Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, School of Chemistry and Chemical Engineering, Liaocheng University , Liaocheng 252059, China.
School of Chemical Engineering, The University of Adelaide , Adelaide, South Australia 5005, Australia.
ACS Nano. 2017 Jul 25;11(7):7293-7300. doi: 10.1021/acsnano.7b03290. Epub 2017 Jun 29.
Dual heteroatom-doped carbon materials are efficient electrocatalysts via a synergistic effect. With nitrogen as the primary dopant, boron, sulfur, and phosphorus can be used as secondary elements for co-doped carbons. However, evaluation and analysis of the promotional effect of B, P, and S to N-doped carbons has not been widely researched. Here we report a robust platform that is constructed through polydopamine to prepare N,B-, N,P-, and N,S-co-doped carbon nanosheets, characterized by similar N species content and efficient B, P, and S doping. Systematic investigation reveals S to have the greatest promotional effect in hydrogen evolution reactions (HER) followed by P and that B decreases the activity of N-doped carbons. Experimental and theoretical analyses show the secondary heteroatom promotional effect is impacted by the intrinsic structures and extrinsic surface areas of both materials, i.e., electronic structures exclusively determine the catalytic activity of active sites, while large surface areas optimize apparent HER performance.
双原子掺杂碳材料通过协同效应成为高效电催化剂。以氮作为主要掺杂元素，硼、硫和磷可以作为共掺杂碳的次要元素。然而，B、P 和 S 对 N 掺杂碳的促进作用的评价和分析尚未得到广泛研究。在这里，我们报告了一种通过聚多巴胺构建的强大平台，用于制备 N，B-、N，P-和 N，S-共掺杂碳纳米片，其具有相似的 N 物种含量和高效的 B、P 和 S 掺杂。系统研究表明，S 在析氢反应（HER）中具有最大的促进作用，其次是 P，而 B 则降低了 N 掺杂碳的活性。实验和理论分析表明，二次杂原子的促进作用受到材料内在结构和外比表面积的影响，即电子结构仅决定活性位的催化活性，而大的比表面积则优化了明显的 HER 性能。
