Modulating interfacial charge distribution of single atoms confined in molybdenum phosphosulfide heterostructures for high efficiency hydrogen evolution
Modulating interfacial charge distribution of single atoms confined in molybdenum phosphosulfide heterostructures for high efficiency hydrogen evolution
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DOI：
10.1016/j.cej.2021.128834
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发表时间：
2021-02-11
影响因子：
15.1
通讯作者：
Ma, Haixia
中科院分区：
文献类型：
--
作者：
Li, Jiachen;Zhang, Chi;Ma, Haixia
非均相催化剂中活性中心的界面电荷调节吸附？中间体的脱附。然而，它是具有挑战性的桥梁界面电荷分布和催化活性。本文中，使用简易的恒电流沉积策略将成本有效的钌（Ru）单原子（SA）锚到碳布上的MoS 2/MoP异质结构（CC@MoS2/MoP/Ru SA）中。电化学测试表明，CC@MoS2/MoP/ Ru自组装膜具有良好的上级碱性析氢反应活性，在-10和-100 mA cmgeo？2所示。CC@MoS2/MoP/Ru SA也表现出至少100 h的高稳定性。双途径动力学分析和密度泛函理论（DFT）计算清楚地揭示了MoS 2/MoP和Ru SAs界面之间协同作用和电荷重新分配的重要性，其调节中间体的吸附和解吸。这项工作将协同作用与界面电荷分布相关联，以促进催化活性，作为指导，以获得先进的电催化剂设计的新见解。
The interfacial charge of active centers in heterogeneous catalysts modulates the sorption?desorption of intermediates. However, it is challenging to bridge the interfacial charge distribution and catalytic activity. Herein, a facile galvanostatic deposition strategy is used to anchor cost-effective ruthenium (Ru) single atoms (SAs) into MoS2/MoP heterosturctures on carbon cloth (CC@MoS2/MoP/Ru SAs). Electrochemical test of CC@MoS2/MoP/ Ru SAs reveals superior alkaline hydrogen evolution reaction (HER) activity with low overpotential of 45 and 114 mV at the current of -10 and -100 mA cmgeo?2 , respectively. The CC@MoS2/MoP/Ru SAs also exhibit high stability for at least 100 h. Dual-pathway kinetic analysis and density functional theory (DFT) calculation clearly unravel the importance of synergy and charge redistribution between the interfaces of MoS2/MoP and Ru SAs, which modulate adsorption and desorption of intermediates. This work correlates the synergy in conjunction with interfacial charge distribution to promote catalytic activity, taking as a guide to get new insight into the design of advanced electrocatalysts.