Zhi Xing, Jiao Yan, Zheng Yao, Qiao Shi-Zhang
School of Chemical Engineering, The University of Adelaide, Adelaide, South Australia, 5005, Australia.
Small. 2019 Mar;15(10):e1804224. doi: 10.1002/smll.201804224. Epub 2019 Feb 4.
Effective electrocatalysts are required for the CO reduction reaction (CRR), while the factors that can impact their catalytic activity are yet to be discovered. In this article, graphitic carbon nitride (g-C N ) is used to investigate the feasibility of regulating its CRR catalytic performance by interfacial electron transfer. A series of g-C N /graphene with and without heteroatom doping (C N /XG, XG = BG, NG, OG, PG, G) is comprehensively evaluated for CRR through computational methods. Variable adsorption energetics and electronic structures are observed among different doping cases, demonstrating that a higher catalytic activity originates from more interfacial electron transfer. An activity trend is obtained to show the best catalytic performance of CRR to methane on C N /XG with an overpotential of 0.45 V (i.e., -0.28 V vs reverse hydrogen electrode [RHE]). Such a low overpotential has never been achieved on any previously reported metallic CRR electrocatalysts, therefore indicating the availability of C N /XG for CO reduction and the applicability of electron transfer modulation to improve CRR catalytic performance.
CO还原反应（CRR）需要高效的电催化剂，然而影响其催化活性的因素尚未被发现。在本文中，采用石墨相氮化碳（g-C₃N₄）来研究通过界面电子转移调节其CRR催化性能的可行性。通过计算方法对一系列有或没有杂原子掺杂的g-C₃N₄/石墨烯（C₃N₄/XG，XG = BG、NG、OG、PG、G）进行CRR综合评估。在不同掺杂情况下观察到可变的吸附能和电子结构，表明较高的催化活性源于更多的界面电子转移。得到了一个活性趋势，显示出C₃N₄/XG对甲烷的CRR具有最佳催化性能，过电位为0.45 V（即相对于可逆氢电极[RHE]为-0.28 V）。如此低的过电位在任何先前报道的金属CRR电催化剂上都从未实现过，因此表明C₃N₄/XG可用于CO还原以及电子转移调制可用于改善CRR催化性能。
