期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 2, 页码 2908-2917出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c21421
关键词
InSe nanosheets; Au nanoparticles; HER; heterojunction; metal-induced
资金
- Scientific Research Fund of Hunan Provincial Education Department [21A0080, 21B0128]
- Program for Changjiang Scholars and Innovative Research Team in University [IRT_17R91]
- Postgraduate Scientific Research Innovation Project of Hunan Province [CX20200560]
- National Natural Science Foundation of China [11874316]
- Hunan Key Laboratory of Two-Dimensional Materials [2018TP1010]
- Guangdong Innovation Platform of Translational Research for Cerebrovascular Diseases
- Guangdong Medical Science and Technology Research Funds [A2019417]
- Key Project of Department of Education of Guangdong Province [2018KCXTD026]
- China Postdoctoral Science Foundation [2020TQ0204, 2020M682904]
This study demonstrates the enhanced hydrogen evolution reaction performance of InSe nanosheets by modifying them with Au nanoparticles. Experimental results show that the modified nanosheets exhibit reduced overpotential and Tafel slope compared to the unmodified ones. First-principles calculations reveal that the modification improves the conductivity of InSe through the injection of free electrons from the Au particles.
Electrocatalytic water splitting for hydrogen production is an efficient, clean, and sustainable strategy to solve energy and environmental problems. As the important alternative materials for noble metals (Pt, Ir, etc.), two-dimensional (2D) materials have been widely applied for electrocatalysis, although the practical performance is restricted by low carrier mobility and slow reaction kinetics. Here, we adopt the strategy of Au nanoparticle modification to achieve the enhanced hydrogen evolution reaction (HER) performance of InSe nanosheets. Experimental results prove that the HER performance of InSe nanosheets is significantly enhanced under the modification of Au nanoparticles, and the overpotential (392 mV) and Tafel slope (59 mV/dec) are significantly reduced compared to sole InSe nanosheets (580 mV and 148.2 mV/dec). First-principles calculations have found that the InSe/Au system exhibits metallicity because the free electrons provided by the Au particles are injected into the InSe, thereby improving its conductivity. The difference charge density and localized charge density of InSe/Au show that Au nanoparticle loading can induce the formation of Au-Se electron-transfer channels with electrovalent bond characteristics, which effectively promotes the charge transfer. Meanwhile, the standard free-energy calculation of the HER process shows that the InSe/Au heterojunction has a H* adsorption/desorption Gibbs free energy [(vertical bar Delta G(H)*vertical bar) = 0.59 eV] closer to the optimal value. This study reveals the theoretical mechanism of metal modification to improve the performance of electrocatalytic HER and is expected to motivate the development of a new strategy for enhancing the catalytic activity of 2D semiconductor materials.
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