Efficient and Reversible Catalysis of Formic Acid-Carbon Dioxide Cycle Using Carbamate-Substituted Ruthenium-Dithiolate Complexes

Hui Min Tsai; Wan Hsiang Lien; Chi Hsuan Liao; Yi Ting Chen; Sheng Cih Huang; Feng Pai Chou; Chin-Yuan Chang; Jen-Shiang K. Yu; Ya-Ting Kao; Tung-Kung Wu

doi:10.1002/cctc.202100730

Efficient and Reversible Catalysis of Formic Acid-Carbon Dioxide Cycle Using Carbamate-Substituted Ruthenium-Dithiolate Complexes

Hui Min Tsai, Wan Hsiang Lien, Chi Hsuan Liao, Yi Ting Chen, Sheng Cih Huang, Feng Pai Chou, Chin-Yuan Chang, Jen-Shiang K. Yu, Ya-Ting Kao, Tung-Kung Wu^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

It is important to develop viable technologies for efficient hydrogen (H₂) production and carbon dioxide (CO₂) conversion to realize the future supply of clean energy and reduction of global CO₂ concentration. Herein, we report a series of carbamate-substituted ruthenium-dithiolate complexes 1–3, [Ru_x(CO)_y(μ-SCH(NCO₂(C(CH₃)₃))CH₂CH₂S)] (x=2, 3, 6 and y=6, 9, 20), which can effectively catalyze the reversible formic acid-carbon dioxide (FA-CO₂/H₂) cycle that can be used to convert CO₂ and produce H₂. Complex 2 effectively dehydrogenates FA to produce H₂ with an unprecedented turnover frequency (TOF) of 1.15×10⁶ h⁻¹ under conditions of sunlight irradiation. Under conditions of high temperature and pressure, complex 3 hydrogenates CO₂ to FA with a high initial TOF of 1.02×10⁶ h⁻¹, resulting in an efficient FA-CO₂/H₂ cycle. These results can potentially help provide the platform for the development of technologies that can be used in future to produce clean energy and control environmental threats.

Original language	American English
Pages (from-to)	4092-4098
Number of pages	7
Journal	ChemCatChem
Volume	13
Issue number	19
DOIs	https://doi.org/10.1002/cctc.202100730
State	Published - 7 Oct 2021

Keywords

Carbon dioxide
Carbon neutral cycle
Catalysis
Hydrogen
Ruthenium H-cluster
Solar energy

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title = "Efficient and Reversible Catalysis of Formic Acid-Carbon Dioxide Cycle Using Carbamate-Substituted Ruthenium-Dithiolate Complexes",

abstract = "It is important to develop viable technologies for efficient hydrogen (H2) production and carbon dioxide (CO2) conversion to realize the future supply of clean energy and reduction of global CO2 concentration. Herein, we report a series of carbamate-substituted ruthenium-dithiolate complexes 1–3, [Rux(CO)y(μ-SCH(NCO2(C(CH3)3))CH2CH2S)] (x=2, 3, 6 and y=6, 9, 20), which can effectively catalyze the reversible formic acid-carbon dioxide (FA-CO2/H2) cycle that can be used to convert CO2 and produce H2. Complex 2 effectively dehydrogenates FA to produce H2 with an unprecedented turnover frequency (TOF) of 1.15×106 h−1 under conditions of sunlight irradiation. Under conditions of high temperature and pressure, complex 3 hydrogenates CO2 to FA with a high initial TOF of 1.02×106 h−1, resulting in an efficient FA-CO2/H2 cycle. These results can potentially help provide the platform for the development of technologies that can be used in future to produce clean energy and control environmental threats.",

keywords = "Carbon dioxide, Carbon neutral cycle, Catalysis, Hydrogen, Ruthenium H-cluster, Solar energy",

author = "Tsai, {Hui Min} and Lien, {Wan Hsiang} and Liao, {Chi Hsuan} and Chen, {Yi Ting} and Huang, {Sheng Cih} and Chou, {Feng Pai} and Chin-Yuan Chang and Yu, {Jen-Shiang K.} and Ya-Ting Kao and Tung-Kung Wu",

note = "Funding Information: We thank the Ministry of Science and Technology, Taiwan (Contract #: MOST 107‐2113‐M‐009‐009, MOST 108‐2113‐M‐009‐009, MOST 110‐2634‐F‐009‐026), the Center for Emergent Functional Matter Science, and the Center for Intelligent Drug Systems and Smart Bio‐devices (IDSB) of the National Yang Ming Chiao Tung University from The Featured Areas Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education in Taiwan. We are grateful to Prof. Chien‐Chung Cheng, Prof. Hsiu‐Fu Hsu, Prof. Lan‐Chang Liang and Prof. Ting‐Yu Lee for their help. 2 Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2021",

