摘要
设计与构建兼具高效光生载流子分离能力和强氧化/还原能力的双功能S型异质结光催化剂,在能源转换与环境净化的光催化应用中具有重要实践价值。本研究通过静电纺丝与水热法系统设计合成了一系列新型x%CoWO_(4)/CdIn_(2)S_(4)复合材料(x%代表CWO与CIS的质量比;x=10, 20, 30, 40, 50)。通过可见光下甲醛降解与产氢实验评估其光催化性能。最优的30%CWO/CIS异质结展现出865.14μmol g^(-1) h^(−1)的卓越产氢性能(420 nm处表观量子效率AQE=3.6%),并在1h内实现69%的甲醛去除率。基于原位红外光谱技术解析了甲醛降解路径。优异的催化性能主要归因于可见光吸收增强、活性位点数量增加及S型异质结的构建。通过原位XPS、电子自旋共振测试、自由基捕获实验及密度泛函理论(DFT)计算,证实了CWO/CIS体系的S型电荷转移机制。该研究为系统性开发兼具气体污染物去除与产氢功能的双功能S型异质结提供了重要见解。
Designing and establishing dual-functional S-scheme heterojunction photocatalysts with efficient separation of photoproduced carriers and intense oxidation/reduction capabilities holds immense practical value for their photocatalytic application in energy conversion and environmental purification.Herein,a novel series of x%CoWO_(4)/CdIn_(2)S_(4)(x%reflects the weight ratio of CWO to CIS;x=10,20,30,40 and 50)composites have been systematically designed and synthesized via electrospinning technique and hydrothermal methods.Their photocatalytic properties were assessed through HCHO removal and H_(2) generation under visible light.As anticipated,the optimized 30%CWO/CIS heterojunction presented an outstanding H_(2) generation performance of 865.14μmol g^(-1) h^(−1) with AQE=3.6%atλ=420 nm,and achieved a 69%removal percentage for HCHO within 1 h.Meanwhile,the pathway of HCHO degradation was presented based on in situ diffuse reflectance infrared Fourier transform spectroscopy(in situ DRIFTS)technique.The great catalytic performance was primarily ascribed to the enhancement in the visible-light absorption,number of active sites,and the construction of S-scheme heterojunction.Furthermore,the S-scheme charge transfer mechanism for the CWO/CIS catalyst system has been confirmed by in situ X-ray photoelectron spectroscopy(in situ XPS),electron spin resonance data,radical capturing experiments,and density functional theory(DFT)calculations.This research contributes valuable understanding for the systematic design and development of bifunctional S-scheme heterojunctions for gaseous pollutants removal and H_(2) production.
作者
陈成鑫
石洪飞
蔡晓燕
毛梁
陈哲
Chengxin Chen;Hongfei Shi;Xiaoyan Cai;Liang Mao;Zhe Chen(Institute of Petrochemical Technology,Jilin University of Chemical Technology,Jilin,132022,Jilin Province,China;School of Materials Science and Physics,China University of Mining and Technology,Xuzhou,221116,Jiangsu Province,China;Caparol Hangzhou Ltd.,Hangzhou,311200,Zhejiang Province,China)
出处
《物理化学学报》
北大核心
2025年第12期84-98,共15页
Acta Physico-Chimica Sinica
基金
国家自然科学基金(22309061,22209203,22309204,22278172)
吉林省教育厅项目(JJKH20240305KJ)
吉林省科学技术厅项目(YDZJ202401372ZYTS)资助。
