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Single tungsten atom steered band-gap engineering for graphitic carbon nitride ultrathin nanosheets boosts visible-light photocatalytic H2 evolution
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2021-04-24 , DOI: 10.1016/j.cej.2021.130004
Fu Zhang , Jihua Zhang , Haifei Wang , Jianming Li , Huanhuan Liu , Xu Jin , Xiaoqi Wang , Genqiang Zhang

In this work, we report a W single atoms modified g-C3N4 porous unltrathin nanosheets (WSA-CN-PUNS) catalyst for photocatalytic H2 evolution, which is synthesized by simply calcining the polyprrole-polyoxometalate/g-C3N4 composite in air. DFT calculation and experimental results reveal that the WSA-CN-PUNS catalyst has a reduced band-gap, dopant-related defect levels and inhibited charge recombination. As a result, the WSA-CN-PUNS shows an activity of 3.02 mmol h−1 g−1 toward H2 production under visible light, which is 9.7 times higher than that of pristine g-C3N4. Meanwhile, for eliminating the waste of sacrifice agent, we demonstrate an alternative approach by coupling the photocatalytic H2 evolution with benzyl alcohol oxidation, and the H2/benzaldehyde production rates are 298.7/305.1 μmol h−1 g−1, respectively. This work not only provides a new strategy for designing high-efficiency single W atom dispersed hybrid catalyst, but also demonstrates the great potential of its practical applications in photocatalytic H2 evolution.



中文翻译:

单个钨原子转向带隙工程为石墨碳氮化物的超薄纳米片提升可见光的光催化ħ 2进化

在这项工作中,我们报告了一种W单原子修饰的gC 3 N 4多孔Unltrathin纳米片(W SA -CN-PUNS)催化剂,用于光催化H 2的演化,该催化剂是通过简单地在以下条件下煅烧聚吡咯-多金属氧酸盐/ gC 3 N 4复合材料而合成的。空气。DFT计算和实验结果表明,W SA -CN-PUNS催化剂具有降低的带隙,掺杂剂相关的缺陷水平和抑制的电荷重组。其结果是,在W SA -CN-双关语表示的3.02毫摩尔h的活性-1-1朝向ħ 2在可见光下的产量是原始gC 3 N 4的9.7倍。同时,为了消除牺牲剂的浪费,我们证明了通过将光催化的H 2释放与苯甲醇氧化偶联的替代方法,并且H 2 /苯甲醛的生产率分别为298.7 / 305.1μmolh -1 g -1。这项工作不仅为设计高效的单W原子分散杂化催化剂提供了新的策略,而且证明了其在光催化H 2释放中的实际应用的巨大潜力。

更新日期:2021-05-25
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