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doi = "10.1002/cctc.202100730",

language = "American English",

volume = "13",

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T1 - Efficient and Reversible Catalysis of Formic Acid-Carbon Dioxide Cycle Using Carbamate-Substituted Ruthenium-Dithiolate Complexes

AU - Tsai, Hui Min

AU - Lien, Wan Hsiang

AU - Liao, Chi Hsuan

AU - Chen, Yi Ting

AU - Huang, Sheng Cih

AU - Chou, Feng Pai

AU - Chang, Chin-Yuan

AU - Yu, Jen-Shiang K.

AU - Kao, Ya-Ting

AU - Wu, Tung-Kung

N1 - Funding Information: We thank the Ministry of Science and Technology, Taiwan (Contract #: MOST 107‐2113‐M‐009‐009, MOST 108‐2113‐M‐009‐009, MOST 110‐2634‐F‐009‐026), the Center for Emergent Functional Matter Science, and the Center for Intelligent Drug Systems and Smart Bio‐devices (IDSB) of the National Yang Ming Chiao Tung University from The Featured Areas Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education in Taiwan. We are grateful to Prof. Chien‐Chung Cheng, Prof. Hsiu‐Fu Hsu, Prof. Lan‐Chang Liang and Prof. Ting‐Yu Lee for their help. 2 Publisher Copyright: © 2021 Wiley-VCH GmbH

PY - 2021/10/7

Y1 - 2021/10/7

N2 - It is important to develop viable technologies for efficient hydrogen (H2) production and carbon dioxide (CO2) conversion to realize the future supply of clean energy and reduction of global CO2 concentration. Herein, we report a series of carbamate-substituted ruthenium-dithiolate complexes 1–3, [Rux(CO)y(μ-SCH(NCO2(C(CH3)3))CH2CH2S)] (x=2, 3, 6 and y=6, 9, 20), which can effectively catalyze the reversible formic acid-carbon dioxide (FA-CO2/H2) cycle that can be used to convert CO2 and produce H2. Complex 2 effectively dehydrogenates FA to produce H2 with an unprecedented turnover frequency (TOF) of 1.15×106 h−1 under conditions of sunlight irradiation. Under conditions of high temperature and pressure, complex 3 hydrogenates CO2 to FA with a high initial TOF of 1.02×106 h−1, resulting in an efficient FA-CO2/H2 cycle. These results can potentially help provide the platform for the development of technologies that can be used in future to produce clean energy and control environmental threats.

AB - It is important to develop viable technologies for efficient hydrogen (H2) production and carbon dioxide (CO2) conversion to realize the future supply of clean energy and reduction of global CO2 concentration. Herein, we report a series of carbamate-substituted ruthenium-dithiolate complexes 1–3, [Rux(CO)y(μ-SCH(NCO2(C(CH3)3))CH2CH2S)] (x=2, 3, 6 and y=6, 9, 20), which can effectively catalyze the reversible formic acid-carbon dioxide (FA-CO2/H2) cycle that can be used to convert CO2 and produce H2. Complex 2 effectively dehydrogenates FA to produce H2 with an unprecedented turnover frequency (TOF) of 1.15×106 h−1 under conditions of sunlight irradiation. Under conditions of high temperature and pressure, complex 3 hydrogenates CO2 to FA with a high initial TOF of 1.02×106 h−1, resulting in an efficient FA-CO2/H2 cycle. These results can potentially help provide the platform for the development of technologies that can be used in future to produce clean energy and control environmental threats.

KW - Carbon dioxide

KW - Carbon neutral cycle

KW - Catalysis

KW - Hydrogen

KW - Ruthenium H-cluster

KW - Solar energy

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U2 - 10.1002/cctc.202100730

DO - 10.1002/cctc.202100730

M3 - Article

AN - SCOPUS:85112781067

SN - 1867-3880

VL - 13

SP - 4092

EP - 4098

JO - ChemCatChem

JF - ChemCatChem

IS - 19

ER -

Efficient and Reversible Catalysis of Formic Acid-Carbon Dioxide Cycle Using Carbamate-Substituted Ruthenium-Dithiolate Complexes

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Keywords

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