Constructing interfacial active sites in Ru/g-C3N4−x photocatalyst for boosting H2 evolution coupled with selective benzyl-alcohol oxidation

光催化 苯甲醇 Boosting(机器学习) 光化学 化学 催化作用 材料科学 化学工程 计算机科学 有机化学 人工智能 工程类
作者
Qing Yang,Ting Wang,Ziqiang Zheng,Bing Xing,Can Li,Benxia Li
出处
期刊:Applied Catalysis B-environmental [Elsevier BV]
卷期号:315: 121575-121575 被引量:144
标识
DOI:10.1016/j.apcatb.2022.121575
摘要

Engineering the interfacial active sites in metal modified semiconductor photocatalysts is highly promising but still challenging for developing heterogeneous photocatalysts with high activity and selectivity. Herein, the Ru/g-C 3 N 4−x photocatalyst consisting of small Ru nanoparticles (NPs) anchored on defective g-C 3 N 4−x nanoflakes with nitrogen-vacancies (V N s) is prepared by a photoinduced method, where the photoexcited electrons of g-C 3 N 4 enable the deposition of Ru NPs and the hole-generated oxidative radicals induce the formation of V N defects on g-C 3 N 4 . The Ru/g-C 3 N 4−x photocatalyst exhibits excellent performance toward the photocatalytic redox coupling reaction of hydrogen evolution and selective oxidation of benzyl alcohol, showing the generation rates of hydrogen and benzaldehyde up to 6.42 and 5.07 mmol∙g cat −1 ∙h −1 , respectively. The underlying photocatalytic mechanism is elucidated by a series of control experiments, in situ characterizations and theoretical calculations. Both experimental and theoretical studies elucidate that the synergy of interfacial Ru sites and V N defects on g-C 3 N 4−x plays a critical role in boosting the photocatalytic redox coupling reaction. The Ru/g-C 3 N 4−x heterointerface not only accelerates the separation of photogenerated charge carriers but also provides the optimum active sites for H 2 evolution and benzyl-alcohol oxidation. • Ru cocatalyst and nitrogen vacancies are synchronously constructed on g-C 3 N 4 . • Interfacial active sites synergistically boost photocatalytic redox coupling reaction. • High production rates of H 2 and benzaldehyde are achieved under simulated sunlight. • Photocatalytic mechanism is elucidated by experiments and calculations.
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