Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′-Diimine Ligand

Handle URI:
http://hdl.handle.net/10754/622782
Title:
Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′-Diimine Ligand
Authors:
Guan, Chao; Zhang, Dandan; Pan, Yupeng; Iguchi, Masayuki; Ajitha, Manjaly John; Hu, Jinsong; Li, Huaifeng ( 0000-0001-9661-803X ) ; Yao, Changguang; Huang, Mei-Hui; Min, Shixiong ( 0000-0001-6248-8804 ) ; Zheng, Junrong; Himeda, Yuichiro; Kawanami, Hajime; Huang, Kuo-Wei ( 0000-0003-1900-2658 )
Abstract:
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 12000 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.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division
Citation:
Guan C, Zhang D-D, Pan Y, Iguchi M, Ajitha MJ, et al. (2017) Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′-Diimine Ligand. Inorganic Chemistry 56: 438–445. Available: http://dx.doi.org/10.1021/acs.inorgchem.6b02334.
Publisher:
American Chemical Society (ACS)
Journal:
Inorganic Chemistry
Issue Date:
17-Dec-2016
DOI:
10.1021/acs.inorgchem.6b02334
Type:
Article
ISSN:
0020-1669; 1520-510X
Sponsors:
This work was supported by King Abdullah University of Science and Technology (KAUST). We thank Carolyn E. Unck for assistance with the manuscript preparation.
Is Supplemented By:
Guan, C., Zhang, D.-D., Pan, Y., Iguchi, M., Ajitha, M. J., Hu, J., … Huang, K.-W. (2017). CCDC 1530235: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1ncbfs; DOI:10.5517/ccdc.csd.cc1ncbfs; HANDLE:http://hdl.handle.net/10754/624600
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/acs.inorgchem.6b02334
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorGuan, Chaoen
dc.contributor.authorZhang, Dandanen
dc.contributor.authorPan, Yupengen
dc.contributor.authorIguchi, Masayukien
dc.contributor.authorAjitha, Manjaly Johnen
dc.contributor.authorHu, Jinsongen
dc.contributor.authorLi, Huaifengen
dc.contributor.authorYao, Changguangen
dc.contributor.authorHuang, Mei-Huien
dc.contributor.authorMin, Shixiongen
dc.contributor.authorZheng, Junrongen
dc.contributor.authorHimeda, Yuichiroen
dc.contributor.authorKawanami, Hajimeen
dc.contributor.authorHuang, Kuo-Weien
dc.date.accessioned2017-01-29T13:51:39Z-
dc.date.available2017-01-29T13:51:39Z-
dc.date.issued2016-12-17en
dc.identifier.citationGuan C, Zhang D-D, Pan Y, Iguchi M, Ajitha MJ, et al. (2017) Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′-Diimine Ligand. Inorganic Chemistry 56: 438–445. Available: http://dx.doi.org/10.1021/acs.inorgchem.6b02334.en
dc.identifier.issn0020-1669en
dc.identifier.issn1520-510Xen
dc.identifier.doi10.1021/acs.inorgchem.6b02334en
dc.identifier.urihttp://hdl.handle.net/10754/622782-
dc.description.abstractWe 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 12000 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.en
dc.description.sponsorshipThis work was supported by King Abdullah University of Science and Technology (KAUST). We thank Carolyn E. Unck for assistance with the manuscript preparation.en
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/acs.inorgchem.6b02334en
dc.titleDehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′-Diimine Liganden
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalInorganic Chemistryen
dc.contributor.institutionNational Institute of Advanced Industrial Science and Technology, 4-2-1 Nigatake, Miyagino-ku, Sendai, Miyagi, 983-8551, Japanen
dc.contributor.institutionCollege of Chemistry, Peking University, Beijing, 100871, Chinaen
dc.contributor.institutionNational Institute of Advanced Industrial Science and Technology, 1-1-1 Higashi, Tsukuba-shi, Ibaraki, 305-8565, Japanen
kaust.authorGuan, Chaoen
kaust.authorZhang, Dandanen
kaust.authorPan, Yupengen
kaust.authorAjitha, Manjaly Johnen
kaust.authorHu, Jinsongen
kaust.authorLi, Huaifengen
kaust.authorYao, Changguangen
kaust.authorHuang, Mei-Huien
kaust.authorMin, Shixiongen
kaust.authorHuang, Kuo-Weien
dc.relation.isSupplementedByGuan, C., Zhang, D.-D., Pan, Y., Iguchi, M., Ajitha, M. J., Hu, J., … Huang, K.-W. (2017). CCDC 1530235: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1ncbfsen
dc.relation.isSupplementedByDOI:10.5517/ccdc.csd.cc1ncbfsen
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624600en
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