Ga-C_(3)N_(4)单原子催化剂高效光驱动CO_(2)环加成  

Integration of Atomically Dispersed Ga Sites with C_(3)N_(4)Nanosheets for Efficient Photo-driven CO_(2)Cycloaddition

作　　者：杨静怡 施思齐[1] 彭怀涛 杨其浩 陈亮[2] YANG Jingyi;SHI Siqi;PENG Huaitao;YANG Qihao;CHEN Liang(School of Material Science and Engineering,Shanghai University,Shanghai 200444,China;Ningbo Institute of Materials Technology and Engineering,Chinese Academy of Sciences,Ningbo 315201,China)

机构地区：[1]上海大学材料科学与工程学院,上海200444 [2]中国科学院宁波材料技术与工程研究所,宁波315201

出　　处：《高等学校化学学报》2022年第9期173-179,共7页Chemical Journal of Chinese Universities

基　　金：浙江省自然科学基金(批准号:LQ22B010005);宁波市自然科学基金(批准号:2021J202)资助。

摘　　要：通过配位锚定策略制备了一种高Ga单原子负载量(质量分数8.42%)的C_(3)N_(4)纳米片(Ga-C_(3)N_(4)),用于高效光驱动CO_(2)环加成反应.研究结果表明,Ga-C_(3)N_(4)中Ga单原子和均匀分布的N位点可分别作为Lewis酸/碱位点来活化环氧化合物和CO_(2).此外,Ga-C_(3)N_(4)具有优异的半导体特性,在光照下产生的光生电子可以显著加快环氧化合物的开环速率,即提升决速步骤的反应效率.通过多功能协同,Ga-C_(3)N_(4)在光照下实现了CO_(2)到环状碳酸酯的高效催化转化.A carbon nitride(C_(3)N_(4))-based catalyst featuring high density of atomically dispersed Ga species(mass fraction of 8.42%)was rationally fabricated(Ga-C_(3)N_(4)) based on a molecule-confined strategy for photo-driven cycloaddition of CO_(2) and epoxides.The atomically dispersed Ga sites and uniform N species in Ga-C_(3)N_(4) served as Lewis acid and Lewis base sites,respectively,cooperating together to promote the activation of substrates.Compared with the thermal-driven catalytic system,the light irradiation favors the photo-generated electron transfer from catalyst(i.e.,Ga-C_(3)N_(4)) to epoxides,facilitating the catalytic efficiency of ring-opening step(i.e.,rate-limiting step).As a result,Ga-C_(3)N_(4) exhibited superior catalytic performance towards the CO_(2) cycloaddition with epoxides under light irradiation.

关 键 词：单原子催化 光驱动 CO_(2)环加成 

分 类 号：O644[理学—物理化学]