Tian Jiaqi, Zhang Yangyang, Shi Zuhao, Liu Zhongyi, Zhao Zaiwang, Li Jun, Li Neng, Huang Hongwei
Henan Institute of Advanced Technology, College of Chemistry, Zhengzhou University, Zhengzhou, 450052, P.R. China.
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan, 430070, P.R. China.
Angew Chem Int Ed Engl. 2025 Feb 3;64(6):e202418496. doi: 10.1002/anie.202418496. Epub 2024 Nov 16.
Photocatalytic CO reduction serves as an important technology for value-added solar fuel production, however, it is generally limited by interfacial charge transport. To address this limitation, a two-dimensional/two-dimensional (2D/2D) p-n heterojunction CuS-BiWO (CS-BWO) with highly connected and matched interfacial lattices was designed in this work via a two-step hydrothermal tandem synthesis strategy. The integration of CuS with BWO created a robust interface electric field and provided fast charge transfer channels due to the work function difference, as well as highly connected and matched interfacial lattices. The p-n heterojunction combination promoted the electron transfer from the Cu to Bi sites, leading to the coordination of Bi sites with high electronic density and low oxidation state. The Bi sites in the BWO nanosheets facilitated the adsorption and activation of CO, and the generation of high-coverage key intermediate b-CO , while CuS (CS) acted as a broad light-harvesting material to provide abundant photoinduced electrons that were injected into the conduction band of BWO for CO photoreduction reaction. Remarkably, the p-n heterojunction CS-BWO exhibited average CO and CH yields of 33.9 and 16.4 μmol g h, respectively, which were significantly higher than those of CS, BWO, and physical mixture CS-BWO samples. This work provided an innovative design strategy for developing high-activity heterojunction photocatalyst for converting CO into value-added solar fuels.
光催化CO还原是生产增值太阳能燃料的一项重要技术,然而,它通常受到界面电荷传输的限制。为了解决这一限制,本工作通过两步水热串联合成策略设计了一种具有高度连通和匹配界面晶格的二维/二维(2D/2D)p-n异质结CuS-BiWO(CS-BWO)。CuS与BWO的整合产生了强大的界面电场,并由于功函数差异提供了快速电荷转移通道,以及高度连通和匹配的界面晶格。p-n异质结组合促进了电子从Cu位点向Bi位点的转移,导致Bi位点与高电子密度和低氧化态配位。BWO纳米片中的Bi位点促进了CO的吸附和活化,以及高覆盖度关键中间体b-CO的生成,而CuS(CS)作为一种宽光谱光捕获材料,提供了丰富的光生电子,这些电子注入到BWO的导带中用于CO光还原反应。值得注意的是,p-n异质结CS-BWO的CO和CH平均产率分别为33.9和16.4 μmol g h,显著高于CS、BWO和物理混合物CS-BWO样品。这项工作为开发用于将CO转化为增值太阳能燃料的高活性异质结光催化剂提供了一种创新设计策略。