Advanced Electrocatalysts for the Oxygen Evolution Reaction: From Single- to Multielement Materials
Abstract
:1. Introduction
2. Fundamentals of Advanced Electrocatalyst Design for Oxygen Evolution Reaction
2.1. Mechanism of Adsorbate Evolution and Its Scaling Relationship
2.2. Design of Efficient Electrocatalysts Based on Scaling Relations
2.3. Strategies for Breaking Scaling Relationships
2.3.1. OOH* Stabilization Independent on OH*
Introduction of a Second Adsorption-Relation Site
Formation of Hydrogen Bond (Or Introduction of Nanoscopic Confinement)
Introducing a Proton Acceptor (OO* + H*)
2.3.2. Direct O-O Coupling in the Absence of *OOH
Oxo Radical Coupling
Lattice-Oxygen-Mediated Mechanism
3. Oxygen Evolution Reaction Electrocatalysts
3.1. Single-Component and Binary-Component Electrocatalysts and Effect of Dopants
3.2. Ternary and Quaternary Component Electrocatalysts
3.3. Multicomponent Electrocatalysts
3.4. Increased Functionality of Single- to Multielement Materials
4. Effect of Supports
5. Summary and Outlook
- The need not to lose sight of the objective of having a unifying descriptor of catalytic activity. However, it is equally essential to carry out theoretical and experimental investigations to understand the factors involved in poor stability in strongly acidic and corrosive environments. It is critically necessary to establish structure–stability relationships, so proposing descriptors that relate catalyst structure, activity, and stability is the key to rational design and will represent a valuable advance in the fundamentals of the OER.
- Future research should try not only to break the scaling relationship but also to optimize the binding energies to achieve a lower overpotential. However, understanding and controlling the competition between different reaction mechanisms remains a major challenge.
- Promote the development of electrocatalysts based on earth-abundant materials, such as low-cost, environmentally friendly transition metals with significant activity, to replace the use of very expensive and scarce iridium in acidic OER electrocatalysts, which is a bottleneck at the high-scale PEM-WE level.
- In the meantime, electrocatalytic processes that are dynamic, surface-active sites, or active species can be generated during the electrochemical process, so it is necessary to pay special attention to the synthesis of the precatalytic material as well as to the operating conditions for its activation. Also, the self-reconstruction of the surface during the OER process can be beneficial or detrimental to the activity and/or stability of the electrocatalyst, usually by agglomeration, dissolution, and detachment of the catalyst. However, the structural reconstruction mechanisms are not entirely clear, so it is necessary to encourage the application of in situ and/or in operando techniques under electrochemical operating conditions, as these are a cornerstone in the development of highly active and stable electrocatalysts that allow a better understanding of the structural evolution of the materials in real time, as well as the nature of the key intermediates and their behavior. Therefore, these techniques allow in-depth understanding of the structure–activity–stability relationship of the OER process.
- The recent perspective based on the concept of high entropy to design advanced materials is opening a new space of many possible combinations, leading us to rethink and explore new phenomena, theories, and applications. Certainly, this poses a great challenge, both theoretically and experimentally. Compared to minor component alloys, HEAs are still at a nascent stage. However, HEAs are promising candidates for improving the performance of both AWEs and PEM-WEs. This class of materials is of particular interest for replacing noble metals such as Ir, Ru, and Pt in acidic media. The synergistic effect of HEAs is mainly based on their elemental diversity; this requires new research methods, e.g., statistical methods, machine learning, data-driven combinatorial synthesis, high throughput, and screening techniques, for the efficient exploration of a suitable composition of HEAs as a cost-effective material and, in the not-too-distant future, more attractive properties might be discovered. However, there are still many fundamental concepts to be clarified and many questions and challenges to be addressed in the field of synthesis, characterization, and analysis of electrochemical data, identification of active sites, origin of high activity, etc.
