Abstract Although both the aerobic photocatalytic oxidation of organic pollutants into CO2 and the anaerobic photocatalytic reduction of CO2 into solar fuels have been intensively studied, few efforts have been devoted to combining these carbon-involved photocatalytic oxidation-reduction processes together, by which an artificial photocatalytic carbon cycling process can be established. The key challenge lies in the exploitation of efficient bifunctional photocatalysts, capable of triggering both aerobic oxidation and anaerobic reduction reactions. In this work, a bifunctional ternary g-C3N4/Bi/BiVO4 hybrid photocatalyst is successfully constructed, which not only demonstrates superior aerobic photocatalytic oxidation performance in degrading an organic pollutant (using the dye, Rhodamine B as a model), but also exhibits impressive photocatalytic CO2 reduction performance under anaerobic conditions. Moreover, a direct conversion of Rhodamine B to solar fuels in a one-pot anaerobic reactor can be achieved with the as-prepared ternary g-C3N4/Bi/BiVO4 hybrid photocatalyst. The excellent bifunctional photocatalytic performance of the g-C3N4/Bi/BiVO4 photocatalyst is associated with the formation of efficient S-scheme hybrid junctions, which contribute to promoting the appropriate charge dynamics, and sustaining favorable charge potentials. The formation of the S-scheme heterojunction is supported by scavenger studies and density functional theory calculations. Moreover, the in-situ formed plasmonic metallic Bi nanoparticles in the S-scheme hybrid g-C3N4/Bi/BiVO4 photocatalyst enhances vectorial interfacial electron transfer. This novel bifunctional S-scheme g-C3N4/Bi/BiVO4 hybrid photocatalyst system provides new insights for the further development of an integrated aerobic-anaerobic reaction system for photocatalytic carbon cycling.

中文翻译：

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双功能 S 型 g-C3N4/Bi/BiVO4 杂化光催化剂用于人工碳循环

摘要 虽然有机污染物的好氧光催化氧化为 CO2 和 CO2 的厌氧光催化还原为太阳能燃料已经得到深入研究，但很少有人致力于将这些涉及碳的光催化氧化还原过程结合在一起，通过人工光催化可以建立碳循环过程。关键挑战在于开发高效的双功能光催化剂，能够触发有氧氧化和厌氧还原反应。在这项工作中，成功构建了双功能三元 g-C3N4/Bi/BiVO4 杂化光催化剂，它不仅在降解有机污染物方面表现出优异的好氧光催化氧化性能（以染料罗丹明 B 为模型），但在厌氧条件下也表现出令人印象深刻的光催化 CO2 还原性能。此外，利用所制备的三元 g-C3N4/Bi/BiVO4 杂化光催化剂，可以在一锅式厌氧反应器中将罗丹明 B 直接转化为太阳能燃料。g-C3N4/Bi/BiVO4 光催化剂优异的双功能光催化性能与有效 S 型混合结的形成有关，这有助于促进适当的电荷动力学，并维持有利的电荷电位。S 型异质结的形成得到清道夫研究和密度泛函理论计算的支持。此外，在 S 型杂化 g-C3N4/Bi/BiVO4 光催化剂中原位形成的等离子体金属 Bi 纳米颗粒增强了矢量界面电子转移。