Xiao Zhaohui, Luo Shengdao, Duan Wei, Zhang Xu, Han Shixing, Liu Yipu, Yang Liang, Lin Shiwei
State Key Laboratory of Marine Resource Utilization in South China Sea, School of Materials Science and Engineering, Hainan University, Haikou, China.
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, China.
Front Chem. 2022 Nov 23;10:1064752. doi: 10.3389/fchem.2022.1064752. eCollection 2022.
Producing hydrogen through water electrolysis is one of the most promising green energy storage and conversion technologies for the long-term development of energy-related hydrogen technologies. MoS is a very promising electrocatalyst which may replace precious metal catalysts for the hydrogen evolution reaction (HER). In this work, doughty-electronegative heteroatom defects (halogen atoms such as chlorine, fluorine, and nitrogen) were successfully introduced in MoS by using a large-scale, green, and simple ball milling strategy to alter its electronic structure. The physicochemical properties (morphology, crystallization, chemical composition, and electronic structure) of the doughty-electronegative heteroatom-induced defective MoS (N/Cl-MoS) were identified using SEM, TEM, Raman, XRD, and XPS. Furthermore, compared with bulk pristine MoS, the HER activity of N/Cl-MoS significantly increased from 442 mV to 280 mV at a current of 10 mA cm. Ball milling not only effectively reduced the size of the catalyst material, but also exposed more active sites. More importantly, the introduced doughty-electronegative heteroatom optimized the electronic structure of the catalyst. Therefore, the doughty-electronegative heteroatom induced by mechanical ball milling provides a useful reference for the large-scale production of green, efficient, and low-cost catalyst materials.
通过水电解制氢是能源相关氢技术长期发展中最具前景的绿色储能和转换技术之一。二硫化钼（MoS）是一种非常有前景的电催化剂，可替代用于析氢反应（HER）的贵金属催化剂。在这项工作中，通过大规模、绿色且简单的球磨策略，成功地在二硫化钼中引入了电负性强的杂原子缺陷（如氯、氟和氮等卤素原子），以改变其电子结构。利用扫描电子显微镜（SEM）、透射电子显微镜（TEM）、拉曼光谱、X射线衍射（XRD）和X射线光电子能谱（XPS）对电负性强的杂原子诱导的缺陷二硫化钼（N/Cl-MoS）的物理化学性质（形态、结晶、化学成分和电子结构）进行了鉴定。此外，与块状原始二硫化钼相比，在电流为10 mA cm时，N/Cl-MoS的析氢活性从442 mV显著提高到280 mV。球磨不仅有效地减小了催化剂材料的尺寸，还暴露了更多的活性位点。更重要的是，引入的电负性强的杂原子优化了催化剂的电子结构。因此，机械球磨诱导的电负性强的杂原子为大规模生产绿色、高效和低成本的催化剂材料提供了有用的参考。
