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

Chao Guan; Dandan Zhang; Yupeng Pan; Masayuki Iguchi; Manjaly John Ajitha; Jinsong Hu; Huaifeng Li; Changguang Yao; Mei-Hui Huang; Shixiong Min; Junrong Zheng; Yuichiro Himeda; Hajime Kawanami; Kuo-Wei Huang

doi:10.1021/acs.inorgchem.6b02334

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

Chao Guan, Dandan Zhang, Yupeng Pan, Masayuki Iguchi, Manjaly John Ajitha, Jinsong Hu, Huaifeng Li, Changguang Yao, Mei-Hui Huang, Shixiong Min, Junrong Zheng, Yuichiro Himeda, Hajime Kawanami, Kuo-Wei Huang

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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.

Original language	English (US)
Pages (from-to)	438-445
Number of pages	8
Journal	Inorganic Chemistry
Volume	56
Issue number	1
DOIs	https://doi.org/10.1021/acs.inorgchem.6b02334
State	Published - Dec 16 2016

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10.1021/acs.inorgchem.6b02334

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@article{40a0c616677d45e9a586aa40e5457679,

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

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.",

author = "Chao Guan and Dandan Zhang and Yupeng Pan and Masayuki Iguchi and Ajitha, {Manjaly John} and Jinsong Hu and Huaifeng Li and Changguang Yao and Mei-Hui Huang and Shixiong Min and Junrong Zheng and Yuichiro Himeda and Hajime Kawanami and Kuo-Wei Huang",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This work was supported by King Abdullah University of Science and Technology (KAUST). We thank Carolyn E. Unck for assistance with the manuscript preparation.",

year = "2016",

month = dec,

day = "16",

doi = "10.1021/acs.inorgchem.6b02334",

language = "English (US)",

volume = "56",

pages = "438--445",

journal = "Inorganic Chemistry",

issn = "0020-1669",

publisher = "American Chemical Society",

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T1 - Dehydrogenation of Formic Acid Catalyzed by a Ruthenium Complex with an N,N′-Diimine Ligand

AU - Guan, Chao

AU - Zhang, Dandan

AU - Pan, Yupeng

AU - Iguchi, Masayuki

AU - Ajitha, Manjaly John

AU - Hu, Jinsong

AU - Li, Huaifeng

AU - Yao, Changguang

AU - Huang, Mei-Hui

AU - Min, Shixiong

AU - Zheng, Junrong

AU - Himeda, Yuichiro

AU - Kawanami, Hajime

AU - Huang, Kuo-Wei

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: This work was supported by King Abdullah University of Science and Technology (KAUST). We thank Carolyn E. Unck for assistance with the manuscript preparation.

PY - 2016/12/16

Y1 - 2016/12/16

N2 - 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.

AB - 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.

UR - http://hdl.handle.net/10754/622782

UR - http://pubs.acs.org/doi/abs/10.1021/acs.inorgchem.6b02334

UR - http://www.scopus.com/inward/record.url?scp=85008929550&partnerID=8YFLogxK

U2 - 10.1021/acs.inorgchem.6b02334

DO - 10.1021/acs.inorgchem.6b02334

M3 - Article

C2 - 27983821

SN - 0020-1669

VL - 56

SP - 438

EP - 445

JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 1

ER -

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

Abstract

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CCDC 1530235: Experimental Crystal Structure Determination : chloro-[p-cymene]-(4,4',5,5'-tetrahydro-1H,1'H-2,2'-bi-imidazole)-ruthenium chloride

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

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Datasets

CCDC 1530235: Experimental Crystal Structure Determination : chloro-[p-cymene]-(4,4',5,5'-tetrahydro-1H,1'H-2,2'-bi-imidazole)-ruthenium chloride

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