Strategies for local electronic structure engineering of two-dimensional electrocatalysts

doi:10.1016/S1872-2067(23)64423-7

Chinese Journal of Catalysis ›› 2023, Vol. 48: 1-14.DOI: 10.1016/S1872-2067(23)64423-7

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Strategies for local electronic structure engineering of two-dimensional electrocatalysts

Cheng-Feng Du^a, Erhai Hu^b^,^c, Hong Yu^a^,^*(), Qingyu Yan^b^,^c^,^*()

^aState Key Laboratory of Solidification Processing, Center of Advanced Lubrication and Seal Materials, Northwestern Polytechnical University, Xi’an 710072, Shaanxi, China
^bEnergy Research Institute, Nanyang Technological University, Singapore 637141, Singapore
^cSchool of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore

Received:2022-12-29 Accepted:2023-03-01 Online:2023-05-18 Published:2023-04-20
Contact: * E-mail: yh@nwpu.edu.cn (H. Yu), alexyan@ntu.edu.sg (Q. Yan).
About author:Hong Yu (Northwestern Polytechnical University) is currently an associate professor in the School of Materials Science and Engineering at Northwestern Polytechnical University, China. She received her B.S. and Ph.D. degrees in materials science and engineering from Nanyang Technological University (Singapore) in 2011 and 2016, respectively. She continued her research as a postdoctoral research fellow in Nanyang Technological University prior to joining Northwestern Polytechnical University in 2017. Her research focuses on the design and synthesis of advanced functional materials for energy conversion and storage.
Qingyu Yan (Nanyang Technology University) is currently a professor in School of Materials Science and Engineering in Nanyang Technology University, Singapore. He obtained his BS in Materials Science and Engineering, Nanjing University (China). He finished his Ph.D. from Materials Science and Engineering Department of State University of New York at Stony Brook. After that, He joined the Materials Science and Engineering Department of Rensselaer Polytechnic Institute as a postdoctoral research associate. He joined School of Materials Science and Engineering of Nanyang Technology University as an assistant professor in early 2008 and became a full Professor in 2018. He is currently the Chair of the Electrochemical Society, Singapore Section. He is a fellow of Royal Society of Chemistry Since 2018. He has published more than 300 papers on the research area of energy conversion and storage.
Supported by:
National Natural Science Foundation of China(51901189);National Natural Science Foundation of China(52272091);Shaanxi Provincial Key R&D Program(2021KWZ-17)

Abstract

Abstract:

Electrocatalytic processes have garnered increased attention for energy conversion and mass production because of their high efficiency and selectivity. In particular, electrocatalysts play a critical role in catalytic performance. Two-dimensional (2D) materials, which feature a large surface area with abundant active sites and tunable physicochemical properties, have been regarded as one of the most important candidates for future electrocatalysis. However, further research efforts are required to specifically optimize their catalytic performance to realize their commercialization. In this account, strategies for regulating the local electronic structures of 2D electrocatalysts, including heteroatom doping, single-atom loading, heterojunction formation, vacancy engineering, and strain engineering, are briefly summarized. Furthermore, the relationship between these strategies and the electrocatalytic performance of the developed materials is discussed. Finally, an outlook of the 2D electrocatalysts is provided.

Key words: Two-dimensional material, Electrocatalysis, Electronic structure, Active site, Heterogeneous

Cheng-Feng Du, Erhai Hu, Hong Yu, Qingyu Yan. Strategies for local electronic structure engineering of two-dimensional electrocatalysts[J]. Chinese Journal of Catalysis, 2023, 48: 1-14.

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Figures/Tables 8

Fig. 1. (a) Schematic illustration of electronic coupling between Ni, Fe, and V atoms in Ni3Fe, Ni3V, and Ni3Fe0.5V0.5. Reprinted with permission from Ref. [72]. Copyright 2018, Springer Nature Limited. (b) Schematic illustration of multimetal oxide nanoplates and the free-energy profiles for OER at U = 1.23 V. Reprinted with permission from Ref. [74]. Copyright 2020, American Chemical Society.

Fig. 2. (a) Optimized structures of NiPS3 and Se-doped NiPS3 models for OH*, O*, and OOH* deposition. Reprinted with permission from Ref. [85]. Copyright 2021, John Wiley and Sons. (b) Optimized structures of H-adsorbed Mo2C, Co-Mo2C, Mo(V)-Mo2C, and Co-Mo(V)-Mo2C slab models (left), and charge density distributions of Co-Mo2C and Co-Mo(V)-Mo2C (right). Reprinted with permission from Ref. [92]. Copyright 2020, John Wiley and Sons.

