Axial Phosphate Coordination in Co Single Atoms Boosts Electrochemical Oxygen Evolution.
Yan Liu, Shuangshuang Zhang, Chi Jiao, Huimei Chen, Gang Wang, Wenjie Wu, Zhiwen Zhuo, Junjie Mao
Author Information
Yan Liu: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.
Shuangshuang Zhang: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.
Chi Jiao: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.
Huimei Chen: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.
Gang Wang: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.
Wenjie Wu: Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190, P. R. China.
Zhiwen Zhuo: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China.
Junjie Mao: Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, P. R. China. ORCID
Cobalt single atoms coordinated with planar four nitrogen atoms (Co N ) represent an efficient electrocatalyst for oxygen evolution reaction (OER), whereas the large energy barrier of CoOH dehydrogenation limits the OER activity. Herein, axial phosphate (PO ) coordination is incorporated in Co N single atoms of cobalt phthalocyanine@carbon nanotubes (P-CoPc@CNT), so as to boost the intrinsic OER performance through manipulating the reaction pathway. With a relative low mass loading of Co (2.7%), the P-CoPc@CNT shows remarkable alkaline OER activity with the overpotential of 300 mV and Tafel slope of 41.7 mV dec , which dramatically outperforms the CoPc@CNT without axial PO coordination. Based on mechanistic analysis, the axial PO coordination directly participates in the OER cycle by the transformation of axial ligand. Specially, the CoOH dehydrogenation process is replaced by the dehydrogenation of HPO -Co N intermediate, which largely decreases the energy barrier and thus benefits the whole OER process.
