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Research Article | Online first | Published: 19 April 2024

Defect-modulated and heteroatom-functionalized Ti3−xC2Ty MXene 3D nanocavities induce growth of MoSe2 nanoflakes toward electrocatalytic hydrogen evolution in all pH electrolytes

Show Author's Information Ming Du1,  Xianzhi Yang2,  Jian Zhang1,3( ),  Wei Chen4,  Huajie Huang5,  Xinbao Zhu6( ),  Xing’ao Li1,3( )
State Key Laboratory for Organic Electronics and Information Displays and Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Centre for Advanced Materials (SICAM), Nanjing University of Posts and Telecommunications (NJUPT), Nanjing 210023, China
College of Electronic and Optical Engineering and College of Flexible Electronics Nanjing University of Posts and Telecommunications (NJUPT), Nanjing 210023, China
New Energy Technology Engineering Lab of Jiangsu Province, College of Science, Nanjing University of Posts and Telecommunications (NJUPT), Nanjing 210023, China
College of Pharmaceutical and Chemical Engineering, Taizhou University, Jiaojiang 318000, China
College of Mechanics and Materials, Hohai University, Nanjing 210098, China
College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China
Keywords:
interfacial interaction, electrocatalytic H2 evolution, MoSe2 nanoflake, self-adapting Ti vacancy defect, heteroatom-functionalized, three-dimensional (3D) MXene nanocavity
Topics:
Nanostructured materials
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Du M, Yang X, Zhang J, et al. Defect-modulated and heteroatom-functionalized Ti3−xC2Ty MXene 3D nanocavities induce growth of MoSe2 nanoflakes toward electrocatalytic hydrogen evolution in all pH electrolytes. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6645-y
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Abstract Full text Electronic supplementary material About this article

Reducing kinetic energy barriers and developing accessible active sites are critical to deliver high hydrogen evolution reaction (HER) efficiency. In this paper, we synthesized defect-modulated and heteroatom (boron)-functionalized three-dimensional (3D) bowl-shaped Ti3−xC2Ty MXene (B-TCT) nanocavities coupled with the vertical growth of MoSe2 nanoflakes. The B-TCT@MoSe2 nanohybrids catalyst delivers the overpotentials of 49.9, 52.7, and 67.8 mV to reach a HER current density of 10 mA·cm−2 under acidic, alkaline, and neutral conditions, respectively. Such outstanding HER activity is predominantly attributed to the heteroatom functionalization, self-adapting Ti vacancy (VTi) defect modulation, and spatial configuration design in the 3D B-TCT nanocavity, which synergistically regulate the electronic structure, activate the basal plane/edge unsaturated sites, and reduce the reaction energy barrier. Experimental and theoretical calculations demonstrate that strong heterogeneous interfacial bonding interactions between B-TCT and MoSe2 can dramatically reduce the free energy of hydrogen adsorption and facilitate efficient interfacial charge migration, thus essentially improving the HER kinetics. We used this 3D porous nanohybrid system assembled by defect-rich lamellar structures to elucidate the advantageous synergistic effects of multiple mechanisms among defect structure, heteroatom functionalization, and interfacial coupling, which provided important insights for the development of efficient hybrid-type catalysts.


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About this article

Defect-modulated and heteroatom-functionalized Ti3−xC2Ty MXene 3D nanocavities induce growth of MoSe2 nanoflakes toward electrocatalytic hydrogen evolution in all pH electrolytes

Show Author's information Ming Du1, Xianzhi Yang2, Jian Zhang1,3( ), Wei Chen4, Huajie Huang5, Xinbao Zhu6( ), Xing’ao Li1,3( )
State Key Laboratory for Organic Electronics and Information Displays and Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Centre for Advanced Materials (SICAM), Nanjing University of Posts and Telecommunications (NJUPT), Nanjing 210023, China
College of Electronic and Optical Engineering and College of Flexible Electronics Nanjing University of Posts and Telecommunications (NJUPT), Nanjing 210023, China
New Energy Technology Engineering Lab of Jiangsu Province, College of Science, Nanjing University of Posts and Telecommunications (NJUPT), Nanjing 210023, China
College of Pharmaceutical and Chemical Engineering, Taizhou University, Jiaojiang 318000, China
College of Mechanics and Materials, Hohai University, Nanjing 210098, China
College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, China

Abstract

Reducing kinetic energy barriers and developing accessible active sites are critical to deliver high hydrogen evolution reaction (HER) efficiency. In this paper, we synthesized defect-modulated and heteroatom (boron)-functionalized three-dimensional (3D) bowl-shaped Ti3−xC2Ty MXene (B-TCT) nanocavities coupled with the vertical growth of MoSe2 nanoflakes. The B-TCT@MoSe2 nanohybrids catalyst delivers the overpotentials of 49.9, 52.7, and 67.8 mV to reach a HER current density of 10 mA·cm−2 under acidic, alkaline, and neutral conditions, respectively. Such outstanding HER activity is predominantly attributed to the heteroatom functionalization, self-adapting Ti vacancy (VTi) defect modulation, and spatial configuration design in the 3D B-TCT nanocavity, which synergistically regulate the electronic structure, activate the basal plane/edge unsaturated sites, and reduce the reaction energy barrier. Experimental and theoretical calculations demonstrate that strong heterogeneous interfacial bonding interactions between B-TCT and MoSe2 can dramatically reduce the free energy of hydrogen adsorption and facilitate efficient interfacial charge migration, thus essentially improving the HER kinetics. We used this 3D porous nanohybrid system assembled by defect-rich lamellar structures to elucidate the advantageous synergistic effects of multiple mechanisms among defect structure, heteroatom functionalization, and interfacial coupling, which provided important insights for the development of efficient hybrid-type catalysts.

Keywords: interfacial interaction, electrocatalytic H2 evolution, MoSe2 nanoflake, self-adapting Ti vacancy defect, heteroatom-functionalized, three-dimensional (3D) MXene nanocavity

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Acknowledgements

Publication history

Received: 23 January 2024
Revised: 05 March 2024
Accepted: 21 March 2024
Published: 19 April 2024

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© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

This study was jointly supported by the National Natural Science Foundation of China (Nos. 52072182 and 51872145), Natural Science Foundation of Jiangsu Province (No. BK20211278), the China Postdoctoral Science Foundation (Nos. 2019M650120 and 2020M671554), the National Synergetic Innovation Center for Advanced Materials (SICAM), and Postgraduate Research Practice Innovation Program of Jiangsu Province (No. KYCX22_0977).

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