Fig. 3. (a) Contour maps of the electron localization function for 2H/1T-Ru-MoS2-Sv. (b) 2D maps of the electron density difference for SA Ru doping and S vacancy on the 2H/1T MoS2. Reprinted with permission from Ref. [108]. Copyright 2019, John Wiley and Sons. XANES spectra at the Ni K-edge (c) and k2-weighted Fourier transforms (d) of the Ni K-edge EXAFS spectra of Ni SACs/Ti3C2Tx, Ni foil, and NiO, and EXAFS fitting results for Ni SACs/Ti3C2Tx. (e) Wavelet-transformed Ni K-edge EXAFS spectra of Ni SACs/Ti3C2Tx, Ni foil, and NiO. Reprinted with permission from Ref. [115]. Copyright 2022, John Wiley and Sons.

Fig. 4. (a) Atomic charges of the transition metals embedded in screened-doped Mo2TiC2Tx. Reprinted with permission from Ref. [103]. Copyright 2019, John Wiley and Sons. (b) Calculated projected density of states (PDOS) of SA Ru-Mo2CO2, Mo2CO2, and Ru (001) with aligned Fermi levels. Mass-normalized NH3 yield rates of SA Ru-doped Mo2CTx (c) and Faradaic efficiencies (d) of the SA Ru-doped Mo2CTx at each applied potential. Reprinted with permission from Ref. [102]. Copyright 2020, John Wiley and Sons.

Fig. 5. (a) Side-views of the differential charge densities of MoS2/graphene (G), LDH/G, and MoS2/LDH bilayer structures with an isosurface value of 0.003 e ??3. Reprinted with permission from Ref. [121]. Copyright 2019, American Chemical Society. (b) ΔGH* calculated at the equilibrium potential (U = 0 V) for NiPS3/Ni2P, Ni2P (001), Ni2P (110), and NiPS3 (110); the insets show the corresponding density functional theory-optimized configurations of H* adsorption. (c) Distribution of the charge density difference at the NiPS3/Ni2P interface, where the red and green regions represent electron accumulation (Δρ = +0.01 e × Bohr?3) and electron depletion (Δρ = ?0.01 e × Bohr?3), respectively. Reprinted with permission from Ref. [124]. Copyright 2019, American Chemical Society.

Fig. 6. (a) d-band centers for CoC2O4, CoC2O4@MXene, and R-CoC2O4@MXene. (b) Differential charge density of R-CoC2O4@MXene (the yellow zone represents charge accumulation, while the blue zone represents charge dispersion). Reprinted with permission from Ref. [129]. Copyright 2022, Springer Nature Limited. (c) Electrostatic potential distribution along the z-axis of the heterojunction of the MoNi4/Mo2TiC2O2 monolayer and (d) differential charge density diagram of the interfacial region. Reprinted with permission from Ref. [131]. Copyright 2022, John Wiley and Sons.

Fig. 7. (a) Structure and density of states (DOS) of the S vacancy (VS), single H-adsorbed VS (H-VS), and double H-adsorbed VS (2H-VS). The total DOS and partial DOS projected on the three nearest neighbor Mo atoms (MoNN) around the VS are shown. Possible charge states q for each defect are also indicated. Reprinted with permission from Ref. [134]. Copyright 2018, American Chemical Society. (b) Relaxed structures after molecular water adsorption onto pristine and defective NiPS3 samples, and dissociative water adsorption to defective NiPS3. Electron density accumulation (or depletion) is shown in red (or blue). Green, violet, orange, red, and light-blue spheres represent Ni, P, S, O, and H atoms, respectively. Reprinted with permission from Ref. [135]. Copyright 2021, John Wiley and Sons.

Fig. 8. (a) Schematic of S vacancy generation in an MoS2 model using different strain conditions. (b) Illustration of Mo adsorption sites with different coordination structures. (c) Calculated free-energy diagram of HER for a pristine MoS2 model under 2%, 4%, and 5% uniaxial/biaxial strain conditions. Reprinted with permission from Ref. [149]. Copyright 2022, John Wiley and Sons.

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Strategies for local electronic structure engineering of two-dimensional electrocatalysts

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