Wei Huifang, Xi Qiaoya, Chen Xi'an, Guo Daying, Ding Feng, Yang Zhi, Wang Shun, Li Juan, Huang Shaoming
Key Laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials Engineering Wenzhou University Wenzhou 325035 P. R. China.
School of Materials and Energy Guangdong University of Technology Guangzhou Guangdong 510006 P. R. China.
Adv Sci (Weinh). 2018 Jan 3;5(3):1700733. doi: 10.1002/advs.201700733. eCollection 2018 Mar.
Molybdenum carbide (MoC) is recognized as an alternative electrocatalyst to noble metal for the hydrogen evolution reaction (HER). Herein, a facile, low cost, and scalable method is provided for the fabrication of MoC-based eletrocatalyst (MoC/G-NCS) by a spray-drying, and followed by annealing. As-prepared MoC/G-NCS electrocatalyst displays that ultrafine MoC nanopartilces are uniformly embedded into graphene wrapping N-doped porous carbon microspheres derived from chitosan. Such designed structure offer several favorable features for hydrogen evolution application: 1) the ultrasmall size of MoC affords a large exposed active sites; 2) graphene-wrapping ensures great electrical conductivity; 3) porous structure increases the electrolyte-electrode contact points and lowers the charge transfer resistance; 4) N-dopant interacts with H better than C atoms and favorably modifies the electronic structures of adjacent Mo and C atoms. As a result, the MoC/G-NCS demonstrates superior HER activity with a very low overpotential of 70 or 66 mV to achieve current density of 10 mA cm, small Tafel slope of 39 or 37 mV dec, respectively, in acidic and alkaline media, and high stability, indicating that it is a great potential candidate as HER electrocatalyst.
碳化钼(MoC)被认为是用于析氢反应(HER)的贵金属替代电催化剂。在此,提供了一种简便、低成本且可扩展的方法,通过喷雾干燥制备基于MoC的电催化剂(MoC/G-NCS),然后进行退火处理。所制备的MoC/G-NCS电催化剂显示出超细的MoC纳米颗粒均匀地嵌入到由壳聚糖衍生的包裹氮掺杂多孔碳微球的石墨烯中。这种设计结构为析氢应用提供了几个有利特性:1)MoC的超小尺寸提供了大量暴露的活性位点;2)石墨烯包裹确保了良好的导电性;3)多孔结构增加了电解质与电极的接触点并降低了电荷转移电阻;4)氮掺杂剂与氢的相互作用优于碳原子,并有利地改变了相邻Mo和C原子的电子结构。结果,MoC/G-NCS在酸性和碱性介质中分别具有70或66 mV的极低过电位以实现10 mA cm的电流密度、39或37 mV dec的小塔菲尔斜率以及优异的HER活性和高稳定性,表明它是HER电催化剂的极具潜力的候选者。