High-Density Defects Activating Fe-Doped Molybdenum Sulfide@NDoped Carbon Heterostructures for Efficient Electrochemical Hydrogen Evolution
High-Density Defects Activating Fe-Doped Molybdenum Sulfide@NDoped Carbon Heterostructures for Efficient Electrochemical Hydrogen Evolution
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高密度缺陷激活掺铁硫化钼@N掺杂碳异质结构以实现高效电化学析氢
DOI：
10.1021/acssuschemeng.1c05538
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发表时间：
2021
期刊：
影响因子：
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通讯作者：
谢海娇
中科院分区：
文献类型：
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作者：
夏晓红;赵改云;闫琦;王彪;王秋风;谢海娇
掺杂引起的空位缺陷有利于优化区域电子结构和增加暴露的活性位点，对提高析氢反应（HER）效率至关重要。在此，我们构建了氮掺杂碳封装的铁掺杂硫化钼（FeMoSN@NC），其具有超薄边缘卷曲层结构。以普鲁士蓝纳米笼为前驱体实现Fe掺杂，在超薄层组装微球的形成中起着至关重要的作用。实验测试和理论计算表明，Fe掺杂不仅可以扩展MoS2(∼11 Å)的层间以获得超薄层，而且可以嵌入MoS2的面内位置形成高密度掺杂和空位缺陷。 Fe掺杂引起的区域活性位点的调节可以增强催化剂的固有催化活性，包括更多的HER活性位点、适当的氢吸附吉布斯自由能（Fe1Mo-VMo,S的-0.11 eV）和较低的载流子转移电阻（9 Ω）。 FeMoSN@NC 作为 HER 电催化剂表现出高效的活性，塔菲尔斜率为 67 mV dec-1，电流密度为 -100 mA mg-1 时的过电势为 150 mV。上述见解为高效硫化钼电催化剂提供了新的过渡金属掺杂策略，具有优化的活性位点和增加的电化学活性面积。
Vacancy defects caused by doping are beneficial to optimizing the regional electronic structure and increasing exposed active sites, and it is vital to improve the efficiency of hydrogen evolution reaction (HER). Herein, we constructed the Fe-doped molybdenum sulfide encapsulated with N-doped carbon (FeMoSN@NC), which with ultrathin edge-curled layer structure. Fe-doping realized with Prussian blue nanocages as the precursors, which plays a crucial role in the formation of ultrathin layer assembled microspheres. Experimental tests and theoretical calculations show that the Fe-doping can not only expand the interlayer of MoS2(∼11 Å) to obtain ultrathin layers but also embed into the in-plane location of MoS2to form high-density doping and vacancy defects. The regulation of regional active sites caused by Fe-doping can enhance the intrinsic catalytic activity of catalyst, including more active sites for HER, appropriate Gibbs free energy of hydrogen adsorption (−0.11 eV of Fe1Mo-VMo,S), and low resistance for carrier transfer (9 Ω). FeMoSN@NC as the HER electrocatalyst exhibits efficient activity with a Tafel slope of 67 mV dec–1and an overpotential of 150 mV at the current density of −100 mA mg–1. The above insights provide new transition metal doping strategy for efficient molybdenum sulfide electrocatalysts with optimized active sites and increased electrochemical active area.