- To improve data quality, standardized measurements of HER and OER properties are necessary as demonstrated by Hung et al. [160]. They recognized that 3D electrodes, such as metal foam materials (Ni, Fe, Co, IrNi-FeNi3 on Ni, and other foams) are an interesting alternative, which exhibit high catalytic activities; however, the impact of parameters such as active area, thickness, porosity, capillarity, and purity need to be better understood. Some of them are not easy to determine experimentally. This contribution presents alternatives for ECSA calculation and highlights that an objective evaluation improves the reliability of the results enriches our fundamental understanding of electrocatalytic activity. Therefore, the implementation of standardized electrochemical parameters to evaluate the performance of electrocatalysts is an area of opportunity to ensure their industrial application.
# | Catalysts | Element(s) | Support Material | Strategy Design | Synthesis Method | Overpotential @ 10 mA cm−2 | Tafel Slope | Stability | Acidic Media | Ref. |
---|---|---|---|---|---|---|---|---|---|---|
mV vs. RHE | mV dec−1 | |||||||||
Single element | ||||||||||
1 | Fe2O3 | Fe | Ti foil | Polymorphism structures | Spray pyrolysis | 650 | 56 | 24 h @ 10 mA cm−2 | 0.5 M H2SO4 | [2] |
2 | Co3O4 crystalline | Co | Fluorine-doped tin oxide (FTO) | Engineering interface | Thermal annealing | 570 | 80 | 12 h @ 10 mA cm−2 | 0.5 M H2SO4 | [161] |
3 | γ-MnO2 | Mn | FTO | Thermal decomposition | 489 | 79 | 8000 h @ 10 mA cm−2 | 1.0 M H2SO4 | [112] | |
4 | Co3O4 nanosheets | Co | Carbon paper | Electroplating and calcination | 370 | 82 | 86.8 h @ 100 mA cm−2 | 0.5 M H2SO4 | [162] | |
5 | IrOx@IrO2 | Ir | w/o S | Structural engineering | Adams fusion | 309 | 45 | 6 h @ 10 mA cm−2 | 0.1 M HClO4 | [163] |
6 | Mesoporous iridium nanosheets | Ir | Vulcan XC-72 carbon | Mesoporous chemistry | Wet chemical/ micelles | 240 | 49 | 8 h @ 10 mA cm−2 | 0.5 M H2SO4 | [164] |
7 | Mn3O4 nanoplates | Mn | --- | Crystal and geometric structure transformation | Rapid thermal annealing | 210 | 54.24 | 20 h @ 10 mA cm−2 | 0.5 M H2SO4 | [113] |
Binary elements | ||||||||||
8 | Fe5Si3 | Fe, Si | w/o S | Multiphase structure | Sintering process | 735 | 381.8 | 1000 cycles | 0.5 M H2SO4 | [165] |
9 | Ag-Co3O4 mesoporous | Co, Ag | FTO | Doping with foreign element (Ag) | Electrodeposition, hydrothermal, and calcination | 680 | 219 | 10 h @ 1.6 V Ag/AgCl | 0.5 M H2SO4 | [166] |
10 | C3N4-CNT-CF | C, N | Carbon fiber | Metal-free based | Annealing treatment | 570 | 129 | 14 h @ 1.63 V RHE | 0.5 M H2SO4 | [167] |
11 | TiO2-modified MnO2 | Mn, Ti | Polycrystalline gold disks | Engineering surface | Sputtering deposition | 510 @ 1 mA cm−2 | 170 | 265 h @ 1.8 V RHE | 0.05 M H2SO4 | [168] |
