摘要
合理利用Z型电荷调节机制是提高光催化CO_(2)还原效率的有效策略.在本工作中,通过将AgVO_(3)量子点(QDs)原位锚定在TiO_(2)纳米片(NSs)上,从而构建了0D/2D AgVO_(3)/TiO_(2)直接Z型异质结光催化剂.TiO_(2)NSs抑制了AgVO_(3)量子点自身的团聚,从而优化了体系的形貌结构.AgVO_(3)QDs增强了复合材料的光吸收能力,从而提高了对太阳光的利用效率.同时,两种单体之间匹配的能带结构和合适的内部界面电场(即(-)AgVO_(3)/(+)TiO_(2))促进了直接Z型异质结的构建,从而显著促进了光生电子-空穴对的分离,并保持了体系中最高的氧化还原电位.优化后的AgVO_(3)/TiO_(2)复合材料在没有任何助催化剂的情况下,表现出具有竞争力的光催化CO_(2)还原效率(CO,47.61μmol h-1g-1),是原始TiO_(2)NSs的20.97倍.本工作提出了一种直接Z型异质结的合理设计方法,为高效光催化CO_(2)还原催化剂的开发提供了指导.
Rationally utilizing Z-scheme charge-regulated mechanisms is an effective strategy to improve photocatalytic CO_(2) reduction efficiency.Herein,AgVO_(3) quantum dots(QDs)are in-situ anchored on TiO_(2) nanosheets(NSs)to construct a 0D/2D AgVO_(3)/TiO_(2) direct Z-scheme heterojunction(DZH).TiO_(2) NSs prevent the self-aggregation of AgVO_(3) QDs,thereby optimizing the morphological structure of the system.AgVO_(3) QDs enhance the optical absorption capacity of the nanohy-brids,thus improving the efficiency of sunlight utilization.Meanwhile,matched energy band structures and the suitable internal interfacial electric field(-)AgVO_(3)/(+)TiO_(2) facilitate the construction of a DZH,significantly boosting the separa-tion of photogenerated electron-hole pairs and maintaining the highest redox potential in the system.The optimized AgVO_(3)/TiO_(2) nanohybrid exhibits competitive photocatalytic CO_(2) reduction efficiency(47.61μmol h-1 g-1 for CO),without any cocatalyst,which is 20.97 times higher than pristine TiO_(2) NSs.This work presents a rational design for a DZH and guides efficient photocatalytic CO_(2) reduction catalyst ex-ploration.
作者
王鋙葶
蒋娟
姚楠
左淦丞
朱文磊
郭秀云
鲜啟鸣
Yuting Wang;Juan Jiang;Nan Yao;Gancheng Zuo;Wenlei Zhu;Xiuyun Guo;Qiming Xian(State Key Laboratory of Pollution Control and Resource Reuse,School of the Environment,Nanjing University,Nanjing 210023,China;Jiangsu Engineering Lab of Water and Soil Eco-Remediation,School of Environment,Nanjing Normal University,Nanjing 210023,China;Key Laboratory of Chinese Cuisine Intangible Cultural Heritage Technology Inheritance,School of Tourism and Cuisine,Yangzhou University,Yangzhou 225127,China)
基金
supported by the National Natural Science Foundation of China (22106072 and 42177356)
the Fundamental Research Funds for the Central Universities (2022300301)
the Natural Science Research Major Project of Jiangsu Higher Education Institutions of China (22KJA610003)
the State Key Laboratory of Pollution Control and Resource Reuse Foundation (PCRRF21032)
the Open Fund of Key Laboratory of Green Chemical Technology of Fujian Province University (WYKFGCT2022-3)
China Postdoctoral Science Foundation (2022M721555)
Jiangsu Funding Program for Excellent Postdoctoral Talent (2023ZB081)。
作者简介
Yuting Wang received her PhD degree in environmental science engineering in 2022 from Nanjing University.Currently,she is a postdoctoral fellow at Nanjing Uni-versity.Her research interests are the synthesis of ad-vanced catalysts for photocatalytic CO_(2) reduction,pollutant degradation,and water splitting,contributed equally to this work;Juan Jiang,contributed equally to this work;Corresponding authors:Gancheng Zuo is an associate professor at the School of Environment,Nanjing Normal University.He received his BS degree in applied chemistry in 2013 from Nanjing University and his PhD degree in chemical engineering and technology in 2020 from Nanjing University of Science and Technology.His current research focuses on functional nanomaterials for energy conversion and pollutant removal.emails:zuogc@njnu.edu.cn;Corresponding authors:Wenlei Zhu is a professor at the School of the Environ-ment,Nanjing University.He obtained his BS and PhD degrees from Nanjing University and Brown University,respectively,followed by postdoctoral experiences at Wa-shington University,Columbia University and University of Delaware for several years.His current research interest focuses on the resource utilization of greenhouse gases.emails:wenleizhu@nju.edu.cn;Corresponding authors:Qiming Xian received his BS in organic chemistry in 1988 from Wuhan University and his PhD in environmental chemistry in 2005 from Nanjing University.Now,he is a professor at Nanjing University.He has long been engaged in the analysis methods of organic pollutants in environ-mental media,environmental behavior and trend,gen-eration mechanism of drinking water disinfection byproducts and health risks,and nanostructured materials for environmental and energy-related applications.emails:xianqm@nju.edu.cn。
