大电流密度过渡金属硫族化合物析氢催化剂界面工程展望

doi:10.1016/S1872-2067(23)64571-1

催化学报 ›› 2024, Vol. 56: 9-24.DOI: 10.1016/S1872-2067(23)64571-1

大电流密度过渡金属硫族化合物析氢催化剂界面工程展望

康馨^,¹, 余强敏^,¹, 张天昊, 胡书萁, 刘鹤鸣, 张致远, 刘碧录^*()

清华大学深圳国际研究生院, 清华-伯克利深圳学院&材料研究院, 深圳盖姆石墨烯中心, 广东深圳518055

收稿日期:2023-10-01 接受日期:2023-11-16 出版日期:2024-01-18 发布日期:2024-01-10
通讯作者: *电子信箱: bilu.liu@sz.tsinghua.edu.cn (刘碧录).
作者简介:¹共同第一作者.
基金资助:
国家杰出青年科学基金项目(52125309);国家自然科学基金(52188101);国家自然科学基金(52303375);广东省基础与应用基础研究基金项目(2022B1515120004);广东创新创业研究团队项目(2017ZT07C341);深圳市基础研究项目(WDZC20220812141108001);深圳鹏瑞基金会清华深圳国际研究生院深圳鹏瑞青年教师项目(SZPR2023002)

A perspective on interface engineering of transition metal dichalcogenides for high-current-density hydrogen evolution

Xin Kang^,¹, Qiangmin Yu^,¹, Tianhao Zhang, Shuqi Hu, Heming Liu, Zhiyuan Zhang, Bilu Liu^*()

Shenzhen Geim Graphene Center, Tsinghua-Berkeley Shenzhen Institute & Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, Guangdong, China

Received:2023-10-01 Accepted:2023-11-16 Online:2024-01-18 Published:2024-01-10
Contact: *E-mail: bilu.liu@sz.tsinghua.edu.cn (B. Liu).
About author:Bilu Liu is a full professor and principal investigator at Tsinghua Shenzhen International Graduate School (Tsinghua SIGS), Tsinghua University, China. He received his bachelor’s degree in materials chemistry from the University of Science and Technology of China (USTC) in 2006, and PhD degree in materials science from the Institute of Metal Research, Chinese Academy of Sciences (IMR, CAS) in 2012. His research interests cover the chemistry and materials science of low-dimensional materials with emphasis on carbon nanostructures, two-dimensional materials, and their heterostructures. His work relates to the growth mechanism investigation, controlled mass production of these materials and their applications in energy, electronics, optoelectronics, and sensing.
First author contact:¹Contributed equally to this work.
Supported by:
National Science Foundation of China for Distinguished Young Scholars(52125309);National Natural Science Foundation of China(52188101);National Natural Science Foundation of China(52303375);Guangdong Basic and Applied Basic Research Foundation(2022B1515120004);Guangdong Innovative and Entrepreneurial Research Team Program(2017ZT07C341);Shenzhen Basic Research Project(WDZC20220812141108001);Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation(SZPR2023002)

摘要/Abstract

摘要：

氢能是未来可持续社会中理想的能量载体, 利用可再生能源电解水制取绿氢的技术受到研究人员的广泛关注. 电解水制绿氢技术由实验室向工业应用跨越的前提是发展大电流密度下性能优异且稳定的电催化剂. 析氢反应(HER)是一种非均相反应, 涉及催化剂-基底、催化剂-电解液、催化剂-气体三个界面. 界面性质会影响电化学传质行为、电荷传输行为和催化剂的力学性质, 从而影响大电流密度下制氢性能. 因此, 优化界面结构和性质是提升大电流密度下电解水催化剂性能并解决电解水技术工业应用挑战的关键.

