Metalloporphyrin-based covalent organic frameworks composed of the electron donor-acceptor dyads for visible-light-driven selective CO2reduction

被引:96
作者
Lv, Haowei [1 ]
Sa, Rongjian [2 ]
Li, Pengyue [1 ]
Yuan, Daqiang [1 ]
Wang, Xinchen [3 ]
Wang, Ruihu [1 ]
机构
[1] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China
[2] Minjiang Univ, Inst Oceanog, Ocean Coll, Fuzhou 350108, Peoples R China
[3] Fuzhou Univ, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
基金
中国国家自然科学基金;
关键词
covalent organic frameworks; photocatalysis; porous materials; CO(2)reduction; metalloporphyrin; CARBON-DIOXIDE; CO2; REDUCTION; ELECTROREDUCTION; PHOTOCATALYSTS; CENTERS;
D O I
10.1007/s11426-020-9801-3
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The visible-light-driven photocatalytic CO(2)reduction with high efficiency is highly desirable but challenging. Herein, we present porphyrin-tetraphenylethene-based covalent organic frameworks (MP-TPE-COF, where M=H-2, Co and Ni; TPE=4,4 ',4 '',4"'-(ethane-1,1,2,2-tetrayl) tetrabenzaldehyde; COF=covalent organic framework) as ideal platforms for understanding photocatalytic CO(2)reduction at molecular level. Experimental and theoretical investigations have demonstrated crucial roles of metalloporphyrin units in selective adsorption, activation and conversion of CO(2)as well as in the separation of charge carriers and electron transfer, thus allowing for flexible modulation of photocatalytic activity and selectivity. CoP-TPE-COF exhibits high CO evolution rate of 2,414 mu mol g(-1)h(-1)with the selectivity of 61% over H(2)generation under visible-light irradiation, while NiP-TPE-COF provides CO evolution rate of 525 mu mol g(-1)h(-1)and 93% selectivity with superior durability. Moreover, the photocatalytic system is feasible for the simulated flue gas, which provides CO evolution rate of 386 mu mol g(-1)h(-1)and selectivity of 77%. This work provides in-depth insight into the structure-activity relationships toward the activation and photoreduction of CO2.
引用
收藏
页码:1289 / 1294
页数:6
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