Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals

Summary: Lead halide perovskites are prospective candidates for CO2 photoconversion. Herein, we report copper-doped lead-free Cs2AgSbCl6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO2 reduction. The 0.2Cu@Cs2AgSbCl6 double perovskite MCs display unprecedented CO2 photor...

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Main Authors: Daofu Wu, Xiaoqing Liu, Changqing Tian, Jinchen Zhou, Junan Lai, Hongmei Ran, Bo Gao, Miao Zhou, Qiang Huang, Xiaosheng Tang
Format: Article
Language:English
Published: Elsevier 2023-08-01
Series:iScience
Subjects:
Online Access:http://www.sciencedirect.com/science/article/pii/S2589004223014323
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author Daofu Wu
Xiaoqing Liu
Changqing Tian
Jinchen Zhou
Junan Lai
Hongmei Ran
Bo Gao
Miao Zhou
Qiang Huang
Xiaosheng Tang
author_facet Daofu Wu
Xiaoqing Liu
Changqing Tian
Jinchen Zhou
Junan Lai
Hongmei Ran
Bo Gao
Miao Zhou
Qiang Huang
Xiaosheng Tang
author_sort Daofu Wu
collection DOAJ
description Summary: Lead halide perovskites are prospective candidates for CO2 photoconversion. Herein, we report copper-doped lead-free Cs2AgSbCl6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO2 reduction. The 0.2Cu@Cs2AgSbCl6 double perovskite MCs display unprecedented CO2 photoreduction capability with CO and CH4 yields of 412 and 128 μmol g−1, respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs2AgSbCl6 MCs. The active sites and reaction intermediates on the surface of the doped Cs2AgSbCl6 are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs2AgSbCl6 MCs facilitate sturdy CO2 adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs2AgSbCl6 doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.
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spelling doaj.art-e3444ed633cf4a7f83f8906fb68554ea2023-07-19T04:23:54ZengElsevieriScience2589-00422023-08-01268107355Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystalsDaofu Wu0Xiaoqing Liu1Changqing Tian2Jinchen Zhou3Junan Lai4Hongmei Ran5Bo Gao6Miao Zhou7Qiang Huang8Xiaosheng Tang9Key Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, ChinaKey Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, ChinaCollege of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, ChinaCollege of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, ChinaKey Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, ChinaCollege of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, ChinaSchool of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, ChinaKey Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China; Corresponding authorCollege of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China; Corresponding authorKey Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China; College of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China; School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China; Corresponding authorSummary: Lead halide perovskites are prospective candidates for CO2 photoconversion. Herein, we report copper-doped lead-free Cs2AgSbCl6 double perovskite microcrystals (MCs) for gas-solid phase photocatalytic CO2 reduction. The 0.2Cu@Cs2AgSbCl6 double perovskite MCs display unprecedented CO2 photoreduction capability with CO and CH4 yields of 412 and 128 μmol g−1, respectively. The ultrafast transient absorption spectroscopy reveals the enhanced separation of photoexcited carriers in copper-doped Cs2AgSbCl6 MCs. The active sites and reaction intermediates on the surface of the doped Cs2AgSbCl6 are dynamically monitored and precisely unraveled based on the in-situ Fourier transform infrared spectroscopy investigation. In combination with density functional theory calculations, it is revealed that the copper-doped Cs2AgSbCl6 MCs facilitate sturdy CO2 adsorption and activation and strikingly enhance the photocatalytic performance. This work offers an in-depth interpretation of the photocatalytic mechanism of Cs2AgSbCl6 doped with copper, which may provide guidance for future design of high-performance photocatalysts for solar fuel production.http://www.sciencedirect.com/science/article/pii/S2589004223014323Optical materialsMaterials propertyChemical property
spellingShingle Daofu Wu
Xiaoqing Liu
Changqing Tian
Jinchen Zhou
Junan Lai
Hongmei Ran
Bo Gao
Miao Zhou
Qiang Huang
Xiaosheng Tang
Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals
iScience
Optical materials
Materials property
Chemical property
title Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals
title_full Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals
title_fullStr Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals
title_full_unstemmed Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals
title_short Enhanced photocatalytic activity and mechanism insight of copper-modulated lead-free Cs2AgSbCl6 double perovskite microcrystals
title_sort enhanced photocatalytic activity and mechanism insight of copper modulated lead free cs2agsbcl6 double perovskite microcrystals
topic Optical materials
Materials property
Chemical property
url http://www.sciencedirect.com/science/article/pii/S2589004223014323
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