. Despite the recent
discovery that graphene electrodes can achieve outstanding
activity when decorated with bird droppings,20 numerous efforts
one of the most promising ways to enable a sustainable feedstock
are still devoted to the massive screening of various
of valuable chemicals and reduce our dependence on fossil fuels.
combinations of materials, with ultrahigh activity being
It is often perceived that the biggest obstacles for the successful
discovered in each case. Inspired by an endless number of
realization of electrocatalytic technologies are the insufficient
remarkable electrocatalysts reported to date,21−25 the author
activity and poor selectivity and stability of the electrocatalysts.
analyzes if the current metrics-oriented research can indeed be a
These challenges fuel the ongoing research in electrocatalysis,
possible way for electrocatalysis to reach new heights.

including engineering of materials and electrodes and design of
electrolytes and electrolytic cells. A significant fraction of current
efforts is devoted to the search for new electrocatalytic materials
and their synthesis and incorporation into complex electrodes.
Taking the electrocatalytic reactions involving oxygen/hydro-
gen as an example, one can find innumerable reports that
celebrate the outstanding activity and stability of various unusual
electrodes and nanomaterials. As such are (in the original
terminology) graphitic C3N4 nanosheets,1 nano-octahedrons
made of N-doped carbon-encapsulated MoN,2 heteronanosh-
eets of Mo/M2C,3 Mo2C-embedded N-doped porous carbon
nanosheets,4 single Mo atoms “anchored” on N-doped carbon,5
Co9S8@MoS2 core−shell heterostructures,6 Co3Mo nano-
particles “nested” in MoOx nanosheet arrays,7 holey 2D
nonlayered heterostructure nanosheets of transition metal
carbides/nitrides,8 Janus hollow graphene with single-atomic
Ni/Fe−N4 sites,9 Pd nanosponges wrapped by graphene
“dots”,10 hollow heterostructure nanorods of Mo-doped
Ni3S2/NixPy,11 2D superholey leaf-like metal carbonitrides,12
open nanoboxes of CoMoOx/CoMoSx/CoSx,13 graphene-
oxide-wrapped mix-valent cobalt phosphate hollow nano-
tubes,14 Ag nanowires shelled with NiMn-layered double
hydroxides (LDH),15 cactus-like hollow spheres of NiCo2S4@
NiFe LDH,16 and numerous other combinations of various
extraordinary systems, with their quantity increasing alarmingly.
All these electrocatalysts show exceptional activity and are often
based on “nanoarchitectonics”,17−19 can exhibit bicatalytic and
even tricatalytic6 performance and are reported to easily
outperform those based on precious metals.
Combing through this massive spree of discoveries, one may
wonder if most materials, especially nanomaterials, are
■
EXPERIMENTAL RESULTS
In the experiment, a cobalt-“impregnated” hazelnut is used as an
electrode material and is tested for the oxygen evolution reaction
(OER). Electrocatalytic OER is regarded as a bottleneck of
water electrolysis and therefore receives significant interest. The
electrocatalytic material was prepared by grinding together
equivalent weights of the hazelnut core and Co(NO3)2·6H2O
and heating the mixture in Ar at 700 °C. The resulting powder
was then mixed with conductive carbon and Nafion and then
was dropcast onto a Pt disk of the rotating disk electrode (RDE).
A curious reader can find further details about this rather
meaningless synthesis in the Supporting Information.
As shown in Figure 1, cyclic voltammetry in 0.1 M KOH
reveals a rapid increase of the current in the anodic direction that
starts at potentials close to 1.6 V vs RHE (reversible hydrogen
electrode). The observed OER activity of the hazelnut-based
material is evidently higher than that of a clean Pt disk in the high
current region. To further interrogate the electrode, chronopo-
tentiometry at 12.8 mA/cm2geo is performed. Even though the
overpotential at the beginning is lower than that of Pt, it shows
an obvious increase with time, signifying the loss of activity
(inset in Figure 1). Thus, these observations indicate that the
Received: January 7, 2022
Published: March 25, 2022

© 2022 American Chemical Society https://doi.org/10.1021/acscatal.2c00123

4296 ACS Catal. 2022, 12, 4296−4301
ACS Catalysis pubs.acs.org/acscatalysis
Figure 1. Cyclic voltammetry and chronopotentiometry (inset) of the
cobalt-“impregnated” hazelnut-derived electrode measured with a
rotating disk electrode (RDE). Bare Pt RDE disk is shown for
comparison.
electrode that went nuts is not suitable for real applications.
