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Two types of cooperative nitrogen vacancies in polymeric carbon nitride for efficient solar-driven H2O2 evolution
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2019-12-30 , DOI: 10.1016/j.apcatb.2019.118581
Yao Xie , Yunxiang Li , Zhaohui Huang , Junying Zhang , Xiaofang Jia , Xu-Sheng Wang , Jinhua Ye

Hydrogen peroxide generation based on photocatalysis is a sustainable and clean process compared with the current industrial way but suffers from low efficiency due to the rapid recombination of carriers and the lack of suitable active sites. To enhance the efficiency in hydrogen peroxide generation, herein, we introduce two types of cooperative N vacancies, i.e., NHx and N2C vacancy, into the framework of polymeric carbon nitride. It is found that the optimized sample delivers a 15 times enhancement in solar-driven H2O2 production as well as excellent stability. And the apparent quantum efficiency reached to 26.78% and 11.86% at 340 nm and 420 nm, respectively. A series of comparative experiments and density functional theory calculations both reveal that NHx and N2C vacancies can accelerate photoexcited charge separation and assist in activating oxygen in the two-electron pathway, respectively. The strategy of targeted introducing two types of cooperative N vacancies provides a novel and promising solution to design and develop efficient catalyst in various photocatalytic reactions. This work will motivate future work in defect chemistry towards various photocatalytic reactions.



中文翻译:

聚合氮化碳中两种类型的协作氮空位,可有效驱使太阳驱动的H 2 O 2逸出

与目前的工业生产方式相比,基于光催化的过氧化氢生产是一种可持续且清洁的工艺,但是由于载体的快速重组和缺乏合适的活性位点而使效率低下。为了提高过氧化氢生成的效率,在本文中,我们将两种类型的协作N空位引入到了聚合氮化碳的框架中,即NH x和N 2C空位。发现优化的样品使太阳能驱动的H 2 O 2增强了15倍生产以及出色的稳定性。在340nm和420nm处,表观量子效率分别达到26.78%和11.86%。一系列比较实验和密度泛函理论计算均表明NH x和N 2C空位可分别加速光激发电荷的分离并协助激活双电子途径中的氧。有针对性地引入两种类型的协作N空位的策略为设计和开发各种光催化反应中的高效催化剂提供了一种新颖而有希望的解决方案。这项工作将激励未来在缺陷化学领域朝着各种光催化反应的方向发展。

更新日期:2019-12-30
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