Hierarchically ordered porous superstructure embedded with readily accessible atomic pair sites for enhanced CO2 electroreduction

Jiao，Lei1,3; Li，Xiaofang1; Wei，Wenbo1; Zhou，Sheng Hua1; Han，Shu Guo1; Ma，Dong Dong1; Mao，Yue1; Xu，Qiang5,6; Wu，Xin Tao1,4; Zhu，Qi Long1,2,3,4

2023-08-05

10.1016/j.apcatb.2023.122638

Applied Catalysis B: Environmental   Impact Factor & Quartile

0926-3373

Herein, a hierarchically ordered porous superstructure of N-doped carbon embedded with readily accessible Fe-Ni diatomic sites (FeNi DASs/HOPSNC) has been synthesized for highly efficient CO electroreduction. By integrating additional secondary mesopores into the ordered macroporous skeleton, this distinctive superstructure exhibits greatly enhanced accessibility and mass transfer. Benefiting from the unique structure merits including the synergistic effect in Fe-Ni atomic pair sites and the multi-level porosity, such diatomic site catalyst affords an outstanding electrocatalytic performance with excellent activity and selectivity for CO-to-CO conversion and remarkable stability. Furthermore, systematic characterizations and density functional theory calculations unveiled that the electronic interaction within the diatomic pairs leads to the optimized electronic state and decreased reaction energy barrier for generating COOH* intermediate and weakening the binding strength of CO*, thereby improving the intrinsic catalytic activity and selectivity. This work may inspire further development of high-performance diatomic site catalysts for CO electroreduction and other electrosynthesis.

Carbon dioxide electroreduction Fe-Ni atomic pair sites Ordered macroporous structure Synergistic effects

English

Corresponding

Natural Science Foundation of Fujian Province[2020J01116];Natural Science Foundation of Fujian Province[2021J06033];National Key Research and Development Program of China[2021YFA1500402];National Natural Science Foundation of China[21901246];National Natural Science Foundation of China[22105203];National Natural Science Foundation of China[22175174];State Key Laboratory of Powder Metallurgy[ZDSYS20210709112802010];

CHEMISTRY

2-s2.0-85151820945

Scopus

1.State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences (CAS),Fuzhou,350002,China
2.Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou,350108,China
3.College of Chemistry and Chemical Engineering,Jiangxi Normal University,Nanchang,330022,China
4.University of Chinese Academy of Sciences,Beijing,100049,China
5.Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials (SKLPM),Department of Chemistry and Department of Materials Science and Engineering,Southern University of Science and Technology (SUSTech),Shenzhen,518055,China
6.Institute for Integrated Cell-Material Sciences (iCeMS),Kyoto University,Kyoto,606-8501,Japan

Jiao，Lei,Li，Xiaofang,Wei，Wenbo,et al. Hierarchically ordered porous superstructure embedded with readily accessible atomic pair sites for enhanced CO2 electroreduction[J]. Applied Catalysis B: Environmental,2023,330.

Jiao，Lei.,Li，Xiaofang.,Wei，Wenbo.,Zhou，Sheng Hua.,Han，Shu Guo.,...&Zhu，Qi Long.(2023).Hierarchically ordered porous superstructure embedded with readily accessible atomic pair sites for enhanced CO2 electroreduction.Applied Catalysis B: Environmental,330.

Jiao，Lei,et al."Hierarchically ordered porous superstructure embedded with readily accessible atomic pair sites for enhanced CO2 electroreduction".Applied Catalysis B: Environmental 330(2023).