Highly selective photocatalytic CO2 reduction and hydrogen evolution facilitated by oxidation induced nitrogen vacancies on g-C3N4

光催化 氮气 光化学 选择性 石墨氮化碳 化学 吸附 氧化还原 氮化物 材料科学 无机化学 催化作用 纳米技术 物理化学 有机化学 图层(电子)
作者
Zhengdong Xu,Yang Chen,Binghao Wang,Yu Ran,Junbo Zhong,Minjiao Li
出处
期刊:Journal of Colloid and Interface Science [Elsevier BV]
卷期号:651: 645-658 被引量:30
标识
DOI:10.1016/j.jcis.2023.08.012
摘要

The introduction of nitrogen vacancies into polymeric carbon nitride (PCN) has been attested to be a reliable strategy to enhance photocatalytic performance. Nitrogen vacancies were considered as active sites to promote the adsorption of target molecules and capture photoexcited electrons to inhibit the recombination of charge pairs, accelerate photoinduced electrons to participate in photocatalytic reaction. In this paper, a series of PCN with rich nitrogen vacancies were prepared by etching of chromic acid solution. Sample 20KCSCN had the highest photocatalytic performance whose evolution efficiency of CO2 to CO and CH4 can reach 3.9 and 0.5 μmol·g−1·h−1, respectively. These evolution efficiencies are 2.9 and 4 times higher than that of the PCN. Meanwhile, 20KCSCN demonstrates high CO conversion selectivity and stability. The successful introduction of nitrogen vacancies not only increases the active sites of PCN surface, but also optimizes the optical structure, which dramatically boosts the separation of photoexcited charge pairs and the reduction capacity of photogenerated electrons. The enhancement mechanism for photocatalytic CO2 reduction performance of PCN was proposed. Besides, photocatalytic H2 evolution experiments were performed on all samples to confirm the universality of PCN photocatalytic activity enhancement etched by chromic acid solution. H2 evolution rate on 20KCSCN can reach 652 μmol·g−1·h−1, which is 1.6-fold higher than that on PCN (254 μmol·g−1·h−1) after 4 h irradiation under a 300 W Xe lamp. This work offers new venue for introducing nitrogen vacancies in PCN to regulate photoexcited charge pairs transfer. The photocatalytic enhancement of CO2 reduction could be used to alleviate the serious issue of excessive CO2 emission and energy crisis.
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