Identifying And Unveiling the Role of Multivalent Metal States for Bidirectional UOR and HER Over Ni, Mo‐Trithiocyanuric Based Coordination Polymer

Author:

Liu Mengying12,Zou Wenhong12,Cong Jing12,Su Nan12,Qiu Silong12,Hou Linxi12ORCID

Affiliation:

1. College of Chemical Engineering Fuzhou University Fuzhou 350116 China

2. Qingyuan Innovation Laboratory Quanzhou 362801 P. R. China

Abstract

AbstractUrea oxidation reaction (UOR), an ideal alternative to oxygen evolution reaction (OER), has received increasing attention for realizing energy‐saving H2 production and relieving pollutant degradation. Normally, most studied Ni‐based UOR catalysts pre‐oxidate to NiOOH and then act as active sites. However, the unpredictable transformation of the catalyst's structure and its dissolution and leaching, may complicate the accuracy of mechanism studies and limit its further applications. Herein, a novel self‐supported bimetallic Mo‐Ni‐C3N3S3 coordination polymers (Mo‐NT@NF) with strong metal–ligand interactions and different H2O/urea adsorption energy are prepared, which realize a bidirectional UOR/hydrogen evolution reaction (HER) reaction pathway. A series of Mo‐NT@NF is prepared through a one‐step mild solvothermal method and their multivalent metal states and HER/UOR performance relationship is evaluated. Combining catalytic kinetics, in situ electrochemical spectroscopic characterization, and density‐functional theory (DFT) calculations, a bidirectional catalytic pathway is proposed by N, S‐anchored Mo5+ and reconstruction‐free Ni3+ sites for catalytic active center of HER and UOR, respectively. The effective anchoring of the metal sites and the fast transfer of the intermediate H* by N and S in the ligand C3N3S3H3 further contribute to the fast kinetic catalysis. Ultimately, the coupled HER||UOR system with Mo‐NT@NF as the electrodes can achieve energy‐efficient overall‐urea electrolysis for H2 production.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Fujian Province

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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