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Base-free hydrogenation of co2 to formic acid in water with an iridium complex bearing a n, n '-diimine ligand
Lu, Sheng-Mei1; Wang, Zhijun1,2,3; Li, Jun1; Xiao, Jianliang2; Li, Can1
刊名Green chemistry
2016
卷号18期号:16页码:4553-4558
ISSN号1463-9262
DOI10.1039/c6gc00856a
通讯作者Li, can(canli@dicp.ac.cn)
英文摘要Hydrogenation of co2 to formic acid using homogeneous catalysts is an attractive approach for the conversion and utilization of co2. to date, the efficiency of this transformation in water without base remains rather low. herein, we describe a highly efficient iridium catalyst, [cp* ir(n, n')cl] cl (n, n' = 2,2'-bi-1,4,5,6-tetrahydropyrimidine), for the direct hydrogenation of co2 to formic acid in water in the absence of a base, achieving an initial tof of over 13 000 h(-1) at 80 degrees c and 5.0 mpa of h-2/co2 (1 : 1) and a ton of over 10 000 at 40 degrees c and 7.6 mpa. the in situ h-1 nmr and reaction kinetics studies show that the reaction is limited in terms of turnover by the co2 insertion step. the kinetic isotope effect (kie) study was applied to understand the effect of water on the reaction, and the inverse kie results imply that the dissociation of the water molecule from the aqua iridium complex affects the kinetics of the catalytic cycle. this work extends the ligand type of the catalyst for co2 hydrogenation and provides a new strategy for catalyst design.
WOS关键词HYPOXIA INDUCIBLE FACTOR ; CARBON-DIOXIDE ; HOMOGENEOUS HYDROGENATION ; CATALYTIC-HYDROGENATION ; AMBIENT CONDITIONS ; AQUEOUS-SOLUTION ; AQUA COMPLEXES ; RAW-MATERIAL ; VALUE CHAIN ; FORMATE
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
语种英语
出版者ROYAL SOC CHEMISTRY
WOS记录号WOS:000381440800019
内容类型期刊论文
URI标识http://www.corc.org.cn/handle/1471x/2374386
专题中国科学院大学
通讯作者Li, Can
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China
2.Univ Liverpool, Dept Chem, Liverpool Ctr Mat & Catalysis, Liverpool L69 7ZD, Merseyside, England
3.Chinese Acad Sci, Grad Univ, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714
Lu, Sheng-Mei,Wang, Zhijun,Li, Jun,et al. Base-free hydrogenation of co2 to formic acid in water with an iridium complex bearing a n, n '-diimine ligand[J]. Green chemistry,2016,18(16):4553-4558.
APA Lu, Sheng-Mei,Wang, Zhijun,Li, Jun,Xiao, Jianliang,&Li, Can.(2016).Base-free hydrogenation of co2 to formic acid in water with an iridium complex bearing a n, n '-diimine ligand.Green chemistry,18(16),4553-4558.
MLA Lu, Sheng-Mei,et al."Base-free hydrogenation of co2 to formic acid in water with an iridium complex bearing a n, n '-diimine ligand".Green chemistry 18.16(2016):4553-4558.
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