二维过渡金属硫族化合物(TMDCs)具有电子结构可调、活性位点丰富、合成方法多样等优势, 自1976年首次应用于光电催化水分解反应、加氢脱硫反应以来, 已有大量工作报道了TMDCs催化剂应用于HER. 本文以TMDCs催化剂为例研究界面工程对大电流密度下HER的提升作用及机制. 探讨了电化学反应中上述三个界面上发生的物理化学过程, 系统分析了大电流密度下质量传输、电荷传输速率受限和力学强度不足三方面挑战, 并总结了适用于大电流密度的催化剂性能描述符. 分别归纳了针对以上三个界面的界面工程策略及相应作用, 简要概括为: (1) 催化剂-基底界面结合力增强、界面电阻降低、界面电子结构调控等策略; (2) 催化剂-电解液界面形貌调控、表面化学、电解液环境调控等策略; (3) 催化剂-气体界面疏气性调控、外场作用等策略. 从反应机理研究、膜电极界面设计及电解槽界面性质调控三个角度对电解水反应界面工程未来的发展与应用提出了建议及展望. 在反应机理方面, 大电流条件下的界面性质如界面电阻、传质行为等仍需更深入的认识. 在膜电极中, 催化剂、离子交换膜、离子型聚合物、气体扩散层所形成的多元界面, 尤其是催化剂-膜界面、催化剂-气体扩散层界面的结构仍需进一步优化以提升膜电极的活性及稳定性. 在电解槽界面性质调控方面, 催化剂-基底界面结合力等参数与催化剂寿命间的关系, 电解过程中界面处的温度场及流场分布, 适配于实际生产系统的电流密度等仍需深入研究.

综上, 本文从基本物理化学过程、策略及作用、挑战与展望等多个方面介绍了界面工程. 本文有助于研究人员理解非均相电化学反应过程中界面的重要作用, 提出催化剂、膜电极、电解槽界面设计新策略, 并开发新型表征方法以深入对界面性质的认识, 推动高效电解水技术的开发及应用.

关键词: 界面工程, 电化学, 制氢反应, 大电流, 过渡金属硫族化合物, 膜电极

Abstract:

abstract: Water electrolysis for green hydrogen production is important for the global carbon neutrality. The industrialization of this technology requires efficient and durable electrocatalysts under high-current-density (HCD) operations. However, the insufficient mass and charge transfer at the various interfaces lead to unsatisfactory HCD activity and durability. Interface engineering is important for designing efficient HCD electrocatalysts. In this perspective, we analyze the processes taking place at three interfaces including the catalyst-substrate, catalyst-electrolyte, and catalyst-gas interfaces, and reveal the correlations between interface interactions and the challenges for HCD electrolysis. We then highlight the development of HCD electrocatalysts that focus on interface engineering using the example of transition metal dichalcogenide based catalysts, which have attracted widespread interests in recent years. Finally, we give an outlook on the development of interface engineering for the industrialization of water electrolysis technology.

Key words: Interface engineering, Electrochemistry, Hydrogen production, High-current-density, Transition metal, dichalcogenides (TMDCs), Membrane electrode assembly

康馨, 余强敏, 张天昊, 胡书萁, 刘鹤鸣, 张致远, 刘碧录. 大电流密度过渡金属硫族化合物析氢催化剂界面工程展望[J]. 催化学报, 2024, 56: 9-24.

Xin Kang, Qiangmin Yu, Tianhao Zhang, Shuqi Hu, Heming Liu, Zhiyuan Zhang, Bilu Liu. A perspective on interface engineering of transition metal dichalcogenides for high-current-density hydrogen evolution[J]. Chinese Journal of Catalysis, 2024, 56: 9-24.

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图/表 12

Fig. 1. Milestones in the development of TMDCs for catalysis. Around 1976, TMDC catalysts were first reported. MoS2 constituted a new class of electrodes with unusual photocatalytic, photo-electrocatalytic, and hydrodesulfurization catalytic properties. Around 2006, MoS2 emerged as a new class of HER electrocatalyst under the theoretical guidance. Studies focused on the identification of active sites. Around 2010, the variety of TMDC catalyst family for HER expanded to CoS2, WS2, TaS2, etc. Researchers promote catalytic performance by enriching active sites and modulating intrinsic activity. Around 2019, the industrialization of water electrolysis technology stimulated the development of HCD HER catalyst and interface engineering played a key role in the catalyst design.

Table 1 Summary of state-of-the-art TMDC electrocatalysts for HER operating under HCD (≥ 1000 mA cm?2) with electrode area ≥ 1 cm2.