Although this conclusion could be drawn without spending time
on pointless experiments, this way the author hopes to draw a
wider attention to the alarming state of the field.
■ DISCUSSION
Looking through the research published in the area of
electrocatalysis in the last 5 years, two major points of concern
can be outlined:
First, the practical value of the data reported in a wide range of
studies is rather low. According to the International Union of
Pure and Applied Chemistry (IUPAC), electrocatalysis is
defined as simply “an electrochemical reaction that takes
advantage of a catalyst”. In the literature, however, the term
“electrocatalysis” is often used whenever the electrochemical
conversion reaction involves species that represent valuable
chemicals (such as H2, O2, HCOOH), with “low” and “high”
activities being defined rather arbitrary and often related to an
entire electrode (which may be rather heterogeneous and ill-
defined chemically and structurally). This allows for a significant
flexibility in how the results are reported and interpreted. For
example, the fact that almost all of the reported OER
electrocatalysts easily “beat” IrO2 (which is a great but expensive
OER electrocatalyst) suggests that IrO2 is apparently not active
enough to stand a direct comparison with most electrocatalysts
reported to date, which is nonsense.
Looking at the evolution of metrics-oriented publishing, one
can go as far as to say that electrocatalytic “activity” is similar to
the “efficiency” in the field of photovoltaics, where strict
reporting standards were developed after similar flexibility in
how the performance was reported had revealed major issues
with the reproducibility of experimental results.26−32 Although
electrocatalysis and photovoltaics are rather different fields, they
seem to experience similar “symptoms”32 such as a low quality of
experiments, low reliability of the reported data, and poor
understanding/characterization of the studied materials and
electrodes (all of which are crucial for an accurate evaluation and
modeling of device performance). To improve the quality of
reported data and overall value of research in the fields of
electrochemistry and electrocatalysis, recommended practices
and critical remarks were published.33−41 While these
publications have certainly made a positive impact, unfortu-
nately only a minority of scientists seem to be following these
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guidelines. For this reason, we believe that raising the value and
impact of research in electrocatalysis is impossible without a
firmer stance adopted by the research community and editorial
boards of scientific journals.
An illustrative example of how stricter (but far f rom perfect)
guidelines help improve the quality of research can be found in
the field of batteries. Looking at the two fieldselectrocatalysis
and batteriesone may notice that the battery community has a
principal focus on the applied research and engineering, with
clear goals and a significant industrial support. This has been
achieved particularly by establishing standards for relevant
experiments and metrics-oriented research that aligned well with
the requirements of the battery industry. For example, the use of
coin, pouch, cylindrical, and prismatic cells with specific sizes
enables cell-standardized research that facilitates the improve-
ments of individual components of the cell and benchmarking
the materials and ideas.42,43 For Li-metal batteries, cell
parameters such as Li-metal anode thickness, cathode
composition (material, binder, conductive carbon), electrolyte
amounts, separator thickness, along with consistent testing
protocols, are all critical for a proper evaluation of the cell-level
performance.43,44 This performance itself is represented by a
wide range of measurable cell characteristics (voltage range,
gravimetric/volumetric energy and power density, cycling
stability, discharge capacity, self-discharge, etc.) that, when
combined with the aforementioned cell parameters, can be used
to assess and compare the outcome of metrics-oriented research.
Nonetheless, it should be noted that the field of batteries
certainly has its own problems and “misalignments” with the
industry (with many types of batteries struggling to find wide
application).43,45 However, in the past decade, this field has
advanced substantially and can serve as a good example of how a
research field can mature under the pressure of market demand.
Importantly, in the case of batteries, one can observe a synergy
effect: by making the research relevant for the industry,
academia improves the quality and impact of its own efforts,
and, in turn, the industry fuels the academic research, both
financially and direction-wise.
With regard to electrocatalysis, it is quite likely that the vast
majority of thousands of reports demonstrating (ultra)high
electrocatalytic performance will never find any real use. The
cost of production of such electrodes is too high to justify their
application while the stability is too low, which is the harsh
reality that often seems to be carefully ignored in the metrics-
oriented electrocatalysis research. Unfortunately, despite a
certain development of the industrial sector,46 there is a large
gap between the academic research and commercial electrolysis.
