碱性电解水析氢反应先进电催化剂的界面工程研究

doi:10.1016/S1872-2067(24)60130-0

催化学报 ›› 2024, Vol. 66: 1-19.DOI: 10.1016/S1872-2067(24)60130-0

• 综述 • 下一篇

碱性电解水析氢反应先进电催化剂的界面工程研究

吴汪洋^a, 杨世丹^a, 钱慧丹^a, 张伶^a^,^*(), 彭立山^b^,^*(), 李莉^a^,^*(), 刘彬^c, 魏子栋^a

^a重庆大学化学化工学院, 特种化学电源全国重点实验室, 化工过程强化与反应国家-地方联合工程实验室, 重庆 400044
^b中国科学院赣江创新研究院, 稀土重点实验室, 江西赣州 341119
^c香港城市大学材料科学与工程学系, 香港九龙塘 999077

收稿日期:2024-07-27 接受日期:2024-08-29 出版日期:2024-11-18 发布日期:2024-11-10
通讯作者: *电子信箱: zhanglinggood@cqu.edu.cn (张伶),liliracial@cqu.edu.cn (李莉),lspeng@gia.cas.cn (彭立山).
基金资助:
国家重点研发计划(2021YFB4000300)

Interface engineering of advanced electrocatalysts toward alkaline hydrogen evolution reactions

Wangyang Wu^a, Shidan Yang^a, Huidan Qian^a, Ling Zhang^a^,^*(), Lishan Peng^b^,^*(), Li Li^a^,^*(), Bin Liu^c, Zidong Wei^a

^aNational Key Laboratory of Special Power Supplies, National-Municipal Joint Engineering Laboratory for Chemical Process Intensification and Reaction, School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
^bKey Laboratory of Rare Earths, Chinese Academy of Sciences, Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341119, Jiangxi, China
^cDepartment of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR, 999077 China

Received:2024-07-27 Accepted:2024-08-29 Online:2024-11-18 Published:2024-11-10
Contact: *E-mail: zhanglinggood@cqu.edu.cn (L. Zhang),iliracial@cqu.edu.cn (L. Li),lspeng@gia.cas.cn (L. Peng).
About author:Ling Zhang (School of Chemistry and Chemical Engineering, Chongqing University) received his B.S. and Ph. D. degrees from Nanjing Tech University in 2014 and Chongqing University in 2022, respectively. Currently, he is a postdoctoral at Chongqing University. His current research interests focus on developing high-performance HER/OER electrocatalysts.
Lishan Peng (Key Laboratory of Rare Earths, Chinese Academy of Sciences, Ganjiang Innovation Academy, Chinese Academy of Sciences) is currently an Associate Professor in the Ganjiang Innovation Academy, Chinese Academy of Sciences. He obtained a Ph.D. degree in Chemical engineering and technology in 2019 at Chongqing University. Subsequently he worked as a postdoctoral researcher at Westlake University (China), the University of Auckland (New Zealand) and the Technical Institute of Physics and Chemistry, Chinese Academy of Sciences. His research interests include the design and theoretical study of advanced electrocatalysts for energy storage and conversion.
Li Li (School of Chemistry and Chemical Engineering, Chongqing University) completed her MSc and PhD degrees in 2004 and 2010, respectively, at Chongqing University. In 2010, she became a faculty member at the College of Chemistry and Chemical Engineering, also at Chongqing University. Her primary research interests revolve around the fundamental studies of electrochemical and electrocatalytic processes through theoretical investigations. Her research focuses on developing new electrocatalysts with high activity and stability, exploring the relationship between catalytic mechanisms and the electronic structure of catalysts, and understanding the underlying mechanisms. She has co-authored over 100 peer-reviewed papers. Some of her main academic achievements include proposing the "triple effect" to explain the enhancement mechanism of doped graphene for ORR, exploring the theoretical foundation for tuning the catalytic activity and stability of carbon-supported Pt-based catalysts, manifesting a general oxygen-vacancies-based regulation mechanism for enhancing the ORR activity of metal oxides, and proposing a "chimney effect" for enhancing HER activity on the interface between metal oxide/metal catalysts.
Supported by:
National Key R&D Program of China(2021YFB4000300)

摘要/Abstract

摘要：

能源需求增加和化石能源燃烧, 造成了严重的环境问题, 威胁人类社会的可持续发展. 开发以氢能为代表的可再生能源是解决人类社会面临的环境危机的必然选择. 电解水制氢耦合风能、太阳能、潮汐能等可再生能源是一种环境友好、可持续的“绿氢”生产方法. 然而, 目前析氢催化剂活性/稳定性差, 制约了电解水制氢技术的大规模应用. 富含异质界面的析氢催化剂具有丰富的物化性质、便于调控的电子结构以及不同活性位点间的协同效应, 受到研究者的广泛关注. 本综述系统地梳理和总结了富含异质界面的碱性析氢催化剂以及电极/溶液界面的研究进展, 对进一步推动该领域的研究具有重要意义.

