Carbon Nitride-Based Ruthenium Single Atom Photocatalyst for CO2 Reduction to Methanol

被引:149
|
作者
Sharma, Priti [1 ]
Kumar, Subodh [1 ]
Tomanec, Ondrej [1 ]
Petr, Martin [1 ]
Zhu Chen, Johnny [2 ]
Miller, Jeffrey T. [2 ]
Varma, Rajender S. [1 ]
Gawande, Manoj B. [1 ,3 ]
Zboril, Radek [1 ,4 ]
机构
[1] Palacky Univ, Czech Adv Technol & Res Inst, Reg Ctr Adv Technol & Mat, Olomouc 77900, Czech Republic
[2] Purdue Univ, Davidson Sch Chem Engn, 480 Stadium Mall Dr, W Lafayette, IN 47907 USA
[3] Inst Chem Technol, Dept Ind & Engn Chem, Mumbai Marathwada Campus, Jalna 431213, Maharashtra, India
[4] VSB Tech Univ Ostrava, Nanotechnol Ctr, CEET, 17 Listopadu 2172-15, Ostrava 70800, Czech Republic
关键词
carbon nitride; photocatalytic reduction of carbon dioxide; photocatalysts; single atom; HETEROGENEOUS CATALYSIS; EFFICIENT CATALYSTS; CHARGE-TRANSFER; DIOXIDE; LIGHT; CONVERSION; G-C3N4; HYDROGENATION; NANOPARTICLES; HYDROXIDE;
D O I
10.1002/smll.202006478
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
With increasing concerns for global warming, the solar-driven photocatalytic reduction of CO2 into chemical fuels like methanol is a propitious route to enrich energy supplies, with concomitant reduction of the abundant CO2 stockpiles. Herein, a novel single atom-confinement and a strategy are reported toward single ruthenium atoms dispersion over porous carbon nitride surface. Ruthenium single atom character is well confirmed by EXAFS absorption spectrometric analysis unveiling the cationic coordination environment for the single-atomic-site ruthenium center, that is formed by Ru-N/C intercalation in the first coordination shell, attaining synergism in N-Ru-N connection and interfacial carrier transfer. From time resolved fluorescence decay spectra, the average carrier lifetime of the RuSA-mC(3)N(4) system is found to be higher compared to m-C3N4; the fact uncovering the crucial role of single Ru atoms in promoting photocatalytic reaction system. A high yield of methanol (1500 mu mol g(-1) cat. after 6 h of the reaction) using water as an electron donor and the reusability of the developed catalyst without any significant change in the efficiency represent the superior aspects for its potential application in real industrial technologies.
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页数:7
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