For example, when considering hydrogen production, alkaline
electrolysis is the most developed technology with the least
investment costs.46 Recent analysis47 shows that renewable
hydrogen becomes economically viable if its cost reaches US
$3.53−3.65 kg−1 (for Germany and Texas, U.S.A.), implying
that hydrogen production via electrolysis can already be cost-
competitive for small- and medium-scale suppliers and will
become attractive for industrial-scale supply within a decade.47
Although such a promising forecast implies that large-scale
commercial electrolysis may soon start penetrating the hydrogen
market, the real electrodes used today in commercial alkaline
electrolyzers do not contain “nanoarchitectured”17−19 materials
but rather are based on cheap materials such as Ni, Ni-based
alloys and steel.48−50 This choice is dictated by the strict market
requirements for electrodes, including being cheap, extremely
stable, and not dependent on critical raw materials.
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One may think that the field of electrocatalysis is in fact going
through important milestones on the way to a sustainable future,
where fuels and chemical feedstocks will be produced from
renewable electricity. Although at first it may sound reasonable,
the author argues that it is hardly true. To be relevant for
industry, research in applied electrocatalysis should go beyond
simple reporting of basic metrics for all imaginable (and
unimaginable) electrodes. The techno-economic analyses
demonstrate the cost complexity of the industrial and scalable
electrocatalytic systems, revealing numerous factors other than
electrode materials that define the costs and ensure the potential
implementation of the electrocatalytic technology.47,51−54 One
can see that, if the reported datasets were collected under
industry-relevant conditions in the cell that is also industry-
standardized, such reports would hold more value from the
metrics point of view. For example, alkaline electrolysis in
industry is operated galvanostatically at 0.1−1 A/cm2 (in 30%
KOH at elevated temperatures) and requires the electrode
stability that considerably exceeds typically reported timescales
(i.e., tens of thousands of hours instead of just a few).46,55
Thus, performance by itself has little meaning unless it is
relevant to technologies or can be benchmarked. With this, the
author strongly encourages that the community and editorial
boards of relevant journals adopt new and clear policies
regarding the reported metrics and their comparison and
reproducibility. Ideally, this should include: (1) standardized
industry-relevant cells56 for different electrochemical processes,
(2) standardized testing protocols, and (3) a mandatory
checklist of the necessary technical information (similar to one
adopted by Nature journals for photovoltaics26). External
evaluation/reproduction of the electrocatalyst’s performance
can provide further credibility to such studies. For example, the
ElectroCat Consortium57 provides electrocatalytic testing
capabilities. (However, the fact that such facilities and services
are hardly available to researchers presents another challenge for
the community.) Such a paradigm shift in the way that
performance is assessed in electrocatalysis can help move the
applied research in the desired direction.
And what about the fundamental relevance of the research
that involves such “nanoarchitectured” electrodes?
This brings us to the second major concern, which is the
scientific meaningfulness of the reported data and experiments.
Electrocatalytic activity and electrochemical response have little
scientific meaning when they are measured on a complex
electrode that consists of multiple components: nanoscale
materials (“nanoboxes”, “nanosponges”, nanosheets, etc.),
conductive additives, binders, and the substrate. Such systems
have an enormous diversity of active sites, and they can exhibit a
spatially nonuniform electrical conductivity, electrode loss, and
poorly defined mass transport during operation. Decoupling
these factors and performing a proper characterization of the
chemical composition and structure of a surface in such cases is
nearly impossible. As a result, the correlation between the
chemistry/structure of specific active sites and their electro-
chemical response cannot be unambiguously established for
such electrodes. In other words, the experimentally measured
datasets represent an averaged picture and cannot be directly
compared to the behavior of specific active sites predicted
through quantum-chemical calculations and molecular model-
ing.
Here another important difference between the fields of
batteries and electrocatalysis that determines the value of
research should be noted: characterizing the bulk properties of a
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material is far easier than probing the chemistry and structure of
a surface. Because the functionality of battery materials
(cathodes and anodes) is largely defined by their bulk properties,
in-depth studies of their behavior during operation are
reasonably accessible in experiments. However, the functionality
of electrocatalysts is governed by the surface properties, which
makes it difficult to conduct high-quality research in this field. As
a result, one can notice that explaining the electrocatalytic
properties of a surface using the results of bulk characterization
has become a rather common practice.
In an ideal scenario, to ensure the electrochemical experiment
provides interpretable and scientifically meaningful data, such
measurements should be done on well-defined surfaces such as
single crystals. When a surface has a known chemical
composition and structure (location of atoms), it shows a
well-defined and spatially uniform electrochemical response. It is
the reason why so many electrochemical studies in the previous
century were done on single-crystalline surfaces, with the latter
undergoing a rather sophisticated surface cleaning and
preparation process to enable a uniform and well-known
chemical composition and structure. Although, strictly speaking,
it is almost impossible to know the exact atomic structure and
composition of the surface under reaction conditions, even for
single crystals the results of such studies can still be related to
quantum-chemical and molecular modeling of adsorption and
bond-breaking reactions in a far more convincing way than for
“nanoarchitectured” electrodes.
