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离子液体辅助合成纳米级 (MoS)(SnO) 负载在还原氧化石墨烯上用于电催化析氢反应。

Ionic Liquid-Assisted Synthesis of Nanoscale (MoS)(SnO) on Reduced Graphene Oxide for the Electrocatalytic Hydrogen Evolution Reaction.

机构信息

Department of Chemistry, University of Missouri , Columbia, Missouri 65211, United States.

Department of Mechanical & Aerospace Engineering, University of Missouri , Columbia, Missouri 65211, United States.

出版信息

ACS Appl Mater Interfaces. 2017 Mar 8;9(9):8065-8074. doi: 10.1021/acsami.6b13578. Epub 2017 Feb 21.

DOI:10.1021/acsami.6b13578
PMID:28187262
Abstract

Layered transition metal dichalcogenides (TMDs) have attracted increased attention due to their enhanced hydrogen evolution reaction (HER) performance. More specifically, ternary TMD nanohybrids, such as MoSSe or bimetallic sulfides, have arisen as promising electrocatalysts compared to MoS and MoSe due to their electronic, morphologic, and size tunabilities. Herein, we report the successful synthesis of few-layered MoS/rGO, SnS/rGO, and (MoS)(SnO)/rGO nanohybrids anchored on reduced graphene oxide (rGO) through a facile hydrothermal reaction in the presence of ionic liquids as stabilizing, delayering agents. Spectroscopic and microscopic techniques (electron microscopy, X-ray diffraction, Raman spectroscopy, neutron activation analysis, and UV-vis spectrophotometry) are used to validate the hierarchical properties, phase identity, and the smooth compositional tunability of the (MoS)(SnO)/rGO nanohybrids. Linear sweep voltammetry measurements reveal that incorporation of Sn into the ternary nanohybrids (as a discrete SnO phase) greatly reduces the overpotential by 90-130 mV relative to the MoS electrocatalyst. Significantly, the (MoS)(SnO)/rGO nanohybrid displays superior catalytic performance over MoS alone, exhibiting a low overpotential (η) of 263 ± 5 mV and a small Tafel slope of 50.8 mV dec. The hybrid catalyst shows high stability for the HER in acidic solutions, with negligible activity loss after 1000 cycles. The hierarchical structures and large surface areas possessing exposed, active edge sites make few-layered (MoS)(SnO)/rGO nanohybrids promising nonprecious metal electrocatalysts for the HER.

摘要

层状过渡金属二硫属化物 (TMD) 因其增强的析氢反应 (HER) 性能而受到越来越多的关注。更具体地说,与 MoS 和 MoSe 相比,三元 TMD 纳米杂化物,如 MoSSe 或双金属硫化物,由于其电子、形态和尺寸可调性,作为有前途的电催化剂而出现。在此,我们通过在离子液体存在下的简便水热反应成功合成了少层 MoS/rGO、SnS/rGO 和 (MoS)(SnO)/rGO 纳米杂化物,这些杂化物锚定在还原氧化石墨烯 (rGO) 上。光谱和显微镜技术(电子显微镜、X 射线衍射、拉曼光谱、中子活化分析和紫外可见分光光度法)用于验证分级性质、相一致性和 (MoS)(SnO)/rGO 纳米杂化物的平滑组成可调性。线性扫描伏安法测量表明,将 Sn 掺入三元纳米杂化物(作为离散的 SnO 相)可将过电位降低 90-130 mV,相对于 MoS 电催化剂。重要的是,(MoS)(SnO)/rGO 纳米杂化物在 MoS 单独存在的情况下表现出优异的催化性能,表现出低过电位(η)为 263 ± 5 mV 和小的塔菲尔斜率为 50.8 mV dec。该混合催化剂在酸性溶液中表现出高 HER 稳定性,在 1000 次循环后活性损失可忽略不计。分层结构和大表面积具有暴露的、活性边缘位点,使少层 (MoS)(SnO)/rGO 纳米杂化物成为 HER 的有前途的非贵金属电催化剂。

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