期刊
CHEMICAL ENGINEERING JOURNAL
卷 445, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136618
关键词
Hydrogen evolution reaction; Strongly coupled 1T-2H MoS2/N-rGO quantum-dot heterostructures; Spatially shaped laser; Controllable modulations; Density functional theory calculations
资金
- Chongqing Natural Science Foundation of China [cstc2021jcyj-cxttX0003]
- National Natural Science Foundation of China (NSFC) [51922005, 52105427]
A controllable strategy for the synthesis of strongly coupled quantum-dot hybrid structures using laser ablation in liquid is presented in this study. The synthesized hybrid structures exhibit enhanced electrochemical hydrogen evolution reaction performance and overcome the limitations of current synthesis methods.
Strongly coupled transition-metal dichalcogenides/carbon hybrids are cost-effective and robust electrocatalysts for hydrogen evolution reaction, and further designing quantum-dot structures of hybrid catalysts often maximizes the accessible active sites and facilitates charge transfer and consequently their catalytic performance. However, the rational design and facile synthesis of such quantum-dot hybrid still remains a central challenge. Herein, an effective and controllable strategy is presented for one-step synthesis of strongly coupled 1T-2H MoS2/N-rGO quantum-dot heterostructures using spatially shaped laser ablation in liquid (LAL). The yield of QDs reaches 75.16 wt%, indicating that the mass production of such QDs is feasible using LAL method. Moreover, both characterizations and density functional theory calculations reveal that the much enhanced electrochemical HER performance arises from the optimized chemical composition, improved conductivity, and strongly coupled structural/electronic features. Correspondingly, the as-formed quantum-dot heterostructures exhibit remarkably low overpotential of 97 mV at 10 mA c(2), a small Tafel slope of 39 mV dec(-1) and high durability, outperformed most previously reported QDs-based electrocatalysts. This versatile strategy overcomes the current limitations of strong-coupled quantum-dot heterostructures materials preparing and offers a synergistic modulation approach for designing highly active HER catalysts viable for practical application.
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