本文主要从碱性析氢反应机理、活性调控策略以及对未来的展望三个方面进行总结和讨论. 首先简要总结了碱性析氢反应机理, 详细论述了反应动力学缓慢的三个原因: (1) 额外的水解离能垒; (2) 过高的界面水分子重组能; (3) 氢键网络的破坏提高了质子转移的能垒. 其次, 概括了目前两类异质界面型析氢催化剂的活性增强策略: (1) 增强异质界面间多组分协同、内建电场与氢溢流; (2) 促进催化剂/电解液界面间水分子富集、再定向与活化. 前者主要通过界面间电荷转移现象来优化各自组分的电子结构, 进而调控活性位点与反应中间体的吸附与解吸能垒, 以优化析氢催化剂动力学; 后者涉及水分子在催化剂界面上的结构排列, 通过增强催化剂/电解液界面电场, 促进水分子在催化剂表面富集, 调控水分子吸附构型, 活化水分子, 降低水分子解离能垒, 提高析氢催化剂的反应活性. 详细汇总了各个策略背后涉及的电荷转移、界面匹配、活性位点微环境优化等机理. 同时, 分别指出了四种调控策略的不足: (1) 基于多组分协同、内建电场与氢溢流效应的策略, 缺乏精确定制异质界面组成、数量的方法, 难以确定电场对析氢反应活性增强的确切机制, 缺少电场方向和强度对析氢活性影响机制的研究, 导致水分子解离、活性氢生成、活性氢迁移和释放四个过程难平衡; (2) 现有表征难以探究界面水分子在催化剂/溶液界面的精确结构及其随时间演变的规律.

综上, 本文系统总结了富含异质界面的析氢催化剂的优势、研究进展以及目前存在的挑战: 如何保证富含异质界面的析氢催化剂在高温、高碱性以及强极化条件下的稳定性. 希望通过本综述推动相关研究人员进一步思考, 并为进一步推动富含异质界面的析氢催化剂在碱水电解制氢中研究, 为开发高活性、高稳定性富含异质界面的析氢催化剂提供一定的参考和借鉴.

关键词: 电催化, 析氢反应, 界面工程, 协同效应, 内建电场, 氢溢流, 界面水结构

Abstract:

Developing efficient, stable, and low-cost electrocatalysts toward alkaline hydrogen evolution reactions (HER) in water electrolysis driven by renewable energy sources has always been discussed over the past decade. To reduce energy consumption and improve energy utilization efficiency, highly active electrocatalytic electrodes are essential for lowering the energy barrier of the HER. Catalysts featuring multiple interfaces have attracted significant research interest recently due to their enhanced physicochemical properties. Reasonable interface modulation can optimize intermediate active species' adsorption energy, improve catalytic active sites' selectivity, and enhance intrinsic catalytic activity. Here, we provided an overview of the latest advancement in interface engineering for efficient HER catalysts. We begin with a brief introduction to the fundamental concepts and mechanisms of alkaline HER. Then, we analyze and discuss current regulating principles in interface engineering for HER catalysts, focusing particularly on optimizing electron structures and modulating microenvironment reactions. Finally, the challenges and further prospects of interface catalysts for future applications are discussed.

Key words: Electrocatalysis, Hydrogen evolution reaction, Interface engineering, Synergistic effect, Built-in electric field, Hydrogen spillover, Structure of interfacial water

吴汪洋, 杨世丹, 钱慧丹, 张伶, 彭立山, 李莉, 刘彬, 魏子栋. 碱性电解水析氢反应先进电催化剂的界面工程研究[J]. 催化学报, 2024, 66: 1-19.

Wangyang Wu, Shidan Yang, Huidan Qian, Ling Zhang, Lishan Peng, Li Li, Bin Liu, Zidong Wei. Interface engineering of advanced electrocatalysts toward alkaline hydrogen evolution reactions[J]. Chinese Journal of Catalysis, 2024, 66: 1-19.

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图/表 14

Fig. 1. Schematic diagram of HER mechanisms in alkaline media (a), and reasons for sluggish alkaline HER kinetics (b). The O, H, H*, and Na+/K+ are colored pink, light green, green, and purple, respectively.