Year	Catalyst	Performance	Test condition	Ref.
2019	MoS₂/Mo₂C	220 mV @1000 mA cm^-2 24 h @200 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Ti foil, electrode area: 1 cm²	[36]
2020	Co-MoS₂	296 mV @1500 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon cloth, electrode area: 1 cm²	[46]
	Co/Se-MoS₂	389 mV @1000 mA cm^-2 360 h @1000 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon fiber paper, electrode area: 1 cm²	[47]
2021	V-MoS₂ film	600 mV @1000 mA cm^-2 24 h @50 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, graphite sheet, electrode area: 1 cm²	[48]
	P-MoS₂@CoP	1.97 V @1000 mA cm^-2 40 h @500 mA cm^-2	two-electrode cell, 30 wt% KOH, carbon cloth, electrode area: 1 cm²	[49]
	CSS-NiS₂/MoS₂	300 mV @1300 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Ni foam, electrode area: 1 cm²	[50]
	MoS₂-Mo₂C	446 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Mo electrode, electrode area: 1 cm²	[51]
	MoSe₂-Mo₂N	462 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Mo mesh, electrode area: 1 cm²	[52]
	NiSe/Ni₃Se₂	336 mV @1250 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, NF, electrode area: 2 cm²	[53]
	2D MoS₂/EC	410 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Cu foam, electrode area: 1.5 cm²	[54]
	Ta-TaS₂	398 mV @2000 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, Ta foil, electrode area: 1 cm²	[35]
2022	Co-MoS₂/V₂C	296 mV @1000 mA cm^-2 50 h @0.33 V	three-electrode cell, 1 mol L^-1 KOH, carbon cloth, electrode area: 1.5 cm²	[55]
	N-WS₂/Co₃N	1.6 V @3600 mA cm^-2 45 h @500 mA cm^-2	two-electrode cell, 1 mol L^-1 KOH + 0.5 mol L^-1 urea, Ni foam, electrode area: 6 cm²	[56]
	CuMo₆S₈	334 mV @2500 mA cm^-2 100 h @2500 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Cu foam, electrode area: 1 cm²	[57]
	MoS₂NS_s	2.25 V @2000 mA cm^-2 40 h @10 mA cm^-2	two-electrode cell, 0.5 mol L^-1 H₂SO₄, CFP electrode, electrode area: 5 cm²	[58]
	MoS₂-P₂	395 mV @1000 mA cm^-2 240 h @-0.3 V vs. RHE	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon cloth, electrode area: 2 cm²	[59]
	WS₂-WC	473 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, W mesh, electrode area: > 1 cm²	[60]
	Ni₃N@2M-MoS₂	1.64 V @1000 mA cm^-2 300 h @1000 mA cm^-2	two-electrode cell, 1 mol L^-1 KOH, NF, electrode area: 1 cm²	[61]
	a-MoWS_x/N-RGO	348 mV @1000 mA cm^-2 24 h @400 mV	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon paper, electrode area: 1 cm²	[62]
	NiMoPSO NCAs	0.551 V @1600 mA cm^-2 73 h @100 mA cm^-2	two-electrode cell, 1 mol L^-1 KOH + 0.5 mol L^-1 N₂H₄, NF, electrode area: 1 cm²	[63]

Table 1 Summary of state-of-the-art TMDC electrocatalysts for HER operating under HCD (≥ 1000 mA cm?2) with electrode area ≥ 1 cm2.

