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Recent advances in electrocatalysts for efficient hydrogen evolution reaction

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Abstract

As a clean energy source, hydrogen plays a critical role in the global mission to achieve carbon neutrality. Among varied hydrogen production techniques, water electrolysis driven by clean energy, such as solar or wind energy, is the most promising and viable option, with the advantages of celerity, high efficiency, cleanliness, and sustainability. However, this process necessitates a highly active and durable hydrogen evolution reaction (HER) catalyst to enhance the overall reaction efficiency. This article thoroughly reviews the recent development of electrocatalysts exhibiting high-performance HER. In particular, a comprehensive look at noble metals platinum (Pt), ruthenium (Ru), iridium (Ir), and non-noble metals, including sulfides, carbides, nitrides and phosphides is taken. Synthesis strategies, methods for enhancing performance, and the correlation between structure, composition, and catalytic performance are discussed. We also pay particular attention to density functional theory (DFT) calculations to reveal the mechanisms behind the improvement of HER performance. Finally, the critical challenges associated with electrochemical water splitting and propose coping strategies are presented.

Graphical abstract

摘要

作为一种清洁能源, 氢气在实现碳中和的全球使命中发挥着关键作用。在各种制氢技术中, 由太阳能或风能等清洁能源驱动的水电解是最有前途和可行的选择, 具有快速、高效、清洁和可持续的优点。然而, 这一过程需要一种高活性和持久的氢气进化反应 (HER) 催化剂来提高整体反应效率。这篇文章全面回顾了近年来表现出高性能HER的电催化剂的发展。我们全面回顾了贵金属–铂 (Pt) 、钌 (Ru) 、铱 (Ir), 以及非贵金属, 包括硫化物、碳化物、氮化物和磷化物。我们讨论了合成策略、提高性能的方法, 以及结构、成分和催化性能之间的相关性。我们还特别关注密度泛函理论 (DFT) 的计算, 以揭示改善HER性能背后的机制。最后, 我们介绍了与电化学水分离有关的关键挑战, 并提出了应对策略。

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Fig. 1

Reproduced with permission from Ref. [47]. Copyright 2022, American Chemical Society. d Schematic illustration of synthesis of PtSA-NiO/Ni; e calculated OH-binding energies and H binding energies for Ni, pure NiO, and O vacancies-modified NiO surface; f calculated energy barriers of water dissociation kinetic and g adsorption free energies of H* on surface of PtSA-NiO/Ni PtSA-NiO and PtSA-Ni catalysts, respectively. Reproduced with permission from Ref. [53]. Copyright 2021, The Author(s). h Schematic illustration of synthesis of Pt/MoS2-NTA/Ti3C2. Reproduced with permission from Ref. [59]. Copyright 2022, Wiley–VCH GmbH

Fig. 2

Reproduced with permission from Ref. [69]. Copyright 2021, Wiley–VCH GmbH. d Schematic illustration of synthesis of cMOF/LDH hetero-nanotree catalysts. Reproduced with permission from Ref. [71]. Copyright 2022, Wiley–VCH GmbH. e Corresponding free-energy diagram of ΔGH*; f charge density redistributions of Co@CNTs|Ru system, where blue, brown and white balls represent Co, C and Ru atoms; g schematic illustration of synthesis of Co@CNTs|Ru. Reproduced with permission from Ref. [85]. Copyright 2022, The Author(s)

Fig. 3

Reproduced with permission from Ref. [98]. Copyright 2021, American Chemical Society. Top and side views of optimized structure of 13 H2O molecule on d graphene and e N,O-C, where gray, white, red and blue represent carbon, hydrogen, oxygen and nitrogen atoms, respectively; f schematic illustration of synthesis of IrNi@N,O-C. Reproduced with permission from Ref. [103]. Copyright 2022, Elsevier B.V. g Schematic illustration of synthesis of NS-Ti3C2Tx; h comparison of overpotential (η) of 10 mA·cm−2 and metal-mass activity at − 0.01 V (vs. RHE) under acidic conditions. Reproduced with permission from Ref. [116]. Copyright 2022, Royal Society of Chemistry

Fig. 4

Reproduced with permission from Ref. [142]. Copyright 2019, The Author(s). b Top-view and side-view sp2 hybrid orbitals (highlighted by red dash circle) at the top of valence band and c empty 2p orbitals (highlighted by red dash circle) perpendicular to basal plane at the bottom of conduction band of C-MoS2; d schematic illustration of synthesis of C-MoS2 and MoS2. Reproduced with permission from Ref. [148]. Copyright 2019, The Author(s). e Schematic illustration of chemical etching process to introduce single S-vacancies. Reproduced with permission from Ref. [147]. Copyright 2020, American Chemical Society. f Raman spectra of Pd-MoS2 and MoS2; g H adsorption free energy. Reproduced with permission from Ref. [143]. Copyright 2018, The Author(s). h TEM and corresponding EDX elemental mapping images of Co-Fe-Pd-MoS2. Reproduced with permission from Ref. [149]. Copyright 2020, WILEY–VCH Verlag GmbH & Co. KGaA, Weinheim

