Ultrathin two-dimensional electrocatalysts: Structure-property relationships, mechanistic insights, and applications in water electrolysis

doi:10.1016/S1872-2067(25)64783-8

Chinese Journal of Catalysis ›› 2025, Vol. 77: 4-19.DOI: 10.1016/S1872-2067(25)64783-8

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Ultrathin two-dimensional electrocatalysts: Structure-property relationships, mechanistic insights, and applications in water electrolysis

Lina Wang^a, Muhan Na^a, Ruofei Du^a, Xiujin Wang^a, Boyang Yu^a, Lan Yang^b, Hui Chen^a^,^*(), Xiaoxin Zou^a^,^*()

^aState Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, Jilin, China
^bBeijing Institute of Smart Energy, Beijing 102209, China

Received:2025-05-15 Accepted:2025-06-30 Online:2025-10-18 Published:2025-10-05
Contact: *xxzou@jlu.edu.cn (X. Zou), chenhui@jlu.edu.cn (H. Chen).
About author:Hui Chen has received his Ph.D. in materials science from Jilin University (China) in June 2018, and completed his postdoctoral training at College of Chemistry, Jilin University from June 2018 to November 2022. He is currently a professor at the State Key Laboratory of Inorganic Synthesis and Preparative Chemistry in Jilin University. His research interests are in catalytic materials for water electrolysis technologies, including alkaline water electrolyzer (AWE) and proton exchange membrane water electrolyzer (PEMWE). Some of his recent progresses include (i) the development of low‐iridium oxygen‐evolution catalysts and anode catalyst layers for PEMWEs, and (ii) the large‐area synthesis of highly active and stable nickel-based electrodes for AWEs. He has authored 40+ peer-reviewed papers and 10 patents.
Xiaoxin Zou (State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University) has received his PhD in inorganic chemistry from Jilin University in June 2011, and then moved to the University of California, Riverside, and Rutgers, The State University of New Jersey, as a postdoctoral scholar from July 2011 to October 2013. He is currently a professor at the State Key Laboratory of Inorganic Synthesis and Preparative Chemistry in Jilin University. His research interests are in hydrogen energy materials chemistry, comprising the elucidation of the atomic basis for water splitting electrocatalysts, prediction and searching of efficient catalysts with novel crystal structures and preparative technology of industrial water splitting catalysts.
Supported by:
State Grid Headquarter Science and Technology project(5419-202320652A-3-2-ZN)

Abstract

Abstract:

The pursuit of sustainable hydrogen production has positioned water electrolysis as a cornerstone technology for global carbon neutrality. However, sluggish kinetics, catalyst scarcity, and system integration challenges hinder its widespread deployment. Ultrathin two-dimensional (2D) materials, with their atomically exposed surfaces, tunable electronic structures, and defect-engineering capabilities, present unique opportunities for next-generation electrocatalysts. This review provides an integrated overview of ultrathin 2D electrocatalysts, discussing their structural diversity, synthetic routes, structure-activity relationships, and mechanistic understanding in water electrolysis processes. Special focus is placed on the translation of 2D materials from laboratory research to practical device implementation, emphasizing challenges such as scalable fabrication, interfacial engineering, and operational durability in realistic electrolyzer environments. The role of advanced characterization techniques in capturing dynamic structural changes and active site evolution is discussed. Finally, we outline future research directions, emphasizing the synergy of machine learning-driven materials discovery, advanced operando characterization, and scalable system integration to accelerate the industrial translation of 2D electrocatalysts for green hydrogen production.

Key words: Two-dimensional material, Water splitting reaction, Electrocatalysis, Catalytic mechanism, Electrolyzer

Lina Wang, Muhan Na, Ruofei Du, Xiujin Wang, Boyang Yu, Lan Yang, Hui Chen, Xiaoxin Zou. Ultrathin two-dimensional electrocatalysts: Structure-property relationships, mechanistic insights, and applications in water electrolysis[J]. Chinese Journal of Catalysis, 2025, 77: 4-19.