Year	Catalyst	Performance	Test condition	Ref.
2019	MoS₂/Mo₂C	220 mV @1000 mA cm^-2 24 h @200 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Ti foil, electrode area: 1 cm²	[36]
2020	Co-MoS₂	296 mV @1500 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon cloth, electrode area: 1 cm²	[46]
	Co/Se-MoS₂	389 mV @1000 mA cm^-2 360 h @1000 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon fiber paper, electrode area: 1 cm²	[47]
2021	V-MoS₂ film	600 mV @1000 mA cm^-2 24 h @50 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, graphite sheet, electrode area: 1 cm²	[48]
	P-MoS₂@CoP	1.97 V @1000 mA cm^-2 40 h @500 mA cm^-2	two-electrode cell, 30 wt% KOH, carbon cloth, electrode area: 1 cm²	[49]
	CSS-NiS₂/MoS₂	300 mV @1300 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Ni foam, electrode area: 1 cm²	[50]
	MoS₂-Mo₂C	446 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Mo electrode, electrode area: 1 cm²	[51]
	MoSe₂-Mo₂N	462 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Mo mesh, electrode area: 1 cm²	[52]
	NiSe/Ni₃Se₂	336 mV @1250 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, NF, electrode area: 2 cm²	[53]
	2D MoS₂/EC	410 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Cu foam, electrode area: 1.5 cm²	[54]
	Ta-TaS₂	398 mV @2000 mA cm^-2	three-electrode cell, 0.5 mol L^-1 H₂SO₄, Ta foil, electrode area: 1 cm²	[35]
2022	Co-MoS₂/V₂C	296 mV @1000 mA cm^-2 50 h @0.33 V	three-electrode cell, 1 mol L^-1 KOH, carbon cloth, electrode area: 1.5 cm²	[55]
	N-WS₂/Co₃N	1.6 V @3600 mA cm^-2 45 h @500 mA cm^-2	two-electrode cell, 1 mol L^-1 KOH + 0.5 mol L^-1 urea, Ni foam, electrode area: 6 cm²	[56]
	CuMo₆S₈	334 mV @2500 mA cm^-2 100 h @2500 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, Cu foam, electrode area: 1 cm²	[57]
	MoS₂NS_s	2.25 V @2000 mA cm^-2 40 h @10 mA cm^-2	two-electrode cell, 0.5 mol L^-1 H₂SO₄, CFP electrode, electrode area: 5 cm²	[58]
	MoS₂-P₂	395 mV @1000 mA cm^-2 240 h @-0.3 V vs. RHE	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon cloth, electrode area: 2 cm²	[59]
	WS₂-WC	473 mV @1000 mA cm^-2	three-electrode cell, 1 mol L^-1 KOH, W mesh, electrode area: > 1 cm²	[60]
	Ni₃N@2M-MoS₂	1.64 V @1000 mA cm^-2 300 h @1000 mA cm^-2	two-electrode cell, 1 mol L^-1 KOH, NF, electrode area: 1 cm²	[61]
	a-MoWS_x/N-RGO	348 mV @1000 mA cm^-2 24 h @400 mV	three-electrode cell, 0.5 mol L^-1 H₂SO₄, carbon paper, electrode area: 1 cm²	[62]
	NiMoPSO NCAs	0.551 V @1600 mA cm^-2 73 h @100 mA cm^-2	two-electrode cell, 1 mol L^-1 KOH + 0.5 mol L^-1 N₂H₄, NF, electrode area: 1 cm²	[63]

Fig. 2. Developments and research status of electrocatalysts for HCD HER. (a) Bar chart of the numbers of articles published per year from 2018 to 2022 on HER (grey) and HCD HER (red). The data for HER were obtained by searching the keywords “(“hydrogen evolution”) OR (“hydrogen production”) OR (“water splitting”)” AND “(“electrocataly*”) OR (“electrochem*”)” from Web of Science. The data for HCD HER were obtained by adding ‘‘(“high current densit*”) OR (“large current densit*”) OR (“A cm?2”) OR (“1000 mA”)) OR (“1500 mA”) OR (“2000 mA”)” as the keywords. Note that the catalysts are not limited to TMDC materials in Fig. 2(a). (b) The red square symbol and line plots show the maximum current density reported in the articles published per year from 2019 to 2022 on TMDC electrocatalysts for HER in three-electrode cells with electrode area ≥ 1 cm2. The grey bars stand for the number of articles achieving HCD of 1000 mA cm?2 with electrode area ≥ 1 cm2. Details of state-of-the-art TMDC electrocatalysts for HCD HER reported from 2019 to 2022 are summarized in Table 1. The data in Fig. 2(b) and Table 1 were obtained by following two steps. First, we add “(“TMDC”) OR (“Transition metal *chalcogenide”) OR (“*chalcogenide”) OR (“*disulfide”)) OR (“MoS2”) OR (“WS2”)” as the keywords. Second, publications with required current density (1000 mA cm?2) and electrode area (≥ 1 cm2) were manually selected from searching results given by Web of Science.

