Ultrafast NaN3-deflagration induced nitrogen vacancy-enriched g-C3N4 for tailoring band structures and enhanced photocatalytic performance

Ultrafast NaN3-deflagration induced nitrogen vacancy-enriched g-C3N4 for tailoring band structures and enhanced photocatalytic performance
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超快 NaN3 爆燃诱导的氮空位富集 g-C3N4 用于定制能带结构并增强光催化性能

DOI:
10.1016/j.jpowsour.2019.226731
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发表时间:
2019-09
影响因子:
9.2
通讯作者:
Yang Guangcheng
Yang Guangcheng
中科院分区:
工程技术2区
文献类型:
--
作者:
Tang Jialin;Liu Yousong;Hu Yingjie;Huang Jianwen;Wang Binshen;Yang Chengtao;Yang Guangcheng

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空位缺陷工程能够操纵无金属光催化剂(例如石墨氮化碳)的电子结构,从而显着增强催化活性。在这里,我们报告了一种通过NaN3爆燃合成富含氮空位的g-C3N4(DCN)的一步原位掺杂策略。在双氰胺缩聚过程中,少量添加NaN3即可在短短5秒内实现超快爆燃,其中部分N原子会被Na纳米团簇瞬间还原,并在g-C3N4的形成过程中留下大量氮空位。如此高含量的二配位氮空位有利于显着提高 g-C3N4 的光学吸收并缩小带隙,这得到了实验和密度泛函理论 (DFT) 计算的支持。由此产生的有缺陷的g-C3N4产物在光电流响应和有机污染物降解方面表现出较高的光催化性能,明显优于原始的g-C3N4。爆燃辅助缺陷工程策略有望用于构建其他高性能无金属光催化剂。
Vacancy defect engineering is capable of manipulating electronic structure of metal-free photocatalysts such as graphitic carbon nitride for significantly enhancing catalytic activities. Here, we report a one-step in-situ doping strategy to synthesize nitrogen-vacancy-enriched g-C3N4(DCN) through NaN3-deflagration. Small addition of NaN3endows ultrafast deflagration within only 5 s during polycondensation of dicyanodiamine, where partial N-atoms suffer from reduction instantaneously by Na-nanoclusters and leaving remarkable numbers of nitrogen vacancies during the formation of g-C3N4. Such high content of two-coordinated nitrogen vacancy benefits dramatically improving optical absorption and narrowed band gap of g-C3N4, which is supported by both experimental and density functional theory (DFT) calculations. The resulting defective g-C3N4products demonstrate high photocatalytic performances in both photocurrent response and organic pollutant degradation, which is significantly superior to that of pristine g-C3N4. The deflagration-assisted defect engineering strategy is promising for constructing other high-performance metal-free photocatalysts.
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