Efficient co-upcycling of glycerol and CO2 into valuable products enabled by a bifunctional Ru-complex catalyst

被引:2
作者
Cui, Tianhua [1 ]
Gong, Huihua [2 ]
Ji, Li [3 ]
Mao, Jiawei [4 ]
Xue, Weichao [1 ]
Zheng, Xueli [1 ]
Fu, Haiyan [1 ]
Chen, Hua [1 ]
Li, Ruixiang [1 ]
Xu, Jiaqi [1 ,5 ]
机构
[1] Sichuan Univ, Coll Chem, Key Lab Green Chem & Technol, Minist Educ, Chengdu 610064, Sichuan, Peoples R China
[2] Neijiang Normal Univ, Coll Chem & Chem Engn, Analyt & Testing Ctr, Neijiang 641112, Peoples R China
[3] Sichuan Res Inst Chem Qual & Safety Testing, Chengdu 610031, Sichuan, Peoples R China
[4] Sichuan Inst Prod Qual Supervis & Inspect, Chengdu 610100, Sichuan, Peoples R China
[5] Ecole Polytech Fed Lausanne, Lab Photon & Interfaces, CH-1015 Lausanne, Switzerland
基金
中国国家自然科学基金;
关键词
CARBON-DIOXIDE; TRANSFER HYDROGENATION; CONVERSION; METHANOL; DEHYDROGENATION; FORMATE;
D O I
10.1039/d4cc02436b
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Glycerol and CO2 are largely produced as by-products in modern industry. Herein, three Ru complexes bearing air- and water-stable NHC-nitrogen-nitrogen ligands are designed as bifunctional catalysts to upcycle glycerol and CO2 simultaneously. Among them, Ru complex 2 featuring an N-H structure shows the highest efficiency with TONs up to 300 000 and 387 000 for formate and lactate, respectively. C-13 labelling experiments clearly manifest that formate is primarily derived from CO2. Furthermore, in situ FTIR spectra suggest that glyceraldehyde from glycerol might serve as a key intermediate to form lactate, while DFT calculations indicate that Ru complex 2 possesses the lowest reaction barriers and can form the Ru = N intermediate, contributing to its higher activity.
引用
收藏
页码:12221 / 12224
页数:4
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