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使用掺杂磷并负载碳量子点的改性石墨相氮化碳在可见光下增强非牺牲性光催化过氧化氢生成:构建电子转移通道

Enhanced nonsacrificial photocatalytic generation of hydrogen peroxide under visible light using modified graphitic carbon nitride with doped phosphorus and loaded carbon quantum dots: Constructing electron transfer channel.

作者信息

Shi Jianhui, Luo Yifei, Yang Tiantian, Wang Hui, Ju Chenke, Pu Kaikai, Shi Jiating, Zhao Ting, Xue Jinbo, Li Yuzhen, Li Houfen, Xu Haiyuan, Li Xiaotong, Fan Zheng

机构信息

College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan, PR China.

College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan, PR China.

出版信息

J Colloid Interface Sci. 2022 Dec 15;628(Pt A):259-272. doi: 10.1016/j.jcis.2022.07.137. Epub 2022 Jul 25.

DOI:10.1016/j.jcis.2022.07.137
PMID:35932665
Abstract

The photocatalytic production of HO by graphite-phase carbon nitride (g-CN) using water and oxygen is a promising and sustainable method. Nevertheless, the yield of HO produced by the pristine g-CN is still far from satisfactory owing to limited optical absorption, rapid photogenerated electron-hole recombination and poor surface electron migration. Therefore, p-PCN/CQDs was designed and synthesized by doping phosphorus (P) and loading carbon quantum dots (CQDs) to modify porous g-CN (p-CN) via a facile method. Herein, P acted as an electron transfer bridge to induce electrons into CQDs, while CQDs acted as an electron trapping material to capture and stabilize photogenerated electrons. Moreover, CQDs could enhance their optical absorption due to its unique optical properties. Notably, p-PCN/CQDs presented highly boosted HO generation activity, its HO production yield for 5 h was up to 494 μM/L and the formation rate constant K in the first hour was 238 μM h without adding sacrificial agents and without bubbling oxygen under visible light, which took precedence among the reported results under the same conditions. It should be noted that the composite p-PCN/CQDs also possessed low HO decomposition behavior based on the effect of CQDs stabilizing electrons. In addition, the possible mechanism of photocatalytic HO generation for p-PCN/CQDs was also proposed. Our research provided a new idea for the design of novel photocatalysts to efficient generation of HO.

摘要

利用水和氧气通过石墨相氮化碳(g-CN)光催化产生活性羟基(HO)是一种很有前景的可持续方法。然而,由于光吸收有限、光生电子-空穴快速复合以及表面电子迁移较差,原始g-CN产生活性羟基的产率仍远不能令人满意。因此,通过一种简便的方法,通过掺杂磷(P)和负载碳量子点(CQDs)来修饰多孔g-CN(p-CN),设计并合成了p-PCN/CQDs。在此,P作为电子转移桥将电子引入CQDs,而CQDs作为电子捕获材料捕获并稳定光生电子。此外,由于其独特的光学性质,CQDs可以增强其光吸收。值得注意的是,p-PCN/CQDs表现出高度增强的活性羟基生成活性,在可见光下不添加牺牲剂且不鼓入氧气的情况下,其5小时的活性羟基产率高达494μM/L,第一小时的生成速率常数K为238μM/h,在相同条件下的报道结果中名列前茅。应该注意的是,基于CQDs稳定电子的作用,复合p-PCN/CQDs还具有较低的活性羟基分解行为。此外,还提出了p-PCN/CQDs光催化产生活性羟基的可能机理。我们的研究为设计高效产生活性羟基的新型光催化剂提供了新思路。

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