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Highly efficient photoelectrocatalytic oxidation of arsenic(III) with a polyoxometalate-thiacalix[4]arene-based metal–organic complex-modified bismuth vanadate photoanode
Green Chemistry ( IF 9.3 ) Pub Date : 2024-02-22 , DOI: 10.1039/d3gc04755e Yuting Song 1 , Jia-Yi Zhang 1 , Jin Yang 1 , Tao Bo 2 , Jian-Fang Ma 1
Green Chemistry ( IF 9.3 ) Pub Date : 2024-02-22 , DOI: 10.1039/d3gc04755e Yuting Song 1 , Jia-Yi Zhang 1 , Jin Yang 1 , Tao Bo 2 , Jian-Fang Ma 1
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The development of highly efficient and environment friendly methods for arsenic pollution treatment has attracted special attention. Herein, a new polyoxometalate-thiacalix[4]arene-based metal–organic complex [Ag2L(HL)][PW12O40]·2C2H5OH·2CH3CN (1) (L = thiacalix[4]arene-based ligand) was synthesized and applied for BiVO4 (BVO) surface modification to efficiently enhance the simulated sunlight-driven photoelectrocatalytic oxidation of arsenic(III). Compared with the pristine BVO, the removal efficiency of arsenic(III) was drastically increased to 312% at 0.6 V with the optimized 1@BVO photoanode (B1-20) versus the saturated calomel electrode (SCE) under the simulated sunlight (100 mW cm−2). The removal efficiency of arsenic(III) (25 mg L−1) with B1-20 was up to 100% within 40 min with a faradaic efficiency of 45%. More importantly, electron spin resonance measurements and reactive species trapping experiments demonstrated that the Z-scheme heterojunction formation of 1 plays a key role in the enhanced photoelectrocatalytic performance of 1@BVO. Furthermore, density functional theory (DFT) calculations were used to investigate the relationship between the photoelectrocatalytic properties and the structure of 1. This work developed a new photoelectrocatalytic application for the polyoxometalate-thiacalix[4]arene-based metal–organic complexes by their efficient combination with BVO.
中文翻译：
多金属氧酸盐-硫杂杯[4]芳烃基金属有机配合物修饰钒酸铋光阳极高效光电催化氧化砷(III)
开发高效、环境友好的砷污染处理方法引起了特别关注。本文中，一种新的多金属氧酸盐-thiacalix[4]芳烃基金属有机配合物[Ag 2 L(HL)][PW 12 O 40 ]·2C 2 H 5 OH·2CH 3 CN ( 1 ) (L = thiacalix[4合成了基于芳烃的配体，并将其应用于BiVO 4 ( BVO )表面修饰，以有效增强模拟太阳光驱动的砷( III )光电催化氧化。与原始BVO相比，在模拟太阳光（100 mW）下，优化的1@BVO光阳极（B1-20）与饱和甘汞电极（SCE）相比，在0.6 V电压下砷（ III ）的去除效率大幅提高至312％厘米-2）。B1-20对砷( III )(25 mg·L -1 )的去除效率在40 min内达到100%，法拉第效率为45%。更重要的是，电子自旋共振测量和活性物质捕获实验表明，1的Z型异质结的形成在增强1@BVO的光电催化性能方面发挥着关键作用。此外，使用密度泛函理论（DFT）计算来研究光电催化性能与1的结构之间的关系。这项工作通过与BVO 的有效结合，开发了多金属氧酸盐-硫杂环[4]芳烃基金属有机配合物的新光电催化应用。
更新日期：2024-02-22
中文翻译：
多金属氧酸盐-硫杂杯[4]芳烃基金属有机配合物修饰钒酸铋光阳极高效光电催化氧化砷(III)
开发高效、环境友好的砷污染处理方法引起了特别关注。本文中，一种新的多金属氧酸盐-thiacalix[4]芳烃基金属有机配合物[Ag 2 L(HL)][PW 12 O 40 ]·2C 2 H 5 OH·2CH 3 CN ( 1 ) (L = thiacalix[4合成了基于芳烃的配体，并将其应用于BiVO 4 ( BVO )表面修饰，以有效增强模拟太阳光驱动的砷( III )光电催化氧化。与原始BVO相比，在模拟太阳光（100 mW）下，优化的1@BVO光阳极（B1-20）与饱和甘汞电极（SCE）相比，在0.6 V电压下砷（ III ）的去除效率大幅提高至312％厘米-2）。B1-20对砷( III )(25 mg·L -1 )的去除效率在40 min内达到100%，法拉第效率为45%。更重要的是，电子自旋共振测量和活性物质捕获实验表明，1的Z型异质结的形成在增强1@BVO的光电催化性能方面发挥着关键作用。此外，使用密度泛函理论（DFT）计算来研究光电催化性能与1的结构之间的关系。这项工作通过与BVO 的有效结合，开发了多金属氧酸盐-硫杂环[4]芳烃基金属有机配合物的新光电催化应用。
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