Zhang Huabin, An Pengfei, Zhou Wei, Guan Bu Yuan, Zhang Peng, Dong Juncai, Lou Xiong Wen David
School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China.
Sci Adv. 2018 Jan 19;4(1):eaao6657. doi: 10.1126/sciadv.aao6657. eCollection 2018 Jan.
Constructing atomically dispersed platinum (Pt) electrocatalysts is essential to build high-performance and cost-effective electrochemical water-splitting systems. We present a novel strategy to realize the traction and stabilization of isolated Pt atoms in the nitrogen-containing porous carbon matrix (Pt@PCM). In comparison with the commercial Pt/C catalyst (20 weight %), the as-prepared Pt@PCM catalyst exhibits significantly boosted mass activity (up to 25 times) for hydrogen evolution reaction. Results of extended x-ray absorption fine structure investigation and density functional theory calculation suggest that the active sites are associated with the lattice-confined Pt centers and the activated carbon (C)/nitrogen (N) atoms at the adjacency of the isolated Pt centers. This strategy may provide insights into constructing highly efficient single-atom catalysts for different energy-related applications.
构建原子分散的铂（Pt）电催化剂对于构建高性能且经济高效的电化学水分解系统至关重要。我们提出了一种新颖的策略，以实现孤立的Pt原子在含氮多孔碳基质（Pt@PCM）中的牵引和稳定。与商业Pt/C催化剂（20重量％）相比，所制备的Pt@PCM催化剂在析氢反应中表现出显著提高的质量活性（高达25倍）。扩展X射线吸收精细结构研究和密度泛函理论计算结果表明，活性位点与晶格限制的Pt中心以及孤立Pt中心邻位的活性炭（C）/氮（N）原子相关。该策略可为构建用于不同能量相关应用的高效单原子催化剂提供见解。
