TY - JOUR
T1 - Composition Tailoring via N and S Co-doping and Structure Tuning by Constructing Hierarchical Pores
T2 - Metal-Free Catalysts for High-Performance Electrochemical Reduction of CO2
AU - Yang, Hengpan
AU - Wu, Yu
AU - Lin, Qing
AU - Fan, Liangdong
AU - Chai, Xiaoyan
AU - Zhang, Qianling
AU - Liu, Jianhong
AU - He, Chuanxin
AU - Lin, Zhiqun
N1 - Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2018/11/19
Y1 - 2018/11/19
N2 - A facile route to scalable production of N and S co-doped, hierarchically porous carbon nanofiber (NSHCF) membranes (ca. 400 cm2 membrane in a single process) is reported. As-synthesized NSHCF membranes are flexible and free-standing, allowing their direct use as cathodes for efficient electrochemical CO2 reduction reaction (CO2RR). Notably, CO with 94 % Faradaic efficiency and −103 mA cm−2 current density are readily achieved with only about 1.2 mg catalyst loading, which are among the best results ever obtained by metal-free CO2RR catalysts. On the basis of control experiments and DFT calculations, such outstanding CO Faradaic efficiency can be attributed to the co-doped pyridinic N and carbon-bonded S atoms, which effectively decrease the Gibbs free energy of key *COOH intermediate. Furthermore, hierarchically porous structures of NSHCF membranes impart a much higher density of accessible active sites for CO2RR, leading to the ultra-high current density.
AB - A facile route to scalable production of N and S co-doped, hierarchically porous carbon nanofiber (NSHCF) membranes (ca. 400 cm2 membrane in a single process) is reported. As-synthesized NSHCF membranes are flexible and free-standing, allowing their direct use as cathodes for efficient electrochemical CO2 reduction reaction (CO2RR). Notably, CO with 94 % Faradaic efficiency and −103 mA cm−2 current density are readily achieved with only about 1.2 mg catalyst loading, which are among the best results ever obtained by metal-free CO2RR catalysts. On the basis of control experiments and DFT calculations, such outstanding CO Faradaic efficiency can be attributed to the co-doped pyridinic N and carbon-bonded S atoms, which effectively decrease the Gibbs free energy of key *COOH intermediate. Furthermore, hierarchically porous structures of NSHCF membranes impart a much higher density of accessible active sites for CO2RR, leading to the ultra-high current density.
KW - CO reduction
KW - electrocatalysis
KW - hierarchical pores
KW - metal-free catalysts
KW - ultrahigh current density
UR - http://www.scopus.com/inward/record.url?scp=85055525602&partnerID=8YFLogxK
U2 - 10.1002/anie.201809255
DO - 10.1002/anie.201809255
M3 - Article
C2 - 30284359
AN - SCOPUS:85055525602
SN - 1433-7851
VL - 57
SP - 15476
EP - 15480
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 47
ER -