Fig. 5

Reproduced with permission from Ref. [151]. Copyright 2021, The Author(s). c Schematic illustration of synthesis of P-WS2 NWAs; d EDX elemental distribution of P-WS2 NWAs; e total DOS of WS2 and P-WS2; f side-view of orbitals around EF of P-WS2; g PDOS of S and W in WS2 (upper), and P, S, W in P-WS2 (lower), respectively. Reproduced with permission from Ref. [153]. Copyright 2021, Tsinghua University Press and Springer-Verlag GmbH. h Schematic illustration of synthesis of CoS@CoNi-LDH/CC heterostructure. Reproduced with permission from Ref. [158]. Copyright 2020, American Chemical Society. i Charge density difference plot at Ni3S2-FeS interface, where light blue, yellow and light purple indicate Ni, S and Fe atoms, respectively. j Positive and k negative values of charge density difference plot at Ni3S2/FeS interface. Reproduced with permission from Ref. [160]. Copyright 2020, Elsevier B.V

Fig. 6

Reproduced with permission from Ref. [169]. Copyright 2021, Elsevier Ltd. b Comparison of free energy profiles of H2 generation in undoped and N, P-doped MoxC. Reproduced with permission from Ref. [170]. Copyright 2021, American Chemical Society. c DOSs of Mo2C@NG, Mo2C and NG catalysts; d calculated Mo d-orbitals of Mo2C@NG and Mo2C catalysts; e ‒COHP functions of Mo2C@NG and NC catalysts, where pCOHP and ICOHP represent local and integral values of COHP, respectively. Reproduced with permission from Ref. [171]. Copyright 2021, The Authors. PDOS of f MoC, g Mo2C, and h MoC-Mo2C heterojunction interface; i relative energy diagram of water dissociation on MoC, Mo2C and MoC-Mo2C in alkaline solution, where TS means transition state; j HRTEM image of MoC-Mo2C powders. Reproduced with permission from Ref. [173]. Copyright 2021, The Author(s). k HRTEM image of interface between Mo2C (100) and MoC (111) in Mo2C/MoC/CNT film; l free energy diagram of HER for different adsorption sites on Mo2C (100), MoC (111) and Mo2C (100)/MoC (111) heterostructure; m XPS spectra of Mo 3d in MoC powder, Mo2C/MoC/CNT film and Mo2C powder; n schematic illustration of synthesis of Mo2C/MoC/CNT. Reproduced with permission from Ref. [174]. Copyright 2022, The Author(s)

Fig. 7

Reproduced with permission from Ref. [189]. Copyright 2021, Elsevier B.V. d Total and partial electronic density of states calculated for Co (111) and MoN (200); e adsorption Gibbs free energy diagram for HER pathway on Co/MoN, Co and MoN. Reproduced with permission from Ref. [190]. Copyright 2021, Elsevier B.V. f Calculated adsorption energies of H2O and H on surface. Reproduced with permission from Ref. [193]. Copyright 2022, Wiley–VCH GmbH. g Synchrotron-based Mo L edge XANES spectra for V0.2Mo0.8N1.2 and MoN1.2; h differential charge density of V-doped MoN1.2, where yellow contour represents electron accumulation; i free energy diagram for HER on MoN1.2 and V-doped Mo5N6, and (inset) schematic top view of corresponding atomic structure. Reproduced with permission from Ref. [200]. Copyright 2022, The Authors

Fig. 8

Reproduced with permission from Ref. [214]. Copyright 2021, Wiley–VCH GmbH. c Schematic illustration of Ni2P@Ti3C2Tx heterostructure; d free energy diagram of HER on Ni2P (blue line) and Ni2P@Ti3C2 MXene (green line) surfaces. Reproduced with permission from Ref. [213]. Copyright 2022, Wiley–VCH GmbH. Raman mapping images of e MoS2 and f converted MoP; g schematic illustration of chemical conversion process from MoS2 to MoP; h high-resolution XPS profiles of S in MoP converted from MoS2. Reproduced with permission from Ref. [216]. Copyright 2022, Wiley–VCH GmbH. EDS elemental mapping images of FeP/Ni2P/CP: i Fe, j P, and k Ni; l simulated DOS of Fe-3d orbital, Ni-3d orbital and P-3p orbital in FeP/Ni2P; m charge density for FeP/Ni2P, where yellow represents charge accumulation and blue represents charge dissipation. Reproduced with permission from Ref. [223]. Copyright 2022, Royal Society of Chemistry

Fig. 9

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 52102470)

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Authors and Affiliations

  1. School of Resources, Environment and Materials, Guangxi University, Nanning, 530004, China

    Huan He, Jin-Hua Mai, Kun-Song Hu & Feng Zhan

  2. School of Transportation Science and Engineering, Beihang University, Beijing, 102206, China

    Han-Qing Yu & Xin-Hua Liu

  3. IDTECH (Suzhou) Co.,Ltd., Suzhou, 215217, China

    Zhen-Guo Zhang

  4. Dyson School of Design Engineering, Imperial College London, London, SW7 2AZ, UK

    Xin-Hua Liu

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  1. Huan He
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He, H., Mai, JH., Hu, KS. et al. Recent advances in electrocatalysts for efficient hydrogen evolution reaction. Rare Met. (2024). https://doi.org/10.1007/s12598-024-02649-1

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