Interfacial Electron Regulation of Rh Atomic Layer-Decorated SnO2 Heterostructures for Enhancing Electrocatalytic Nitrogen Reduction

Reversible hydrogen electrode Ammonia production
DOI: 10.1021/acsami.1c25240 Publication Date: 2022-03-03T13:47:28Z
ABSTRACT
Ammonia (NH3), which serves as a fertilizer supply, is struggling to satisfy the ever-growing population requirements over world. The electrocatalytic nitrogen reduction NH3 production highly desired but shows extremely poor activity and selectivity of reported electrocatalysts. In this work, we rationally design novel Rh atomic layer-decorated SnO2 heterostructure catalyst through interfacial engineering strategy, simultaneously achieving highest yield rate (149 μg h-1 mgcat-1) Faradaic efficiency (11.69%) at -0.35 V vs reversible hydrogen electrode. This result superior optimum response previously SnO2- or Rh-based catalysts for electrochemical reduction. Both X-ray absorption spectra characterization density functional theory calculations reveal strong electron interaction between layer heterostructure, effectively regulated transfer d-band center. downshift center results in greatly reduced H adsorption energy accelerated reaction kinetics work endows new insight into regulation weakening further enhancing N2
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