Pyrrolic-nitrogen doped graphene:a metal-free electrocatalyst with high efficiency and selectivity for the reduction of carbon dioxide to formic acid:a computational study
Searching for metal-free catalysts for the carbon dioxide reduction reaction(CO2RR)has been a key challenge in the electrosynthesis of fuels for CO2 utilization.In this work,we investigated the potential of N-doped graphene as the electrocatalyst of CO2RR by means of comprehensive density functional theory(DFT)computations.The computations revealed that N-doping can modify the electronic properties of graphene for enhancing the electrochemical reduction of CO2 into CO and HCOOH,resulting in a low free energy barrier for the potential-limiting step to form the key intermediate COOH as well as the strong adsorption energy of adsorbed COOH and the weak adsorption energy of CO or HCOOH.The highest catalytic activity toward CO2RR is shown by pyrrolic N-doped graphene due to its lowest overpotential of 0.24 V among all N-doped graphenes,and leads exclusively to HCOOH as the product.Therefore,our results demonstrated that N-doped graphene holds great promise as an electrocatalyst for the CO2RR with high efficiency and selectivity by suitably tuning its N species.
Yuejie Liu Jingxiang Zhao Qinghai Cai
Modern Lab Center,Harbin Normal University,Harbin 150025,China College of Chemistry and Chemical Engineering,Harbin Normal University,Harbin 150025,China Modern Lab Center,Harbin Normal University,Harbin 150025,China;College of Chemistry and Chemical Eng
国内会议
大连
英文
286-293
2016-09-24（万方平台首次上网日期，不代表论文的发表时间）