摘要
The advancement in catalysis techniques for sustainable environmental applications,particularly an alternative to the current Haber-Bosch process for NH_(3),has recently gained widespread attention.Although photocatalytic conversion of N_(2) to NH_(3) using solar energy is an eco-friendly method,it has the limitation of low quantum yield.Recently,2D Bi-based photocatalysts which exhibit higher visible light absorption than TiO_(2) and higher stability than MXene have been an active research topic,and their performance can be enhanced through improved visible light absorption properties by incorporating plasmonic gold nanoparticles while nitrogen adsorption could be enhanced through oxygen vacancy(OV)processes.In the present study,we explore the application of 2D nanosized Bi_(2)O_(3–x) and gold nanoparticles for visible light photo generation of NH_(3).HRTEM and XPS reveal that the formation of AuNP and nano-sized Bi_(2)O_(3–x) in AuNP/Bi_(2)O_(3–x) heterozygote structure promotes the charge carrier mobility and charge transport at the interface,resulting in a 2.6-fold increase in the photocatalytic activity compared to micro-sized Bi_(2)O_(3–x) with AuNP.The improved photocatalytic performance can be ascribed to significant enhancement of visible light absorption by plasmonic nanoparticles,fast charge transport and mobility(due to sheet morphology)and the N_(2) activation by OV in AuNP/Bi_(2)O_(3–x) heterozygote.Through a systematic experimental investigation involving catalysts,concentration,pH,and scavengers,the highest photocatalytic performance was achieved with the heterozygote structures of AuNP/n-Bi_(2)O_(3–x) under optimized conditions,yielding 432.5μmol gcat^(-1) h^(-1) of NH_(3).
基金
Financial support for this work by the National Research Foundation of Korea(2022R1F1A1074682,2022R1A4A1031687)
Korea University,and the KU-KIST Research Fund.
