State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
State Key Laboratory of Catalysis, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, China.
Nat Commun. 2017 Apr 12;8:14430. doi: 10.1038/ncomms14430.
Hydrogen production through water splitting has been considered as a green, pure and high-efficient technique. As an important half-reaction involved, hydrogen evolution reaction is a complex electrochemical process involving liquid-solid-gas three-phase interface behaviour. Therefore, new concepts and strategies of material design are needed to smooth each pivotal step. Here we report a multiscale structural and electronic control of molybdenum disulfide foam to synergistically promote the hydrogen evolution process. The optimized three-dimensional molybdenum disulfide foam with uniform mesopores, vertically aligned two-dimensional layers and cobalt atoms doping demonstrated a high hydrogen evolution activity and stability. In addition, density functional theory calculations indicate that molybdenum disulfide with moderate cobalt doping content possesses the optimal activity. This study demonstrates the validity of multiscale control in molybdenum disulfide via overall consideration of the mass transport, and the accessibility, quantity and capability of active sites towards electrocatalytic hydrogen evolution, which may also be extended to other energy-related processes.
通过水分解生产氢气被认为是一种绿色、纯净和高效的技术。作为涉及的一个重要半反应，析氢反应是一个涉及固-液-气三相界面行为的复杂电化学过程。因此，需要新的材料设计概念和策略来平滑每个关键步骤。在这里，我们报告了一种通过多尺度结构和电子控制二硫化钼泡沫来协同促进析氢过程的方法。优化的具有均匀介孔、垂直排列的二维层和钴原子掺杂的三维二硫化钼泡沫表现出高的析氢活性和稳定性。此外，密度泛函理论计算表明，具有适中钴掺杂含量的二硫化钼具有最佳的活性。这项研究通过全面考虑质量传输以及活性位点对电催化析氢的可及性、数量和能力，证明了在二硫化钼中进行多尺度控制的有效性，这也可能扩展到其他与能源相关的过程。