Fig. 2. (a) Side view of RuO2/Ni (001). (b) Differential charge density of RuO2/Ni (001) projected on the side view. (c) A “Chimney Effect” at the interface. Reprinted with permission from Ref. [87]. Copyright 2019, Elsevier. (d) Chemisorption models of H and OH intermediates on the surfaces of NiMoPOx and the Ni(OH)2/NiMoPOx hybrid. Calculated adsorption energy diagram of the water dissociation step (e) and hydrogen ad-desorption (f). (g) Electrode surface area-normalized polarization curves in 1.0 mol L-1 KOH aqueous solution. (h) Calculated free energy of hydrogen ad-desorption. Reprinted with permission from Ref. [88]. Copyright 2020, Royal Society of Chemistry.

Fig. 3. (a) Charge density distributions between Ru2P/WO3 and different substrates (C, NPC) with a value of 0.002 e?-3. Green represents positive charges and red represents negative charges. (b) Kinetic barriers of water dissociation on the active sites of different catalysts. (c) Calculated Gibbs free energy diagrams for the HER at equilibrium potential vs. RHE for different catalysts. (d) Proposed HER mechanism in alkaline media for the Ru2P/WO3@NPC nanocomposite. Reprinted with permission from Ref. [90]. Copyright 2020, John Wiley and Sons. (e) PDOS of Ru d band and the corresponding band center for MoO2@Ru, MoO2/MoO3@Ru, and MoO3@Ru. (f,g) Water dissociation energies and *H adsorption free energy of different catalysts. (h) Schematic diagram of the mechanism of enhanced HER for MoO2@Ru. Reprinted with permission from Ref. [92]. Copyright 2023, John Wiley and Sons.

Fig. 4. (a) BEF for Ni metal and MoO2 semiconductor. (b) Polarization curves for the HER. Reprinted with permission from Ref. [100]. Copyright 2023, Elsevier. (c) HRTEM image of Ni2P-CoCH/CFP. (d) Energy band diagram of Ni2P and CoCH. (e) Charge density difference plot at the Ni2P-CoCH interface. (f) The calculated H* adsorption Gibbs free energy. (g) Charge density difference plot at the WO3/Ni2P interface. Free energy diagrams of water dissociation (h) and hydrogen adsorption (i). Reprinted with permission from Ref. [101]. Copyright 2023, John Wiley and Sons.

Fig. 5. (a) BEF for Os metal and OsSe2 alloy. (b) Gibbs free energies of HER on Os sites. Reprinted with permission from Ref. [103]. Copyright 2022, John Wiley and Sons. (c) UPS spectra. (d) Diagram of electron redistribution in the Ru NCs/P,O-NiFe LDH. (e) Differential charge density of the Ru NCs/P,O-NiFe LDH. (f) Free energy diagram for HER on different catalysts. (g) HER polarization curves. Reprinted with permission from Ref. [104]. Copyright 2023, John Wiley and Sons.

Fig. 6. Charge-density difference diagram (a) and Plane‐averaged electronic potential (b) along the perpendicular direction of NiS2-ReS2 and NiS2-ReS2-V (V represents Re vacancies). Free energy diagrams of water dissociation (c) and hydrogen adsorption (d). Reprinted with permission from Ref. [106]. Copyright 2024, John Wiley and Sons.

Fig. 7. (a) Diagram of hydrogen spillover. Reprinted with permission from Ref. [114]. Copyright 2024, John Wiley and Sons. (b) Plots of Cφ vs. η of different catalysts. (c) Calculated free energy for HER on Pt/CoP and Pt2Ir1/CoP. (d) Electron density difference map of interfaces. (e) The optimized H* adsorption spillover. Reprinted with permission from Ref. [42]. Copyright 2021, Springer Nature.

Fig. 8. (a) Work function diagram between Ru and MoO2. (b) Energy barriers for HER on different sites. (c) Fitted data of Cφ vs. η. (d) CV curve of Ru/MoO2. Reprinted with permission from Ref. [114]. Copyright 2024, John Wiley and Sons. (e) Energy barriers for water dissociation on the Ru site. (f) Energy barriers for H* adsorption on Ru site. (g) Hydrogen spillover energy barrier with and without potential. Reprinted with permission from Ref. [98]. Copyright 2024, John Wiley and Sons.

