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Jointly Enhanced Nitrate and Water Activation by Precisely Ligand Substituent Regulation in Bimetallic Cluster for
Yali Dai1, Youqiong Fang2, Yuzhuo Yang1
1Department of Materials Science and Engineering, Centre For Atomic Engineering of Advanced Materials, Key Laboratory of Functional Inorganic Material Chemistry of Anhui Province, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei, China.
Abstract:
Herein, Cu4Pt2 bimetallic series clusters (Cu4Pt2(R-C6H5-C≡C)4(dppy)4(PF6)2, dppy = diphenyl-2-pyridylphosphine, R = CF3, F, MeO, abbreviation as R-Cu4Pt2) are synthesized to realize multitask simultaneous processing in NO3RR, in which NO3 - activation and conversion performs on Cu site, while Pt site is responsible for H2O dissociation and *H continuous supplementation. The precisely perturbation in electronic structure of metal active site is further achieved by ligand substituent micro-regulation strategy. Based on the electron push-and-pull effect, as the electron-withdrawing ability of ligand substituent increases (-MeO < -F < -CF3), the electronic density of metal active site gradually decreases, concurrently promoting NO3 - adsorption and activation, H2O dissociation and *H production, thereby improving NO3RR activity. As a result, CF3-Cu4Pt2 shows the best NO3RR performance with a high Faradaic efficiency of 91.84% and a satisfactory NH3 yield rate of 13.65 mgNH3 mgcat -1 h-1 at -0.5 V (vs RHE), followed by F-Cu4Pt2 and MeO-Cu4Pt2. Comprehensive electrochemical experiments, in situ mechanism studies, and theoretical calculations confirm the co-enhanced NO3 - and H2O activation through fine substituent adjustment. This work not only inspires the construction of multi-functional catalytic sites with superiority complementation for complex reactions, but also illuminates an achievable pathway to design future advanced catalysts via exquisite ligand micro-regulation.
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