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Figures/Tables 8

Fig. 1. Schematic diagrams of 2D metal oxides (e.g., Honeycomb oxides, ABO2-type oxides and RP pervoskite), LDHs and TMDs with 1T, 2H, and 3R crystal phases.

Fig. 2. Schematic illustration of top-down and bottom-up synthesis methods for 2D materials.

Fig. 3. Schematic illustration of active site modulation strategies for 2D electrocatalysts, including phase engineering, heteroatomic doping, defect engineering, morphological control and strain effect.

Fig. 4. (a) TEM images of Pt-MoS2. (b) HAADF-STEM images of Pt-MoS2, with the red circle represented single Pt atoms. (c) Theoretical volcano plot of HER activity for various metal-doped MoS2 systems. (a-c) Reprinted with permission from Ref. [104]. Copyright 2015, The Royal Society of Chemistry. (d) ACTEM image of MoS2 monolayer with different S-vacancies. (e) Schematic illustration of top and side views of MoS2 basal planes incorporating strained S-vacancies. (f) ?GH versus %x-strain for various %S-vacancy. (d-f) Reprinted with permission from Ref. [108]. Copyright 2016, Springer Nature.

Fig. 5. (a) Theoretical volcano plot delineating the OER activity of edge sites and in-plane sites in layered iridium oxides. (b) Schematic illustration of the synthesis of high porous layered IrOx. Reprinted with permission from Ref. [113]. Copyright 2024, Chinese Chemical Society. (c) Schematic illustration of the synthesis of multi-defect HxIrOy nanosheets. (d) HAADF-STEM image of multi-defect HxIrOy nanosheets. Reprinted with permission from Ref. [112]. Copyright 2025, Wiley-VCH. (e) SEM image of 3R-IrO2. The proton transportation pathway along (f) interlayers and (g) intralayers of 3R-IrO2. Reprinted with permission from Ref. [114]. Copyright 2021, Elsevier Inc.

Fig. 6. (a) Synthesis of CAPist-L1 catalyst and the corresponding cross-sectional SEM image. (b) Long-term durability of CAPist-L1, NiFe-LDH, CAPist-L1(H2O) and IrO2 evaluated at 1000?mA/cm-2. Reprinted with permission from Ref. [118]. Copyright 2024, Springer Nature. (c) Structure of (Ni, Fe)3S2/NFF and the schematic illustration of its dual role as both anode and cathode catalysts in an electrolyzer. (d) Optical photos of large-area NFF before and after the sulfuration treatment. e) SEM images of (Ni, Fe)3S2/NFF in different selected areas. Reprinted with permission from Ref. [119]. Copyright 2024, Wiley-VCH.

Fig. 7. (a) HAADF-STEM image and (b) the corresponding aberration-corrected aberration HAADF-STEM image for Re0.03Ir0.97O2. (c) The polarization curve of Re0.03Ir0.97O2-based PEM electrolyzer. Reprinted with permission from Ref. [122]. Copyright 2025, Wiley‐VCH. (d) Schematic illustration of multilevel structural optimization for H-IrOx FPs-based anodic catalyst layer. (e) The 3D model of porous H-IrOx FPs. (f) Relative contributions of ηKinetic, ηOhmic, and ηTransport for H-IrOx FPs-, H-IrOx SPs- and R-IrO2 NPs-based PEMWE. Reprinted with permission from Ref. [127]. Copyright 2024, Wiley‐VCH. (g) Schematic representation of low-ionomer-dependent anode catalyst layer based on ?-HxIrOy. (h) Nyquist plots of ?-HxIrOy at 98% RH under varying temperatures. (i) Cross-section SEM image and the corresponding elemental mapping of ?-HxIrOy catalyst layer. Reprinted with permission from Ref. [113]. Copyright 2025, Wiley-VCH.

Fig. 8. Future development for 2D electrocatalytic materials.

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Ultrathin two-dimensional electrocatalysts: Structure-property relationships, mechanistic insights, and applications in water electrolysis

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