Fig. 9. (a) Calculated free energy for H* on different sites. Reprinted with permission from Ref. [116]. Copyright 2021, John Wiley and Sons. (b) The differential charge density distributions between Ru and NiMoO4-x and NiMoO4. (c) Calculated free energy diagram of Ru/NiMoO4-x and Ru/NiMoO4-x. (d) Diagram of the possible path of hydrogen spillover. Reprinted with permission from Ref. [112]. Copyright 2023, John Wiley and Sons.

Fig. 10. (a) Calculated free energy diagram for HER. Reprinted with permission from Ref. [41]. Copyright 2022, Springer Nature. HER mechanism (b) and reaction energy (c) on different sites. Reprinted with permission from Ref. [117]. Copyright 2024, Royal Society of Chemistry.

Fig. 11. Laser-induced coulostatic potential transients collected for the Pt (111) (a) and Pt(111)/Ni(OH)2 (b). Reprinted with permission from Ref. [53]. Copyright 2017, Springer Nature. (c) In situ electrochemical Raman spectra (grey curves) of the O-H stretching mode. (d) AIMD simulations and in situ electrochemical Raman spectra of the hydrogen-bond network of interfacial water. Reprinted with permission from Ref. [124]. Copyright 2019, Springer Nature.

Fig. 12. In situ electrochemical Raman spectra at different catalyst surfaces in 0.1 mol L-1 HClO4 (a) and 0.1 mol L-1 NaOH (b,c). (d,e) In situ electrochemical Raman spectra of the O-H stretching mode in catalysts with different Ni contents. Reprinted with permission from Ref. [55]. Copyright 2020, John Wiley and Sons.

Fig. 13. (a) Simulated distribution of potential and hydrated K+ concentration for TiO2-Pt/C. (b) The energy barrier of water dissociation. (c) Radial distribution function of interface water structure in KOH solution. (d) The energy barrier of H* ad-desorption. Reprinted with permission from Ref. [131]. Copyright 2022, American Chemcial Society. (e) Charge density analyses of CoP and IrRu. (f) Interfacial water orientation simulated by AIMD. (g) The energy barrier of water dissociation. Reprinted with permission from Ref. [132]. Copyright 2023, John Wiley and Sons.

Table 1 Comparison between Alkaline HER catalysts of various strategies in 1 mol L-1 KOH (The overpotential values with the symbol (~) are extracted from their corresponding LSV plots).

Strategy	Catalyst	η₁₀ (mV)	η₁₀₀ (mV)	η₅₀₀ (mV)	Year	Ref.
Synergistic effects	Ni/Ni(OH)₂	77	~150	—	2020	[89]
	(Ru-Co)O_x	44	89	—	2020	[135]
	Ni(OH)_x/NiNiPO_x	51	72	—	2020	[88]
	Ru₂P/WO₃/NPC	15	—	—	2021	[90]
	Pt-Co/CoO_x	28	—	—	2021	[136]
	CoFe-LDH@NiSe	38	~250	—	2022	[137]
	Ni/NiO-cp	72	~180	—	2022	[78]
	MoO₂@Ru NT	22	~50	89	2023	[92]
	Co/CoO/Co₂Mo₃O₈	78	213	~280	2023	[75]
	CFO/CoFe-LDH	—	188	~280	2024	[138]
BEF	Os-OsSe₂	23	—	—	2022	[103]
	Ru-CMOP	—	114	183	2022	[96]
	Ni₂P/Ni₅P₄	62	166	380	2023	[97]
	Ni₂P-CoCH/CFP	62	143	—	2023	[101]
	RuNCs/P,O-NiFe LDH/NF	29	200	—	2024	[104]
	NiS₂‐ReS₂‐V	42	140	—	2024	[106]
	20-WO₃/Ni₂P/NF	—	180	269	2024	[102]
	Mo₅N₆-Ni₃S₂ HNPs/NF	59	300	—	2024	[97]
Hydrogen spillover	Pt/CoP	21	~100	—	2019	[113]
	PtIr/CoP	5	50	—	2021	[42]
	Ni₃S₂/Cr₂S₃	55	160	207	2022	[110]
	Cr, Fe-CoP/NF	27	~95	~140	2024	[139]
	Ru₁-Mo₂C	11	57	—	2024	[117]
	Ru/MoO₂	9	110	—	2024	[114]
Water regulation	TiO₂-Pt/C	26	~60	100	2022	[131]
Water regulation	IrRu DSACs	10	78	286	2023	[132]

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碱性电解水析氢反应先进电催化剂的界面工程研究

Interface engineering of advanced electrocatalysts toward alkaline hydrogen evolution reactions

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