Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada N6A 5B9.
Department of Materials Science and Engineering, McMaster University, Hamilton, Ontario, Canada L8S 4L8.
Nat Commun. 2016 Nov 30;7:13638. doi: 10.1038/ncomms13638.
Platinum-based catalysts have been considered the most effective electrocatalysts for the hydrogen evolution reaction in water splitting. However, platinum utilization in these electrocatalysts is extremely low, as the active sites are only located on the surface of the catalyst particles. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their efficiency by utilizing nearly all platinum atoms. Here we report on a practical synthesis method to produce isolated single platinum atoms and clusters using the atomic layer deposition technique. The single platinum atom catalysts are investigated for the hydrogen evolution reaction, where they exhibit significantly enhanced catalytic activity (up to 37 times) and high stability in comparison with the state-of-the-art commercial platinum/carbon catalysts. The X-ray absorption fine structure and density functional theory analyses indicate that the partially unoccupied density of states of the platinum atoms' 5d orbitals on the nitrogen-doped graphene are responsible for the excellent performance.
基于铂的催化剂被认为是水分解析氢反应中最有效的电催化剂。然而，这些电催化剂中铂的利用率极低，因为活性位点仅位于催化剂颗粒的表面。将催化剂纳米粒子缩小到单原子，通过利用几乎所有的铂原子，极大地提高其效率是非常可取的。在这里，我们报告了一种使用原子层沉积技术生产孤立的单铂原子和团簇的实用合成方法。对单铂原子催化剂进行了析氢反应的研究，结果表明，与最先进的商业铂/碳催化剂相比，它们具有显著增强的催化活性（高达 37 倍）和高稳定性。X 射线吸收精细结构和密度泛函理论分析表明，氮掺杂石墨烯上铂原子 5d 轨道的部分非占据态密度是优异性能的原因。