Fig. 3. Two new criteria to evaluate catalyst performance under HCD conditions. (a) Rη/j defined as Δη/Δlog/j/ which can describe the reaction kinetics under large η. Here η stands for the overpotential and j stands for the current density. (b) Rη/j of HC-MoS2/Mo2C and Pt/C in a wide current range of 0?1000 mA cm?2. (c) Dv defined as $\frac{\overline{V_{1}}-\overline{V_{2}}}t$ or $\frac{\mathrm{j}_1-\mathrm{j}_2}t$. DA defined as $\frac{\overline{\mathrm{V}_1}-\overline{\mathrm{V}_2}}{\mathrm{t}\overline{\mathrm{V}_1}}$ or $\frac{\text{j}_1\overline{\mathrm{j}_2}}{\mathrm{t}\overline{\mathrm{j}_1}}$. Here t stands for the duration of the chronopotentiometry (CP) or the chronoamperometry (CA) test. V?1, V?2, j?1, and j?2 stand for the average of potentials in a CP test or current densities in a CA test during the initial/final 10% t. (d) Dv of RuMoNi electrocatalyst. The overpotential increase of a durable RuMoNi electrocatalyst after ten years’ operation is speculated to be 56 mV based on the DV.

Table 2 HER performance of Pt-based materials under HCD of 500 and 1000 mA cm?2.

Standard material	Catalyst	Electrolyte	η₅₀₀ (mV)	η₁₀₀₀(mV)	Ref.
Pt/C	Pt/C-nickel foam (NF)	1 mol L^‒1 KOH	370	490	[69]
	Pt/C	1 mol L^‒1 KOH	355	415	[70]
	Pt/C-Cu foam	1 mol L^‒1 KOH	400	450	[57]
	Pt/C-NF	1 mol L^‒1 KOH	281	444	[71]
	Pt/C-Cu foam	0.5 mol L^‒1 H₂SO₄	340	400	[70]
	Pt/C-Cu sheet	0.5 mol L^‒1 H₂SO₄	328	760	[40]
Pt foil	Pt foil	1 mol L^‒1 KOH	570	822	[36]
	Pt foil	1 mol L^‒1 KOH	500	640	[42]
	Pt foil	0.5 mol L^‒1 H₂SO₄	270	435	[35]
	Pt foil	0.5 mol L^‒1 H₂SO₄	380	660	[36]
Pt mesh	Pt mesh	0.5 mol L^‒1 H₂SO₄	560	958	[70]
Pt wire	Pt wire	1 mol L^‒1 KOH	310	388	[70]
Pt wire	Pt wire	0.5 mol L^‒1 H₂SO₄	87	109	[38]

Fig. 4. Schematics of the interfaces between the catalyst, substrate, electrolyte, and gas. (a) Schematics show the charge transfer process and Fb on the catalyst-substrate interface. (b) Schematics show the charge transfer and mass transfer processes on the catalyst-electrolyte interface. (c) Schematics show the mass transfer process and Fa on the catalyst-gas interface.

Fig. 5. Three interfaces (catalyst-substrate, catalyst-gas, and catalyst-electrolyte interfaces) and interface engineering strategies to manipulate the interface properties.

Fig. 6. Catalyst-substrate interface engineering. (a,b) Chevrel phase CuMo6S8 catalyst with strong interfacial binding force. Reprinted with permission from Ref. [57]. Copyright 2022, Springer Nature. (c?e) Pt alloy-CoP hybrids with tunable ΔΦ by electronic metal-support interaction. Reprinted with permission from Ref. [87]. Copyright 2021, Springer Nature. (f?h) Electronic property modulation of single-atom Pt on TMDCs. Reprinted with permission from Ref. [88]. Copyright 2021, Springer Nature.

