Hydrogen Production via Aqueous-Phase Reforming of Ethanol Catalyzed by Ruthenium Alkylidene Complexes

Wang，Qian1; Xia，Yihao1; Chen，Zhijian1; Wang，Yifan1; Cheng，Fanrui1; Qin，Lei1; Zheng，Zhiping1,2

2022-04-25

10.1021/acs.organomet.1c00555

ORGANOMETALLICS   影响因子和分区

0276-7333

1520-6041

A series of ruthenium alkylidene complexes were adopted to catalyze aqueous-phase reforming of ethanol for Hproduction at readily achievable temperatures (<100 °C). The best results were obtained using (SIMes)Ru(PCy)(3-methyl-2-butenylidene)Cl(SIMes, 1,3-bis(2,4,6-trimethylphenyl)-4,5-dihydroimidazol-2-ylidene; PCy, tricyclohexylphosphine) with a five-day reaction producing a maximum turnover number (TON) of 47,295; this value is the second-largest one known for homogeneously catalyzed ethanol dehydrogenation. Kinetic experiments confirmed that the reforming process undergoes a second-order reaction kinetics, with both ethanol and water contributing to Hproduction. Analyses of the reaction mixture using an in situ H NMR experiment revealed a possible intermediate coordinated with a hydride ligand, based on which and previous work a plausible mechanism was proposed.

SCI ; EI

英语

第一

SUSTech["Y01216127","Y01216227"] ; Distinguished Expert Fund from Nanshan District of Shenzhen[K19219502] ; Basic and Applied Basic Research Programs of Guangdong Province[2020A1515110990] ; Jilin Provincial Science Research Foundation of China[20200403154SF] ; Special Funds for the Cultivation of Guangdong College Students' Scientific and Technological Innovation ("Climbing Program" Special Funds)[pdjh2020c0034] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; Shenzhen Nobel Prize Scientists Laboratory Project (Shenzhen Grubbs Institute)[C17783101] ; Post-doctorate Scientific Research Fund for stay at Shenzhen[K21217515]

Chemistry

Chemistry, Inorganic & Nuclear ; Chemistry, Organic

WOS:000795504700002

AMER CHEMICAL SOC

20221612006560

Catalysis ; Coordination reactions ; Hydrogen production ; Nuclear magnetic resonance spectroscopy ; Reaction intermediates ; Reaction kinetics ; Ruthenium compounds

Gas Fuels:522 ; Chemical Reactions:802.2 ; Chemical Products Generally:804 ; Organic Compounds:804.1

CHEMISTRY

2-s2.0-85128383994

Scopus

1.Department of Chemistry,Southern University of Science and Technology,Shenzhen,Guangdong,518055,China
2.Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis,Southern University of Science and Technology,Shenzhen,518055,China

Wang，Qian,Xia，Yihao,Chen，Zhijian,et al. Hydrogen Production via Aqueous-Phase Reforming of Ethanol Catalyzed by Ruthenium Alkylidene Complexes[J]. ORGANOMETALLICS,2022,41(8):914-919.

Wang，Qian.,Xia，Yihao.,Chen，Zhijian.,Wang，Yifan.,Cheng，Fanrui.,...&Zheng，Zhiping.(2022).Hydrogen Production via Aqueous-Phase Reforming of Ethanol Catalyzed by Ruthenium Alkylidene Complexes.ORGANOMETALLICS,41(8),914-919.

Wang，Qian,et al."Hydrogen Production via Aqueous-Phase Reforming of Ethanol Catalyzed by Ruthenium Alkylidene Complexes".ORGANOMETALLICS 41.8(2022):914-919.