Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′‑Diimine Ligand
We report a ruthenium complex containing an N,N′-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any organic additives. A turnover frequency of 12 000 h–1 and a turnover number of 350 000 at 90 °C were achieved in the HCOOH/HCOONa aqueous soluti...
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| Published in | Inorganic chemistry Vol. 56; no. 1; pp. 438 - 445 |
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| Main Authors | , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
03.01.2017
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| Online Access | Get full text |
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| Abstract | We report a ruthenium complex containing an N,N′-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any organic additives. A turnover frequency of 12 000 h–1 and a turnover number of 350 000 at 90 °C were achieved in the HCOOH/HCOONa aqueous solution. Efficient production of high-pressure H2 and CO2 (24.0 MPa (3480 psi)) was achieved through the decomposition of formic acid with no formation of CO. Mechanistic studies by NMR and DFT calculations indicate that there may be two competitive pathways for the key hydride transfer rate-determining step in the catalytic process. |
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| AbstractList | We report a ruthenium complex containing an N,N'-diimine ligand for the selective decomposition of formic acid to H
and CO
in water in the absence of any organic additives. A turnover frequency of 12 000 h
and a turnover number of 350 000 at 90 °C were achieved in the HCOOH/HCOONa aqueous solution. Efficient production of high-pressure H
and CO
(24.0 MPa (3480 psi)) was achieved through the decomposition of formic acid with no formation of CO. Mechanistic studies by NMR and DFT calculations indicate that there may be two competitive pathways for the key hydride transfer rate-determining step in the catalytic process. We report a ruthenium complex containing an N,N'-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any organic additives. A turnover frequency of 12 000 h-1 and a turnover number of 350 000 at 90 °C were achieved in the HCOOH/HCOONa aqueous solution. Efficient production of high-pressure H2 and CO2 (24.0 MPa (3480 psi)) was achieved through the decomposition of formic acid with no formation of CO. Mechanistic studies by NMR and DFT calculations indicate that there may be two competitive pathways for the key hydride transfer rate-determining step in the catalytic process.We report a ruthenium complex containing an N,N'-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any organic additives. A turnover frequency of 12 000 h-1 and a turnover number of 350 000 at 90 °C were achieved in the HCOOH/HCOONa aqueous solution. Efficient production of high-pressure H2 and CO2 (24.0 MPa (3480 psi)) was achieved through the decomposition of formic acid with no formation of CO. Mechanistic studies by NMR and DFT calculations indicate that there may be two competitive pathways for the key hydride transfer rate-determining step in the catalytic process. We report a ruthenium complex containing an N,N′-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any organic additives. A turnover frequency of 12 000 h–1 and a turnover number of 350 000 at 90 °C were achieved in the HCOOH/HCOONa aqueous solution. Efficient production of high-pressure H2 and CO2 (24.0 MPa (3480 psi)) was achieved through the decomposition of formic acid with no formation of CO. Mechanistic studies by NMR and DFT calculations indicate that there may be two competitive pathways for the key hydride transfer rate-determining step in the catalytic process. |
| Author | Kawanami, Hajime Pan, Yupeng Hu, Jinsong Huang, Kuo-Wei Ajitha, Manjaly J Zheng, Junrong Iguchi, Masayuki Himeda, Yuichiro Min, Shixiong Yao, Changguang Zhang, Dan-Dan Li, Huaifeng Huang, Mei-Hui Guan, Chao |
| AuthorAffiliation | KAUST Catalysis Center and Division of Physical Sciences and Engineering College of Chemistry Peking University National Institute of Advanced Industrial Science and Technology |
| AuthorAffiliation_xml | – name: Peking University – name: KAUST Catalysis Center and Division of Physical Sciences and Engineering – name: National Institute of Advanced Industrial Science and Technology – name: College of Chemistry |
| Author_xml | – sequence: 1 givenname: Chao surname: Guan fullname: Guan, Chao – sequence: 2 givenname: Dan-Dan surname: Zhang fullname: Zhang, Dan-Dan – sequence: 3 givenname: Yupeng surname: Pan fullname: Pan, Yupeng – sequence: 4 givenname: Masayuki surname: Iguchi fullname: Iguchi, Masayuki – sequence: 5 givenname: Manjaly J surname: Ajitha fullname: Ajitha, Manjaly J – sequence: 6 givenname: Jinsong surname: Hu fullname: Hu, Jinsong – sequence: 7 givenname: Huaifeng surname: Li fullname: Li, Huaifeng – sequence: 8 givenname: Changguang surname: Yao fullname: Yao, Changguang – sequence: 9 givenname: Mei-Hui surname: Huang fullname: Huang, Mei-Hui – sequence: 10 givenname: Shixiong surname: Min fullname: Min, Shixiong – sequence: 11 givenname: Junrong surname: Zheng fullname: Zheng, Junrong – sequence: 12 givenname: Yuichiro surname: Himeda fullname: Himeda, Yuichiro – sequence: 13 givenname: Hajime surname: Kawanami fullname: Kawanami, Hajime – sequence: 14 givenname: Kuo-Wei orcidid: 0000-0003-1900-2658 surname: Huang fullname: Huang, Kuo-Wei email: hkw@kaust.edu.sa |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/27983821$$D View this record in MEDLINE/PubMed |
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| Snippet | We report a ruthenium complex containing an N,N′-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any... We report a ruthenium complex containing an N,N'-diimine ligand for the selective decomposition of formic acid to H and CO in water in the absence of any... We report a ruthenium complex containing an N,N'-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any... |
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| Title | Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′‑Diimine Ligand |
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