12 | Ag-Co3O4 (400) | Co, Ag | w/o S | Doping with foreign element (Ag) | Hydrothermal and annealed (400 °C) | 470 | 92 | 1000 cycles | 0.5 M H2SO4 | [169] |
13 | Co3O4/CeO2 | Co, Ce | FTO | Engineering interface | Electrodeposition | 423 | 88.1 | - | 0.05 M H2SO4 | [170] |
14 | 2D MoS2 nanosheets | Mo, S | w/o S | Polymorphism/ heteroatoms | Exfoliation and deposition | 420 | 322 | 2 h @ 10 mA cm−2 | 0.5 M H2SO4 | [171] |
15 | W0.57Ir0.43O3-δ | Ir, W | FTO | Structural engineering | Plasma synthesis | 370 | 125 | 0.56 h | 1.0 M H2SO4 | [172] |
16 | Cu0.3Ir0.7Oδ | Ir, Cu | Ti plate | Doping with foreign element (Cu) | Hydrothermal and annealing | 351 | 63 | 1.67 h @ 1.68 V RHE | 0.1 M HClO4 | [173] |
17 | IrTe NTs | Ir, Te | Vulcan XC-72 carbon | Surface engineering | Galvanic replacement | 290 | 60.3 | 2000 cycles | 0.1 M HClO4 | [174] |
18 | IrCu0.77 | Ir, Cu | Vulcan XC-72 carbon | Polyol method | 282 | 78.6 | --- | 0.1 M HClO4 | [175] | |
19 | RuNiOx | Ru, Ni | Carbon fiber paper | Dealloying treatment | Dip coating | 280 @ 50 mA cm−2 | 51.91 | 10 h @ 1.5 V RHE | 0.5 M H2SO4 | [176] |
20 | IrMoOx nanofibers | Ir, Mo | --- | Electronic modulation | Electrospinning and calcination | 267 | 46.09 | 30 h | 0.5 M H2SO4 | [177] |
21 | Fe2O3/TiO2 NWs/Ti | Fe, Ti | Ti foam | Structural engineering | Facile ion exchange process and calcination | 230 @ 1 mA cm−2 | 110.7 | 20 h @ 1.9 V SCE | 0.5 M H2SO4 | [178] |
22 | Mn0.73Ru0.27O2-δ | Ru, Mn | w/o S | Oxygen vacancies | Pyrolysis | 208 | 65.3 | 10 h @ 10 mA cm−2 | 0.5 M H2SO4 | [179] |
23 | Zn-doped RuO2 hollow nanorod | Ru, Zn | w/o S | Doping with foreign element (Zn) | Annealing process under air | 206 | 45.65 | 30 h @ 10 mA cm−2 | 0.5 M H2SO4 | [180] |
24 | Mn-doped RuO2 nanocrystals | Ru, Mn | w/o S | Doping with foreign element (Mn) | Annealing process under air | 158 | 42.94 | 10 h @ 10 mA cm−2 | 0.5 M H2SO4 | [181] |
25 | Ru/MnO2 | Ru, Mn | w/o S | Surface engineering/self-reconstruction | One-step cation exchange method | 161 | 29.4 | 10 h @ 10 mA cm−2 | 0.1 M HClO4 | [50] |
Ternary elements | ||||||||||
26 | Ni0.5Mn0.5Sb1.7Oγ | Ni, Mn, Sb | Antimony-doped tin oxide | Phase restructuring | Sputter deposition | 672 | 85 | 168 h @ 10 mA cm−2 | 1.0 M H2SO4 | [182] |
27 | Ni40Fe40P20 | Ni, Fe, P | w/o S | Heteroatoms | Melting spinning | 540 | 40 | 30 h @ 10 mA cm−2 | 0.05 M H2SO4 | [183] |
28 | Mo-Co9S8 | Mo, Co, S | Carbon cloth | Heteroatoms | solvothermal method | 370 | 90.3 | 24 h @ 1.6 V RHE | 0.5 M H2SO4 | [184] |
29 | F-doped Cu1.5Mn1.5O4 nanoparticles | Cu, Mn, F | Porous Ti foil | Doping with foreign element (F) | Chemical synthesis and heat treatment | 320 @ 9.15 mA cm−2 | 60 | 24 h @ 1.55 V RHE | 0.5 M H2SO4 | [185] |
30 | CP@NCNT | Co, P, N | N-doped CNT | Heteroatoms | Spray drying | 317 | 75 | 24 h @ 15 mA cm−2 | 0.5 M H2SO4 | [186] |
