Enhanced photodegradation of toxic organic pollutants using dual-oxygen-doped porous g-C3N4: Mechanism exploration from both experimental and DFT studies
Enhanced photodegradation of toxic organic pollutants using dual-oxygen-doped porous g-C3N4: Mechanism exploration from both experimental and DFT studies
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使用双氧掺杂多孔 g-C3N4 增强有毒有机污染物的光降解：实验和 DFT 研究的机制探索
DOI：
10.1016/j.apcatb.2019.02.008
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发表时间：
2019-07
期刊：
影响因子：
--
通讯作者：
Wang Xiangke
中科院分区：
文献类型：
--
作者：
Zhang Sai;Liu Yang;Gu Pengcheng;Ma Ran;Wen Tao;Zhao Guixia;Li Lei;Ai Yuejie;Hu Chun;Wang Xiangke
以尿素和草酸铵为原料，采用热聚合法制备了可见光驱动的双氧掺杂多孔g-C3 N4（OPCN）光催化剂。引入的O原子优选同步取代对位的两个sp2杂化的N原子（即，N1′和N4′位）的双氧掺杂的g-C3 N4。与多孔结构一起，OPCN表现出增大的比表面积，缩小的带隙和扩大的可见光响应。在可见光照射下，最佳OPCN的光催化活性约为纯g-C3 N4的9倍，对双酚A（BPA）的去除率也高于纯g-C3 N4，对各种氯酚、酚类和染料的去除率也很高.结合实验和密度泛函理论计算，这种双氧掺杂的结构导致有效的电荷转移和分离的OPCN在可见光照射下，通过形成的e-和h+相关的共轭离域系统的表面，这有助于其与有机污染物和吸附O2的界面接触。结果表明，BPA的降解很容易被光诱导的h+诱导，然后被O2自由基dot-彻底矿化。另一方面，产生了更多的O2自由基点自由基，由于其强氧化能力，也可以直接氧化BPA。OPCN催化剂在光催化反应过程中具有良好的上级稳定性和重复使用性。本工作为制备高性能的非金属光催化剂用于废水处理提供了一个新的视角。
Novel visible-light-driven dual-oxygen-doped porous g-C3N4(OPCN) photocatalysts were synthesized by a facile thermal copolymerization of urea and ammonium oxalate. The introduced O atoms were preferable to synchronously substitute for two sp2-hybridized N atoms in the para-positions (i.e., N1′ and N4′ sites) of the melem unit by forming dual-O-doped g-C3N4. Together with porous structures, OPCN exhibited enlarged specific surface area, narrowed band gap and expanded visible light response. The photocatalytic activity of the optimal OPCN was approximately 9 times higher than that of pure g-C3N4for bisphenol A (BPA) removal under visible light irradiation, and efficient removal rates for various chlorophenols, phenols and dyes were also observed. Combined with experiments and DFT calculations, this dual-O-doped structure resulted in effective charge transfer and separation of OPCN under visible light irradiation by forming e−and h+-related conjugated delocalized systems on the surface, which contributed to its interfacial contact with organic pollutants and adsorbed O2. As a result, the degradation of BPA was readily induced by photoinduced h+and then thoroughly mineralized by O2radical dot−. On the other hand, more O2radical dot−radicals were generated, which could also oxidize BPA directly due to their strong oxidation power. The superior stability and reusability of OPCN catalysts were also revealed during photoreaction. This work provides a novel viewpoint to fabricate high-performance nonmetal photocatalysts for wastewater treatment.
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影响因子：
16.6
作者：
Lau VW;Moudrakovski I;Botari T;Weinberger S;Mesch MB;Duppel V;Senker J;Blum V;Lotsch BV
通讯作者：
Lotsch BV
影响因子：
11.4
作者：
Jixiang Yuan;Qiang Wu;Peng Zhang;J. Yao;T. He;Yaan Cao
通讯作者：
Jixiang Yuan;Qiang Wu;Peng Zhang;J. Yao;T. He;Yaan Cao
通过受控超薄g-C3N4层增强核壳结构g-C3N4@TiO2的光催化活性
影响因子：
22.1
作者：
Wang, Yingying;Yang, Wenjuan;Zhu, Yongfa
通讯作者：
Zhu, Yongfa
类囊体启发的多壳 g-C3N4 纳米胶囊具有增强的可见光捕获和电子转移特性，可实现高效光催化
影响因子：
17.1
作者：
Tong, Zhenwei;Yang, Dong;Jiang, Zhongyi
通讯作者：
Jiang, Zhongyi
影响因子：
9.5
作者：
Xue, Jinjuan;Ma, Shuaishuai;He, Man
通讯作者：
He, Man