Wang Zhenguo, Xu Wangqiong, Yu Ke, Feng Yu, Zhu Ziqiang
Key Laboratory of Polar Materials and Devices (MOE), Department of Electronics, East China Normal University, Shanghai 200241, China.
Nanoscale. 2020 Mar 12;12(10):6176-6187. doi: 10.1039/d0nr00207k.
A novel electrocatalytic material VS2@V2C was proposed for the first time and successfully prepared by a one-step hydrothermal method. T-VS2 nanosheets were uniformly and vertically embedded on the V2C (MXene) matrix with a fewer layer structure. Owing to the fast charge transfer process at the interface of the two-phase structure and good conductivity, the composite material showed a lower hydrogen evolution overpotential and a very low Tafel slope in highly alkaline and highly acidic electrolytes (164 mV and 47.6 mV dec-1 in 1.0 M KOH; 138 mV and 37.9 mV dec-1 in 0.5 M H2SO4) under a current density of 20 mV cm-2. More importantly, high-efficiency and stable electrolysis of seawater was achieved at a current density greater than 100 mA cm-2, and the catalytic performance was significantly better than that of platinum-based alloys. First-principles calculations mechanically confirmed that VS2@V2C had higher carrier mobility and lower free energy of hydrogen adsorption. The VS2 nanosheets that grew outwards could provide support to avoid agglomeration on the catalyst surface and the edge sulfur sites of VS2 could promote the binding of adsorbed hydrogen atoms and the desorption of hydrogen molecules. Our work is expected to provide a valuable reference for the design and synthesis of the structure of industrial catalysts for hydrogen production from seawater in the future.
首次提出了一种新型电催化材料VS2@V2C,并通过一步水热法成功制备。T-VS2纳米片均匀且垂直地嵌入具有较少层结构的V2C(MXene)基体上。由于两相结构界面处快速的电荷转移过程和良好的导电性,该复合材料在高碱性和高酸性电解质中(在1.0 M KOH中为164 mV和47.6 mV dec-1;在0.5 M H2SO4中为138 mV和37.9 mV dec-1),在20 mV cm-2的电流密度下表现出较低的析氢过电位和非常低的塔菲尔斜率。更重要的是,在大于100 mA cm-2的电流密度下实现了海水的高效稳定电解,其催化性能明显优于铂基合金。第一性原理计算从机理上证实了VS2@V2C具有更高的载流子迁移率和更低的氢吸附自由能。向外生长的VS2纳米片可以提供支撑以避免在催化剂表面团聚,并且VS2的边缘硫位点可以促进吸附氢原子的结合和氢分子的脱附。我们的工作有望为未来海水制氢工业催化剂结构的设计与合成提供有价值的参考。