Song Xiancheng, Li Bin, Peng Wenchao, Wang Chi, Li Kai, Zhu Yuanzhi, Mei Yi
Faculty of Chemical Engineering, Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials, Kunming University of Science and Technology, Kunming 650500, Yunnan, China.
Nanoscale. 2021 Mar 21;13(11):5892-5900. doi: 10.1039/d0nr09133b. Epub 2021 Mar 16.
The electrocatalytic hydrogen evolution reaction (HER) is a green chemistry route for sustainable energy production. Compared to 2H-phase molybdenum disulfide (MoS), the 1T-phase MoS (1T-MoS) has higher theoretical activity and faster charge transfer kinetics, but the HER performance of 1T-MoS is commonly hindered by limited active edge/defect as well as poor structural stability. Herein, we synthesize a well-defined 2D vdW heterostructure composed of Pd doped 1T-MoS and black phosphorus (BP) nanosheets via electrostatic self-assembly. The spontaneous Pd doping under mild reaction conditions could introduce catalytically active sulfur vacancies in MoS without triggering a wide range of 1T to 2H phase transformation. The hetero-interfacial charge transfer from BP to Pd-1T-MoS can effectively improve the intrinsic activity of Pd-1T-MoS with a relatively low S vacancy concentration and simultaneously stabilize the 1T-phase structure. Due to the wide-range light absorption of BP nanosheets and the high carrier mobilities of 2D materials, the HER activity of the obtained Pd-1T-MoS/BP could be further enhanced under ≥420 nm visible light illumination.
电催化析氢反应（HER）是实现可持续能源生产的绿色化学途径。与2H相二硫化钼（MoS）相比，1T相MoS（1T-MoS）具有更高的理论活性和更快的电荷转移动力学，但其HER性能通常受到活性边缘/缺陷有限以及结构稳定性差的阻碍。在此，我们通过静电自组装合成了一种由钯掺杂的1T-MoS和黑磷（BP）纳米片组成的明确二维范德华异质结构。在温和反应条件下自发进行的钯掺杂可在MoS中引入催化活性硫空位，而不会引发大范围的1T相向2H相转变。从BP到Pd-1T-MoS的异质界面电荷转移能够在相对较低的硫空位浓度下有效提高Pd-1T-MoS的本征活性，同时稳定1T相结构。由于BP纳米片的宽范围光吸收以及二维材料的高载流子迁移率，在≥420 nm可见光照射下，所制备的Pd-1T-MoS/BP的HER活性可进一步增强。
