Li Wenpeng, Chen Yajie, Zhang Jiajia, Zeng Fanze, Bao Jinyu, Liu Lu, Tian Guohui
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin, 150080, P. R. China.
Small. 2024 Dec;20(49):e2406487. doi: 10.1002/smll.202406487. Epub 2024 Sep 11.
Constructing heterojunction photocatalysts with optimized architecture and components is an effective strategy for enhancing CO photoreduction by promoting photogenerated carrier separation, visible light absorption, and CO adsorption. Herein, defect-rich photocatalysts (NiP@Ce-BDC-CeO HOOs) with S-scheme heterojunction and hollowed-out octahedral architecture are prepared by decomposing Ce-BDC octahedrons embedded with NiP nanoparticles and subsequent lactic acid etching for CO photoreduction. The hollowed-out octahedral architecture with multistage pores (micropores, mesopores, and macropores) and oxygen vacancy defects are simultaneously produced during the preparation process. The S-scheme heterojunction boosts the quick transfer and separation of photoinduced charges. The formed hollowed-out multi-stage pore structure is favorable for the adsorption and diffusion of CO molecules and gaseous products. As expected, the optimized photocatalyst exhibits excellent performance, producing CO with a yield of 61.6 µmol h g, which is four times higher than that of the original Ce-BDC octahedrons. The X-ray photoelectron spectroscopy, scanning Kelvin probe, and electron spin resonance spectroscopy characterizations confirm the S-schematic charge-transfer route. The key intermediate species during the CO photoreduction process are detected by in situ Fourier transform infrared spectroscopy to support the proposed mechanism for CO photoreduction. This work presents a synthetic strategy for excellent catalysts with potential prospects in photocatalytic applications.
构建具有优化结构和组分的异质结光催化剂是通过促进光生载流子分离、可见光吸收和CO吸附来增强CO光还原的有效策略。在此,通过分解嵌入NiP纳米颗粒的Ce-BDC八面体并随后进行乳酸蚀刻以实现CO光还原,制备了具有S型异质结和中空八面体结构的富缺陷光催化剂(NiP@Ce-BDC-CeO HOOs)。在制备过程中同时产生了具有多级孔(微孔、介孔和大孔)和氧空位缺陷的中空八面体结构。S型异质结促进了光生电荷的快速转移和分离。形成的中空多级孔结构有利于CO分子和气态产物的吸附和扩散。正如预期的那样,优化后的光催化剂表现出优异的性能,CO产率为61.6 μmol h g,比原始的Ce-BDC八面体高出四倍。X射线光电子能谱、扫描开尔文探针和电子自旋共振光谱表征证实了S型电荷转移途径。通过原位傅里叶变换红外光谱检测CO光还原过程中的关键中间物种,以支持所提出的CO光还原机理。这项工作提出了一种合成策略,用于制备在光催化应用中具有潜在前景的优异催化剂。