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Plasmon and N-vacancy synergistically enhanced tubular carbon nitride-based S-scheme heterojunction photocatalyst with one stone five birds function: Pathways, DFT calculation and mechanism insight
Journal of Catalysis ( IF 6.5 ) Pub Date : 2024-10-21 , DOI: 10.1016/j.jcat.2024.115813 Feng Sun, Qian Xu, Haiyang Liu, Da Xu, Xinxing Wang, Chuan Luo, Tianqi Wang, Hui Yu, Wensheng Yu, Xiangting Dong
Journal of Catalysis ( IF 6.5 ) Pub Date : 2024-10-21 , DOI: 10.1016/j.jcat.2024.115813 Feng Sun, Qian Xu, Haiyang Liu, Da Xu, Xinxing Wang, Chuan Luo, Tianqi Wang, Hui Yu, Wensheng Yu, Xiangting Dong
From the perspectives of innovation and broad-spectrum, tubular carbon nitride-based photocatalyst, viz. , Ag/AgI/g-C3 N4 S-scheme heterojunction photocatalyst, with enhancement of nitrogen vacancy and localized surface plasmon resonance (LSPR) effect is reasonably devised and manufactured via combining hydrothermal, calcination and photo-reduction techniques. The optimal specimen displays high photocatalytic activity in removal of dyes [such as crystal violet (CV), 100.00 %/60 min], antibiotics [such as levofloxacin (LEV), 88.72 %/50 min] and Cr(VI) (100.00 %, 30 min), photocatalytic hydrogen evolution (1023.3 μmol h−1 g−1 ) and H2 O2 generation (866.2 μmol h−1 g−1 ), achieving broad-spectrum natures, viz. , realizing the function of “one stone five birds”. The broad-spectrum natures are attributed to the synergisms of nitrogen vacancy, LSPR effect of Ag, hollow tube structure and S-scheme heterojunction, which facilitate the separation and migration of photo-generated carriers and inject “hot electrons” generated by Ag into the conduction band of Ag/AgI/g-C3 N4 , increase the specific surface area and broaden the spectral response range. Further, the degraded intermediates of CV and LEV and possible degradation pathways are rationally advanced by the aid of LCMS spectra, the predicted toxicity of degraded intermediates of LEV is assessed by Toxicity Estimation Software (T.E.S.T.), and the biotoxicity of CV, LEV and Cr(VI) solutions after photocatalytic degradation is further assessed by feat of cultivate rice. Synergistically enhanced photocatalytic mechanism of Ag/AgI/g-C3 N4 hollow tube S-scheme heterojunction is confirmed based upon a series of sound experiments, fs-TA spectra, in-situ XPS and DFT calculation, etc .
中文翻译:
等离激元和 N 空位协同增强管状氮化碳基 S 型异质结光催化剂,具有一石五鸟功能:途径、DFT 计算和机理洞察
从创新和广谱的角度出发,通过结合水热、煅烧和光还原技术,合理设计并制造了增强氮空位和局域表面等离子体共振 (LSPR) 效应的管状氮化碳基光催化剂,即 Ag/AgI/g-C3N4 S 型异质结光催化剂。最佳样品在去除染料[如结晶紫(CV),100.00 %/60 min]、抗生素[如左氧氟沙星(LEV),88.72 %/50 min]和Cr(VI)(100.00 %,30 min)、光催化析氢(1023.3 μmol h−1 g−1)和H2O2生成(866.2 μmol h−1 g−1)方面表现出较高的光催化活性,实现了广谱性质,即实现了“一石五鸟”的功能。广谱性质归因于氮空位、Ag 的 LSPR 效应、空心管结构和 S 型异质结的协同作用,它们促进了光生载流子的分离和迁移,并将 Ag 产生的“热电子”注入 Ag/AgI/g-C3N4 的导带,增加了比表面积并拓宽了光谱响应范围。此外,借助LCMS光谱合理推进了CV和LEV降解中间体及其可能的降解途径,利用毒性估计软件(T.E.S.T.)评估了LEV降解中间体的预测毒性,并通过培养稻的壮举进一步评价了光催化降解后CV、LEV和Cr(VI)溶液的生物毒性。通过一系列声音实验、fs-TA光谱、原位XPS和DFT计算等,证实了Ag/AgI/g-C3N4空心管S型异质结协同增强的光催化机理。
更新日期:2024-10-21
中文翻译:
等离激元和 N 空位协同增强管状氮化碳基 S 型异质结光催化剂,具有一石五鸟功能:途径、DFT 计算和机理洞察
从创新和广谱的角度出发,通过结合水热、煅烧和光还原技术,合理设计并制造了增强氮空位和局域表面等离子体共振 (LSPR) 效应的管状氮化碳基光催化剂,即 Ag/AgI/g-C3N4 S 型异质结光催化剂。最佳样品在去除染料[如结晶紫(CV),100.00 %/60 min]、抗生素[如左氧氟沙星(LEV),88.72 %/50 min]和Cr(VI)(100.00 %,30 min)、光催化析氢(1023.3 μmol h−1 g−1)和H2O2生成(866.2 μmol h−1 g−1)方面表现出较高的光催化活性,实现了广谱性质,即实现了“一石五鸟”的功能。广谱性质归因于氮空位、Ag 的 LSPR 效应、空心管结构和 S 型异质结的协同作用,它们促进了光生载流子的分离和迁移,并将 Ag 产生的“热电子”注入 Ag/AgI/g-C3N4 的导带,增加了比表面积并拓宽了光谱响应范围。此外,借助LCMS光谱合理推进了CV和LEV降解中间体及其可能的降解途径,利用毒性估计软件(T.E.S.T.)评估了LEV降解中间体的预测毒性,并通过培养稻的壮举进一步评价了光催化降解后CV、LEV和Cr(VI)溶液的生物毒性。通过一系列声音实验、fs-TA光谱、原位XPS和DFT计算等,证实了Ag/AgI/g-C3N4空心管S型异质结协同增强的光催化机理。