Xiao Yi, Tao Xueqin, Qiu Ganhua, Dai Zhifeng, Gao Peng, Li Benxia
Department of Chemistry, College of Science, Zhejiang Sci-Tech University, Hangzhou 310018, China.
College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou, Zhejiang 310026, China.
J Colloid Interface Sci. 2019 Aug 15;550:99-109. doi: 10.1016/j.jcis.2019.04.081. Epub 2019 Apr 29.
Constructing Z-scheme photocatalysts is an effective approach to enhance the conversion efficiency of solar to chemical energy. Herein, WO/g-CN heterostructures have been synthesized by growing WO ultrathin nanowires on g-CN nanosheets via a convenient solvothermal process. Various characterizations were performed on the materials to understand the structure-performance relationship. The photocatalytic properties of the WO/g-CN heterostructures were evaluated by the two oxidation reactions, phenol degradation and oxidative NC coupling of benzylamines, under a simulated sunlight (360 ≤ λ ≤ 780 nm). With tuning the WO/g-CN mass ratio, the optimal photocatalyst of WO(30)/g-CN containing 30 wt% WO nanowires exhibited the highest activity in both the photocatalytic reactions. The generations and contributions of the active species in the photocatalytic reactions were identified by electron spin resonance (ESR) spectra and active-species-eliminating experiments. Accordingly, the photocatalytic mechanism of WO/g-CN heterostructures has been expounded based on the direct Z-scheme electron transfer between the two semiconductors as well as the synergistic actions of active sites on WO nanowires and g-CN nanosheets. This work demonstrates a rational paradigm to construct 1D/2D semiconductor heterostructures and provides further insights into Z-scheme photocatalytic mechanism for boosting solar-driven pollutant degradation and organic transformation.
构建Z型光催化剂是提高太阳能向化学能转化效率的有效途径。在此,通过简便的溶剂热法在g-CN纳米片上生长WO超薄纳米线,合成了WO/g-CN异质结构。对材料进行了各种表征,以了解其结构-性能关系。在模拟太阳光(360≤λ≤780nm)下,通过苯酚降解和苄胺氧化偶联这两个氧化反应,评估了WO/g-CN异质结构的光催化性能。通过调节WO/g-CN的质量比,含有30wt%WO纳米线的WO(30)/g-CN最佳光催化剂在这两个光催化反应中均表现出最高活性。通过电子自旋共振(ESR)光谱和活性物种消除实验,确定了光催化反应中活性物种的产生和贡献。据此,基于两种半导体之间的直接Z型电子转移以及WO纳米线和g-CN纳米片上活性位点的协同作用,阐述了WO/g-CN异质结构的光催化机理。这项工作展示了构建一维/二维半导体异质结构的合理范例,并为促进太阳能驱动的污染物降解和有机转化的Z型光催化机理提供了进一步的见解。