Base-free hydrogenation of CO2 to formic acid in water with an iridium complex bearing a N, N '-diimine ligand
文献类型：期刊论文
| 作者 | Lu, Sheng-Mei2; Wang, Zhijun1,2,3; Li, Jun2; Xiao, Jianliang1; Li, Can2 |
| 刊名 | GREEN CHEMISTRY
 |
| 出版日期 | 2016 |
| 卷号 | 18期号:16页码:4553-4558 |
| ISSN号 | 1463-9262 |
| DOI | 10.1039/c6gc00856a |
| 文献子类 | Article |
| 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 |
| 语种 | 英语 |
| WOS记录号 | WOS:000381440800019 |
| 出版者 | ROYAL SOC CHEMISTRY |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/170292]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Li, Can |
| 作者单位 | 1.Univ Liverpool, Dept Chem, Liverpool Ctr Mat & Catalysis, Liverpool L69 7ZD, Merseyside, England 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, 457 Zhongshan Rd, Dalian 116023, Peoples R China 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. |
入库方式： OAI收割
来源：大连化学物理研究所
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