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首页> 外文期刊>Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications >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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Enhanced photodegradation of toxic organic pollutants using dual-oxygen-doped porous g-C3N4: Mechanism exploration from both experimental and DFT studies

机译:使用双氧掺杂多孔G-C3N4增强了有毒有机污染物的光降解:实验和DFT研究的机制探索

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摘要

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-C3N4 for 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 O-2. As a result, the degradation of BPA was readily induced by photoinduced h(+) and then thoroughly mineralized by O-2(center dot-). On the other hand, more O2(center 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.
机译:通过尿素和草酸铵的容易的热共聚合,合成了新型的可见光驱动的双氧掺杂多孔G-C3N4(OPCN)光催化剂。通过形成双O掺杂G-C3N4,优选引入的O原子在熔融单元的对位(即,N1'和N4位点)中同步地替代于熔融单元的两个SP2杂交的N原子。与多孔结构一起,OPCN表现出比特定表面积,带隙隙窄和膨胀的可见光反应。最佳OPN的光催化活性比在可见光照射下的双酚A(BPA)除去的纯G-C3N4高约9倍,并且还观察到各种氯化苯酚,酚和染料的有效的去除率。结合实验和DFT计算,通过在表面上形成e( - )和H(+)相关的​​共轭分层系统,导致该双O掺杂结构在可见光照射下的有效电荷转移和OPCN的分离,这是贡献的它与有机污染物和吸附的O-2界面接触。结果,通过光致强H(+)容易地诱导BPA的降解,然后通过O-2(中心点)彻底矿化。另一方面,产生更多O2(中心点)基团,这也可以由于其强的氧化能力而直接氧化BPA。在光反应期间也揭示了OPCN催化剂的优异稳定性和可重用性。这项工作提供了一种新的观点,用于制造用于废水处理的高性能非金属光催化剂。

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  • 作者单位

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

    Guangzhou Univ Sch Environm Sci &

    Engn Guangzhou 510006 Guangdong Peoples R China;

    North China Elect Power Univ MOE Key Lab Resources &

    Environm Syst Optimizat Coll Environm Sci &

    Engn Beijing 102206 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 催化;
  • 关键词

    Photocatalytic degradation; Graphitic carbon nitride; Dual-O-doped; Porous structure; Density functional theory;

    机译:光催化降解;石墨碳氮化物;双O掺杂;多孔结构;密度函数理论;

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