31 | IrNiCu DNF/C | Ir, Ni, Cu | Vulcan XC-72 carbon | Nanoframe structure | Chemical etching | 303 | 48 | 2500 cycles | 0.1 M HClO4 | [187] |
32 | FeN4/NF/EG | Fe, N, C | Exfoliated graphene | Dual element-doping (N, C) | Electrodeposition and carbonization | 294 | 129 | 24 h @ 20 mA cm−2 | 0.5 M H2SO4 | [188] |
33 | Co-doped IrCu | Ir, Co, Cu | Vulcan XC-72 carbon | Doping with foreign element (Co) | Chemical etching | 293 | 50 | 2000 cycles | 0.1 M HClO4 | [189] |
34 | W-Ir-B | Ir, W, B | w/o S | Biphasic structure | Arc melting and drop casting | 291 | 78 | 120 h @ 100 mA cm−2 | 0.5 M H2SO4 | [190] |
35 | RuO2/(CoMn)3O4 | Ru, Co, Mn | Carbon cloth | Interface engineering | Hydrothermal process | 270 | 77 | 24 h @ 10 mA cm−2 | 0.5 M H2SO4 | [116] |
36 | HNC-Co | Co, N, C | Carbon paper | Dual element-doping (N, C) | Polymerization, reduction, and pyrolysis | 265 | 85 | 100 h | 0.5 M H2SO4 | [191] |
37 | SrTi0.67Ir0.33O3 | Ir, Sr, Ti | w/o S | Ir doping | Polymerized complex method | 247 | 43 | 20 h @ 10 mA cm−2 | 0.1 HClO4 | [192] |
38 | C-RuO2-RuSe-5 | Ru, Se, C | w/o S | Inducing interstitial atoms | Hydrothermal method | 212 | 49.5 | 30 h @ 10 mA cm−2 | 0.5 M H2SO4 | [193] |
39 | Ru NCs/Co2P Hollow microspheres | Ru, Co, P | w/o S | Heteroatoms | Hydrothermal | 197 | 89 | 10 h | 0.5 M H2SO4 | [194] |
Quaternary elements | ||||||||||
40 | InFeCo-CCP | Fe, Co, In, N | w/o S | Organic/ inorganic polymeric | Coordination-substitution polymerization | 710 | 99 | 48 h @ 1.75 V RHE | 0.5 M H2SO4 | [195] |
41 | P-NSC/Ni4Fe5S8 | Ni, Fe, N, S | w/o S | Heteroatoms/ porous | Pyrolysis (1000 °C) | 550 | 72.1 | 10,000 cycles | 0.5 M H2SO4 | [196] |
42 | Fe35Ni35Co10P20 | Fe, Ni, Co, P | w/o S | Amorphous multialloy | Arc-melting technique | 497 | 79 | 20 h @ 1.73 V RHE | 0.5 M H2SO4 | [197] |
43 | Ni42Li2O5 | Steel (Ni, Fe, Mn), Li | AISI Ni42 steel | Surface engineering | Electrooxidation | 445 | 260 | 5.6 h @ 10 mA cm−2 | 0.05 M H2SO4 | [198] |
44 | Mn-doped FeP/Co3(PO4)2 | Fe, Co, Mn, P | Carbon cloth | Heteroatoms | Hydrothermal | 390 | 472 | 10,000 cycles | 0.5 M H2SO4 | [199] |
45 | Ba[Co-POM]/CP | Co, W, Ba, P | Carbon paste | Polyoxometalate | Metathesis | 361 | 97 | 24 h @ 1.48 V RHE | 1.0 M H2SO4 | [200] |
46 | CoMoNiS-NF-31 | Co, Mo, Ni, S | Nickel foam | Heteroatoms/ hierarchical structure | One-pot hydrothermal | 228 | 78 | --- | 0.5 M H2SO4 | [121] |
Multi-elements | ||||||||||
47 | FeCoNiMnW | Fe, Co, Ni, Mn, W | Carbon paper | Multimetal alloy | Electrodeposition | 332 | 145 | 1 h | 0.5 H2SO4 | [201] |
48 | Al89Ag1Au1Co1 Cu1Fe1Ir1Ni1Pd1 Pt1Rh1Ru1 | Ir, Ru, Pt, Pd, Au, Rh, Ag, Al, Co, Cu, Fe, Ni, | w/o S | Multimetal alloy | Arc melting and one-step dealloying | 258 | 84.2 | 11.11 h @ 10 mA cm−2 | 0.5 H2SO4 | [202] |
49 | FeCoNiIrRu | Ir, Ru, Fe, Co, Ni | Carbon nanofibers | Multimetal alloy | Electrospinning | 241 | 153 | 4 h | 0.5 H2SO4 | [203] |