Fig. 7. Catalyst-electrolyte interface engineering. (a?c) MoS2 nanostructured electrode with improved performance. Reprinted with permission from Ref. [93]. Copyright 2014, Wiley-VCH. (d?f) Ni3N@2M-MoS2 composite with two kinds of separated reaction sites. Reprinted with permission from Ref. [61]. Copyright 2022, Wiley-VCH. (g,h) Molybdate anion corrosion-resistant layer over the catalyst-electrolyte interface of the RuMoNi electrocatalyst repelling chlorine ions through electrostatic repulsive force. Reprinted with permission from Ref. [5]. Copyright 2023, Springer Nature.

Fig. 8. Catalyst-gas interface engineering. (a) Schematics for the forces on a single bubble adhering on the electrode surface. F1, F2, and F3 stand for the buoyancy force, the drag force from the flow of liquid past the electrode surface, and the interfacial tension force, respectively. θ stands for the contact angle. R stands for bubble radius. (b,c) Aerophobic PEI improves HER by promoting bubble detachment. Reprinted with permission from Ref. [123]. Copyright 2022, Wiley-VCH. (d?f) HER performance of mosaic Pt/PtS catalyst and other Pt catalysts. Reprinted with permission from Ref. [94]. Copyright 2021, Wiley-VCH. (g) Schematics for the current distribution, the direction of the Lorentz force (FL) in the left part, and the Lorentz-force-driven convection pattern, the so-called magnetohydrodynamic effect in the right part. Reprinted with permission from Ref. [124]. Copyright 2011, Elsevier Ltd. (h) Bubble detaching diameters with and without magnetic fields. (i) CA curves with and without magnetic fields. Reprinted with permission from Ref. [125]. Copyright 2019, Elsevier Ltd.

Table 3 Classification of the literature on catalyst-substrate, catalyst-electrolyte, and catalyst-gas interfaces respectively, based on the interface, catalyst, and effect.

Interface	Catalyst	Interaction	Note	Ref.
Catalyst-substrate	CuMo₆S₈	mechanical strength	strong interfacial binding force	[57]
	MoS_2(1‒_x₎Se₂_x/NiSe₂		chemical bonding between MoS_2(1‒_x₎Se₂_x and NiSe₂	[73]
	CoS₂/rGO-CNT		entanglement of the flexible CNT	[74]
	Ta-TaS₂	interfacial resistance	monolith electrode with almost zero interfacial resistance	[35]
	MoS₂-MGF		interconnective highly conductive skeleton	[73]
	Crumpled MoS₂		size and distribution of electrocatalyst	[80]
	Pt alloy-CoP	electronic structure	tunable difference of work function between substrate and electrocatalyst	[87]
	Pt SACs-MoSe₂	electronic structure	electronic metal-support interaction modulating electronic structure of electrocatalyst	[88]
	MoS₂@Ni₂P	heterostructure catalyst	generating new interfacial electronic state and enabling higher conductivity	[90]
	MoS₂/Mo₂C	heterostructure catalyst	increasing active sites and enhancing mass transfer ability	[36]
Catalyst-electrolyte	Micro-/ nanostructured CoS₂	micro-/ nanostructuring	accelerating the bubble detachment and maintaining the catalyst-electrolyte interface	[31]
	Crumpled MoS₂	micro-/ nanostructuring	size and distribution of electrocatalyst	[80]
	LSC/MoSe₂	interface chemistry	electron-rich surface with favorable intermediate adsorption energy	[72]
	Ni₃N@2M-MoS₂		separated reaction sites to overcome the competitive adsorption of intermediates	[61]
	Ni(OH)₂/MoS₂		metal hydroxides as water dissociation promoters stimulating the process on the MoS₂ edge sites	[102]
	NiCo₂S₄/ReS₂		spin-crossover promoting water dissociation thermodynamically	[103]
	RuMoNi	electrolyte engineering	corrosion-resistant layer formed by anion adsorption	[5]
	CoFePO-Ni foam		anion and cation doping in metal compounds promoting HER kinetics	[110]
	Pd, Ru-MoS_2‒_xOH_y		di-anionic MoS₂ surface with OH and S improving the water dissociation kinetic	[111]
Catalyst-gas	edge-MoS₂/CoS₄@NFs	aerophobicity	aerophobicity by designing the electrode with micro-/nanostructures	[121]
	MoS₂@C supertubes		aerophobicity by making use of the confining effect from the tubular mesoporous graphite framework	[122]
	PEI hydrogel-modified electrode		surface modification increasing the aerophobicity	[123]
	Mosaic PtS		aerophobicity by engineering the active site distribution	[94]
	Ni-PTFE	external field	magnetic field facilitating bubble detachment	[125]
	Pt electrode	external field	intensified effect of centrifugal force field on gas evolution	[128]

