空位缺陷
三聚氰胺
煅烧
氮气
光催化
催化作用
化学
反应性(心理学)
原位
光化学
化学工程
材料科学
有机化学
结晶学
病理
工程类
替代医学
医学
作者
Yuhan Li,Miaoli Gu,Min Zhang,Xianming Zhang,Kangle Lv,Yunqi Liu,Wingkei Ho,Fan Dong
标识
DOI:10.1016/j.cej.2020.124421
摘要
The introduction of nitrogen vacancy to C3N4 holds promise in the photocatalytic behavior improvement. Yet, minimal literatures on reaction and stability mechanisms are presently available in the NO-oxidation reaction of C3N4. Here C3N4 with three coordinated (N3C) nitrogen vacancy was prepared by directly calcining the mixture of azodicarbonamide and melamine. Unlike previously reported C3N4 that exhibits an obvious deactivation beyond 30 min (>10% loss of reactivity after one cycle) and high in-situ formed NO2 concentration (>100 ppb), the C3N4 with three coordinated (N3C) nitrogen vacancy exerts increased NO-oxidation performance (40.3%, ~2.28 times higher than that of pristine C3N4 with a NO-removal rate of 17.7%) and suppressed in-situ produced NO2 (36.3 ppb, decreased by 76.6 ppb compared to pure C3N4) as well excellent stability (<2% loss of activity after a 5 h cycling test). DFT calculations reveal that, intermediates (NO2) and end-products (NO2– and NO3–) can weakly adsorp on the surface of C3N4 with three coordinated (N3C) nitrogen vacancy, thus rendering a well maintained activity. Based on the time-dependent ESR measurements, the 1O2 generation, which achieving from the O2 activation process, can compensate for the consumption of major reactive species and thus support the remarkable reusability. Therefore, this study provides a potential and sustainable route for the steady and efficient NO-oxidation.
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