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修饰NADH模拟物的金属-有机三元环光催化制氢 被引量:1
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作者 赵亮 楚少帅 +3 位作者 蔡俊凯 魏建伟 李亚楠 段春迎 《无机化学学报》 SCIE CAS CSCD 北大核心 2021年第5期769-777,共9页
将含有不同还原型烟酰烟腺嘌呤二核苷酸(NADH)活性中心模拟物的有机配体H_(2)L^(1)和H_(2)L^(2)与钴离子配位自组装获得2例具有氧化还原活性且带有正电荷的金属-有机大环Co-L^(1)和Co-L^(2)。选择阴离子型钌基光敏剂[Ru(dcbpy)_(3)]^(4-... 将含有不同还原型烟酰烟腺嘌呤二核苷酸(NADH)活性中心模拟物的有机配体H_(2)L^(1)和H_(2)L^(2)与钴离子配位自组装获得2例具有氧化还原活性且带有正电荷的金属-有机大环Co-L^(1)和Co-L^(2)。选择阴离子型钌基光敏剂[Ru(dcbpy)_(3)]^(4-)(dcbpy=2,2′-联吡啶-4,4′-二羧酸)作为光敏中心,金属-有机大环结构作为质子还原催化剂,通过静电作用力将光敏中心封装在其空腔内部以加速光诱导电子转移(PET)过程,构建了人工光合成体系并应用于光解水制氢研究。相比于未修饰NADH模拟物的金属-有机大环Co-L^(3)以及未修饰NADH模拟物但配位环境相同的单核催化剂Co-L^(4),由Co-L^(1)和Co-L^(2)构建的金属-有机大环主客体超分子体系的光催化产氢效率分别提高1.6和6倍,可能是由于NADH活性中心模拟物的引入以及主客体超分子体系的形成有利于光敏中心与催化中心之间的光致电子转移过程。 展开更多
关键词 金属-有机大环 NADH模拟物 -客体复合物 光诱导电子转移 光催化制氢
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Transition metal-nitrogen sites for electrochemical carbon dioxide reduction reaction 被引量:4
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作者 Chengcheng Yan Long Lin +1 位作者 Guoxiong Wang Xinhe Bao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第1期23-37,共15页
Electrochemical CO2 reduction reaction(CO2RR)powered by renewable electricity has emerged as the most promising technique for CO2 conversion,making it possible to realize a carbon‐neutral cycle.Highly efficient,robus... Electrochemical CO2 reduction reaction(CO2RR)powered by renewable electricity has emerged as the most promising technique for CO2 conversion,making it possible to realize a carbon‐neutral cycle.Highly efficient,robust,and cost‐effective catalysts are highly demanded for the near‐future practical applications of CO2RR.Previous studies on atomically dispersed metal‐nitrogen(M‐Nx)sites constituted of earth abundant elements with maximum atom‐utilization efficiency have demonstrated their performance towards CO2RR.This review summarizes recent advances on a variety of M‐Nx sites‐containing transition metal‐centered macrocyclic complexes,metal organic frameworks,and M‐Nx‐doped carbon materials for efficient CO2RR,including both experimental and theoretical studies.The roles of metal centers,coordinated ligands,and conductive supports on the intrinsic activity and selectivity,together with the importance of reaction conditions for improved performance are discussed.The mechanisms of CO2RR over these M‐Nx‐containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO2RR. 展开更多
关键词 Electrochemical carbon dioxide reduction reaction Metal‐nitrogen sites Metal‐nitrogen containing macrocyclic complexes Metal organic frameworks Zeolitic imidazolate frameworks Carbon material doped with metal‐nitrogen sites
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