首页|Coupling Au with BOx matrix induced by Closo-boron cluster for electrochemical synthesis of ammonia
Coupling Au with BOx matrix induced by Closo-boron cluster for electrochemical synthesis of ammonia
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Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BOx substrates(Au-BOx),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BOx possesses excel-lent NRR activity(NH3 yield of 48.52 μg h-1 mgca1t,Faraday efficiency of 56.18%),and exhibits high sta-bility and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond,which considerably facilitates the hydrogenation of*N2-*NH3.The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utiliz-ing boron clusters as reducing and stabilizing agents.
Key Laboratory of Flexible Electronics(KLOFE)& Institute of Advanced Materials(IAM),School of Flexible Electronics(Future Technologies),Nanjing Tech University,Nanjing 211816,Jiangsu,China
College of Chemistry and Molecular Sciences,Wuhan University,Wuhan 430072,Hubei,China
National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaJiangsu Provincial Funds