50 | Al96Ni1Co1Ir1Mo1 | Ir, Al, Ni, Co, Mo | Carbon powder | Multimetal alloy | Induction-melting furnace and chemical etching | 233 | 55.2 | 7000 cycles | 0.5 H2SO4 | [126] |
51 | IrPdRhMoW | Ir, Pd, Rh, Mo, W | w/o S | Multimetal alloy/structural engineering | Oil-phase method | 188 | --- | 100 h @ 100 mA cm−2 | 0.5 H2SO4 | [127] |
Author Contributions
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
Abbreviations
AEM | Alkaline electrolyte membrane |
AMO | Amorphous manganese oxides |
AWE | Alkaline water electrolyzers |
BEDPs | Binding energy distribution patterns |
CPET | Concerted proton–electron transfer |
CUS | Coordinatively unsaturated |
DEMS | Differential electrochemical mass spectrometry |
DFT | Density functional theory |
ESSI | Electrochemical step symmetry index |
HCP | Hexagonal close-packed structure |
HEAs | High-entropy alloys |
HER | Hydrogen evolution reaction |
IMCs | Intermetallic compounds |
LDH | Double-layered hydroxides |
LOM | Lattice oxygen mechanism |
MOFs | Metalorganic frameworks |
MD | Molecular dynamics |
MWCNTs | Multiwalled carbon nanotubes |
NAP | Near ambient pressure |
NPs | Nanoparticles |
OER | Oxygen evolution reaction |
ONB | Oxygen nonbonding states |
PEM | Proton exchange membrane |
PEM-WE | Proton exchange membrane water electrolyzer |
RDS | Rate-determining step |
RHE | Reversible hydrogen electrode |
RPS | Rate-determining potential step |
SHE | Standard hydrogen electrode |
SI-SECM | Surface interrogation scanning electrochemical microscopy |
STEM-EDS | Scanning transmission electron microscopy–energy dispersive X-ray spectroscopy |
UV-vis | Ultraviolet–visible |
XAS | X-ray absorption spectroscopy |
XPS | X-ray photoelectron spectroscopy |
XRD | X-ray diffraction |
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Electrolyte | Half-Cell Reaction | |
---|---|---|
Hydrogen evolution reaction (HER) | ||
Acid | (1) | |
Alkaline | (2) | |
Oxygen evolution reaction (OER) | ||
Acid | (3) | |
Alkaline | (4) |
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Higareda, A.; Hernández-Arellano, D.L.; Ordoñez, L.C.; Barbosa, R.; Alonso-Vante, N. Advanced Electrocatalysts for the Oxygen Evolution Reaction: From Single- to Multielement Materials. Catalysts 2023, 13, 1346. https://doi.org/10.3390/catal13101346
Higareda A, Hernández-Arellano DL, Ordoñez LC, Barbosa R, Alonso-Vante N. Advanced Electrocatalysts for the Oxygen Evolution Reaction: From Single- to Multielement Materials. Catalysts. 2023; 13(10):1346. https://doi.org/10.3390/catal13101346
Chicago/Turabian StyleHigareda, América, Diana Laura Hernández-Arellano, Luis Carlos Ordoñez, Romeli Barbosa, and Nicolas Alonso-Vante. 2023. "Advanced Electrocatalysts for the Oxygen Evolution Reaction: From Single- to Multielement Materials" Catalysts 13, no. 10: 1346. https://doi.org/10.3390/catal13101346