Interface engineering of advanced electrocatalysts toward alkaline hydrogen evolution reactions

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

Chinese Journal of Catalysis ›› 2024, Vol. 66: 1-19.DOI: 10.1016/S1872-2067(24)60130-0

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)

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60130-0

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Figures/Tables 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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Interface engineering of advanced electrocatalysts toward alkaline hydrogen evolution reactions

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