Table 3 Classification of the literature on catalyst-substrate, catalyst-electrolyte, and catalyst-gas interfaces respectively, based on the interface, catalyst, and effect.

Interface	Catalyst	Interaction	Note	Ref.
Catalyst-substrate	CuMo₆S₈	mechanical strength	strong interfacial binding force	[57]
	MoS_2(1‒_x₎Se₂_x/NiSe₂		chemical bonding between MoS_2(1‒_x₎Se₂_x and NiSe₂	[73]
	CoS₂/rGO-CNT		entanglement of the flexible CNT	[74]
	Ta-TaS₂	interfacial resistance	monolith electrode with almost zero interfacial resistance	[35]
	MoS₂-MGF		interconnective highly conductive skeleton	[73]
	Crumpled MoS₂		size and distribution of electrocatalyst	[80]
	Pt alloy-CoP	electronic structure	tunable difference of work function between substrate and electrocatalyst	[87]
	Pt SACs-MoSe₂	electronic structure	electronic metal-support interaction modulating electronic structure of electrocatalyst	[88]
	MoS₂@Ni₂P	heterostructure catalyst	generating new interfacial electronic state and enabling higher conductivity	[90]
	MoS₂/Mo₂C	heterostructure catalyst	increasing active sites and enhancing mass transfer ability	[36]
Catalyst-electrolyte	Micro-/ nanostructured CoS₂	micro-/ nanostructuring	accelerating the bubble detachment and maintaining the catalyst-electrolyte interface	[31]
	Crumpled MoS₂	micro-/ nanostructuring	size and distribution of electrocatalyst	[80]
	LSC/MoSe₂	interface chemistry	electron-rich surface with favorable intermediate adsorption energy	[72]
	Ni₃N@2M-MoS₂		separated reaction sites to overcome the competitive adsorption of intermediates	[61]
	Ni(OH)₂/MoS₂		metal hydroxides as water dissociation promoters stimulating the process on the MoS₂ edge sites	[102]
	NiCo₂S₄/ReS₂		spin-crossover promoting water dissociation thermodynamically	[103]
	RuMoNi	electrolyte engineering	corrosion-resistant layer formed by anion adsorption	[5]
	CoFePO-Ni foam		anion and cation doping in metal compounds promoting HER kinetics	[110]
	Pd, Ru-MoS_2‒_xOH_y		di-anionic MoS₂ surface with OH and S improving the water dissociation kinetic	[111]
Catalyst-gas	edge-MoS₂/CoS₄@NFs	aerophobicity	aerophobicity by designing the electrode with micro-/nanostructures	[121]
	MoS₂@C supertubes		aerophobicity by making use of the confining effect from the tubular mesoporous graphite framework	[122]
	PEI hydrogel-modified electrode		surface modification increasing the aerophobicity	[123]
	Mosaic PtS		aerophobicity by engineering the active site distribution	[94]
	Ni-PTFE	external field	magnetic field facilitating bubble detachment	[125]
	Pt electrode	external field	intensified effect of centrifugal force field on gas evolution	[128]

Fig. 9. Perspectives for future developments in interface engineering, including the understanding of interfaces under HCD conditions, designing MEA interfaces in electrolyzer, and tuning interface properties in the industry-level electrolyzer. In the future, interface engineering will accelerate the industrialization of water electrolysis and contribute to the sustainable society.

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大电流密度过渡金属硫族化合物析氢催化剂界面工程展望

A perspective on interface engineering of transition metal dichalcogenides for high-current-density hydrogen evolution

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