文献类型：期刊文献

英文题名：Atomically Dispersed High-Density Al-N4 Sites in Porous Carbon for Efficient Photodriven CO2 Cycloaddition

作者：Yang, Qihao[1,2];Peng, Huaitao[1,3];Zhang, Qiuju[1,2];Qian, Xu[1,4];Chen, Xu[1,2];Tang, Xuan[5,6];Dai, Sheng[5,6];Zhao, Jiajun[7];Jiang, Kun[7];Yang, Qiu[8];Sun, Jian[9];Zhang, Linjuan[9];Zhang, Nian[10];Gao, Honglin[3];Lu, Zhiyi[1,2];Chen, Liang[1,2]

机构：[1]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Ningbo 315201, Peoples R China;[2]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[3]Yunnan Univ, Sch Mat & Energy, Natl Ctr Int Res Photoelect & Energy Mat, Yunnan Key Lab Micronano Mat & Technol, Kunming 650091, Yunnan, Peoples R China;[4]Univ Sci & Technol China, Hefei 230029, Peoples R China;[5]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Inst Fine Chem, Shanghai 200237, Peoples R China;[7]Shanghai Jiao Tong Univ, Sch Mech Engn, Interdisciplinary Sci Res Ctr, Inst Fuel Cells, Shanghai 200240, Peoples R China;[8]Ningbo New Mat Testing & Evaluat Ctr Co Ltd, Ningbo New Mat Innovat Ctr, East Dist Bldg 1 1,2660 Yongjiang Ave, Ningbo 315100, Peoples R China;[9]Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China;[10]Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China

年份：2021

卷号：33

期号：45

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20213810911382);WOS:【SCI-EXPANDED(收录号:WOS:000696905000001)】；

基金：Q. Y., H. P., and Q. Z. contributed equally to this work. This work was supported by the National Key Research and Development Program of China (2018YFB0704300), the National Natural Science Foundation of China (21803074, 51872306, and 21865039), the Science and Technology Innovation 2025 Program in Ningbo (2019B10046, 2020Z059, and 2020Z107), Hundred Talents Program in Chinese Academy of Sciences, the China Postdoctoral Science Foundation (2019M660146 and 2019M662127), the National Postdoctoral Program for Innovative Talents (BX20190340), Shanghai Rising-star Program (20QA1402400), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Feringa Nobel Prize Scientist Joint Research Center, Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21000000), K.C. Wong Education Foundation (GJTD-2018-10), Youth Innovation Promotion Association (201842), and Chinese Academy of Sciences.

语种：英文

外文关键词：carbon-based catalysts; CO; (2) cycloaddition; photodriven reactions; single-atom catalysis

摘要：Highly active catalysts that can directly utilize renewable energy (e.g., solar energy) are desirable for CO2 value-added processes. Herein, aiming at improving the efficiency of photodriven CO2 cycloaddition reactions, a catalyst composed of porous carbon nanosheets enriched with a high loading of atomically dispersed Al atoms (approximate to 14.4 wt%, corresponding to an atomic percent of approximate to 7.3%) coordinated with N (AlN4 motif, Al-N-C catalyst) via a versatile molecule-confined pyrolysis strategy is reported. The performance of the Al-N-C catalyst for catalytic CO2 cycloaddition under light irradiation (approximate to 95% conversion, reaction rate = 3.52 mmol g(-1) h(-1)) is significantly superior to that obtained under a thermal environment (approximate to 57% conversion, reaction rate = 2.11 mmol g(-1) h(-1)). Besides the efficient photothermal conversion induced by the carbon matrix, both experimental and theoretical analysis reveal that light irradiation favors the photogenerated electron transfer from the semiconductive Al-N-C catalyst to the epoxide reactant, facilitating the formation of a ring-opened intermediate through the rate-limiting step. This study not only provides an advanced Al-N-C catalyst for photodriven CO2 cycloaddition, but also furnishes new insight for the rational design of superior photocatalysts for diverse heterogeneous catalytic reactions in the future.