Certainly, the author does not propose to solely use single-
crystalline surfaces. Not all types of materials can be made in a
single-crystalline and well-defined form, while meaningful data
can be collected on many systems if the experiments are properly
designed. The author proposes that the experiments should be
designed in such a way as to minimize the chemical and material
complexity of the electrodes, with the aim of obtaining an
interpretable electrochemical response. For example, one can
significantly reduce the material complexity by (1) conducting
experiments on single-crystalline and well-faceted particles58,59
(which certainly cannot replace the studies of single crystals
because the surface chemistry of such particles can be quite
different from that of single crystals), (2) using nanoparticles
that have a relatively simple chemical composition and/or
narrow size distribution,60 (3) conducting single-particle
experiments (especially those concerning material evolution
and degradation),59,61 (4) avoiding62,63 structurally undefined
conductive support such as carbon black that can affect64 the
response of the electrode, (5) using flat electrode geo-
metries59,63 that experience little mass transport limitations
and are accessible for probing,59,65,66 and by many other ways.
Unfortunately, in the majority of reports, the complexity of the
materials significantly exceeds the quality of their character-
ization, making it almost impossible to understand the science
behind such experiments. In some cases, the lack of scientific
rigor is further exacerbated by the authors’ reliance on the
density functional theory (DFT) calculations of adsorption on
well-defined “model” (and hardly relevant) surfaces that are
supposed to “explain” the high electrocatalytic activity of a
complex system measured experimentally. To avoid this
inconsistency, one should perform a rigorous characterization
of the surface to ensure it does not undergo reconstruction and
indeed has the state that is assumed in calculations.
Here it should also be mentioned that the DFT calculations
themselves have uncertainties that are associated with the choice
of functionals.67−69 Determining the accuracy of such
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ACS Catalysis pubs.acs.org/acscatalysis
calculations is tricky and, ideally, requires experimental
verification. Properly designed experiments can enlighten
theoreticians about the accuracy70 of their approaches, even
though such “validating” experiments should be perfectly
defined (well-defined surface, sophisticated characterization,
and electrochemistry) and, therefore, may involve significant
efforts. The author hopes that, by bringing this vitally important
research direction to the community’s attention, the develop-
ment of accurate DFT approaches for electrochemical systems
can be facilitated.
Finally, it should be noted that the electrochemical analysis
performed in most studies is insufficient for understanding the
response of the studied systems. In most cases, it includes simple
cyclic voltammetry of a rather complex composite electrode that
is complemented by chronopotentiometry for a stability test,
with little analysis of the data (probably due to the electrode’s
complexity). At the same time, there is a wide range of
electrochemical and electroanalytical techniques that can
significantly benefit electrocatalysis research. As such are the
pulse voltammetry techniques;71,72 potentiodynamic electro-
chemical impedance spectroscopy;73 the measurements of CO,
hydrogen, and oxygen adsorption/desorption peaks as well as
underpotential deposition (UPD) of metals for the estimation of
the active surface area;74,75 and various other methods.76 The
fundamental processes that take place during electrocatalysis are
very complex and difficult to disentangle. The improvement of
the research quality is paramount for both understanding the
fundamental mechanisms and advancing applied electro-
catalysis.
■
CONCLUSIONS
Although pursuing crazy ideas is often perceived as a possible
way toward discoveries, the author strongly discourages from
taking the term “crazy” literally. The history of science shows
that any field can experience difficulties with research quality
when the standards for metrics-oriented publications are poorly
defined and the reward for such publications is high. Keeping the
focus on the scientific rigor and meaningfulness while designing
research projects is crucial when one aims to move the field
forward.
■
ASSOCIATED CONTENT
*
sı Supporting Information
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acscatal.2c00123.
Description of the experimental part (PDF)
■ AUTHOR INFORMATION
Corresponding Author
Andrew R. Akbashev − Division for Research with Neutrons
and Muons (NUM), Paul Scherrer Institute, 5232 Villigen,
Switzerland; orcid.org/0000-0003-1573-1773;
Email: andrei.akbasheu@psi.ch
Complete contact information is available at:
https://pubs.acs.org/10.1021/acscatal.2c00123
Notes
The author declares no competing financial interest.
■
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