Zheng Yao, Jiao Yan, Li Lu Hua, Xing Tan, Chen Ying, Jaroniec Mietek, Qiao Shi Zhang
School of Chemical Engineering, The University of Adelaide , Adelaide, South Australia 5005, Australia.
ACS Nano. 2014 May 27;8(5):5290-6. doi: 10.1021/nn501434a. Epub 2014 May 1.
Replacement of precious Pt catalyst with cost-effective alternatives would be significantly beneficial for hydrogen production via electrocatalytic hydrogen evolution reaction (HER). All candidates thus far are exclusively metallic catalysts, which suffer inherent corrosion and oxidation susceptibility during acidic proton-exchange membrane electrolysis. Herein, based on theoretical predictions, we designed and synthesized nitrogen (N) and phosphorus (P) dual-doped graphene as a nonmetallic electrocatalyst for sustainable and efficient hydrogen production. The N and P heteroatoms could coactivate the adjacent C atom in the graphene matrix by affecting its valence orbital energy levels to induce a synergistically enhanced reactivity toward HER. As a result, the dual-doped graphene showed higher electrocatalytic HER activity than single-doped ones and comparable performance to some of the traditional metallic catalysts.
用具有成本效益的替代物取代昂贵的铂催化剂，对于通过电催化析氢反应（HER）制氢将具有显著的益处。迄今为止，所有候选物均为纯金属催化剂，在酸性质子交换膜电解过程中，它们存在固有的腐蚀和氧化敏感性问题。在此，基于理论预测，我们设计并合成了氮（N）和磷（P）双掺杂石墨烯，作为一种用于可持续高效制氢的非金属电催化剂。N和P杂原子可通过影响石墨烯基质中相邻C原子的价轨道能级来共同激活该C原子，从而诱导出对HER协同增强的反应活性。结果，双掺杂石墨烯表现出比单掺杂石墨烯更高的电催化HER活性，并且与一些传统金属催化剂具有相当的性能。
