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Vol. 15 (2023)

Graphene Quantum Dot-Mediated Atom-Layer Semiconductor Electrocatalyst for Hydrogen Evolution

https://doi.org/10.1007/s40820-023-01182-7
Bingjie Hu
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, BaoShan District, Shanghai 200444, People’s Republic of China
Kai Huang
State Key Laboratory of Chemical Engineering, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Bijun Tang
School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore
Zhendong Lei
School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore
Zeming Wang
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, BaoShan District, Shanghai 200444, People’s Republic of China
Huazhang Guo
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, BaoShan District, Shanghai 200444, People’s Republic of China
Cheng Lian
State Key Laboratory of Chemical Engineering, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, People’s Republic of China
Zheng Liu
School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore
http://orcid.org/0000-0002-8825-7198
Liang Wang
Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, BaoShan District, Shanghai 200444, People’s Republic of China
http://orcid.org/0000-0002-3771-4627

Corresponding Author: Liang Wang

wangl@shu.edu.cn

Nano-Micro Letters, Vol. 15 (2023), Article Number: 217

Abstract

The hydrogen evolution reaction performance of semiconducting 2H-phase molybdenum disulfide (2H-MoS2) presents a significant hurdle in realizing its full potential applications. Here, we utilize theoretical calculations to predict possible functionalized graphene quantum dots (GQDs), which can enhance HER activity of bulk MoS2. Subsequently, we design a functionalized GQD-induced in-situ bottom-up strategy to fabricate near atom-layer 2H-MoS2 nanosheets mediated with GQDs (ALQD) by modulating the concentration of electron withdrawing/donating functional groups. Experimental results reveal that the introduction of a series of functionalized GQDs during the synthesis of ALQD plays a crucial role. Notably, the higher the concentration and strength of electron-withdrawing functional groups on GQDs, the thinner and more active the resulting ALQD are. Remarkably, the synthesized near atom-layer ALQD-SO3 demonstrate significantly improved HER performance. Our GQD-induced strategy provides a simple and efficient approach for expanding the catalytic application of MoS2. Furthermore, it holds substantial potential for developing nanosheets in other transition-metal dichalcogenide materials.


Highlights:
1 The functional groups on graphene quantum dots (GQDs) for boosting the formation of MoS2 nanosheets via theoretical calculations were predicted.
2 Near atom-layer-QD@SO3 with about 2 nm were synthesized using a functionalized GQD-induced in-situ bottom-up approach.
3 Mechanistic insight on the role of functionalized GQDs was elaborated, namely, electron-withdrawing group functionalized GQDs facilitate the formation of nanosheet architectures of MoS2 compared to electron-donating group.

Keywords

Graphene quantum dots MoS2 nanosheets Atom-layer Semiconductor electrocatalysts Hydrogen evolution reaction
Hu, Bingjie, Kai Huang, Bijun Tang, Zhendong Lei, Zeming Wang, Huazhang Guo, Cheng Lian, Zheng Liu, and Liang Wang. 2023. “Graphene Quantum Dot-Mediated Atom-Layer Semiconductor Electrocatalyst for Hydrogen Evolution”. Nano-Micro Letters 15 (September):217. https://doi.org/10.1007/s40820-023-01182-7.
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