Reversible Hydrogen Uptake/Release over a Sodium Phenoxide-Cyclohexanolate Pair

Yu, Yang; He, Teng; Wu, Anan; Pei, Qijun; Karkamkar, Abhijeet; Autrey, Tom; Chen, Ping

doi:10.1002/anie.201810945

Title: Reversible Hydrogen Uptake/Release over a Sodium Phenoxide-Cyclohexanolate Pair

Journal Article · Mon Dec 17 00:00:00 EST 2018 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201810945· OSTI ID:1506689

Yu, Yang ^[1]; He, Teng ^[2]; Wu, Anan ^[3]; Pei, Qijun ^[1]; Karkamkar, Abhijeet ^[4]; Autrey, Tom ^[4];

^[5]

Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 China; University of Chinese Academy of Sciences, Beijing 100049 China
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 China
Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 China
Pacific Northwest National Laboratory, Richland WA 99352 USA
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 China; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023 China; Collaborative Innovation Centre of Chemistry for Energy Materials (iChEM⋅2011), Xiamen University, Fujian 361005 China

Storing hydrogen reversibly in the mass-produced cycloalkane and arene pairs provides a solution to the large-scale energy storage and long-distance hydrogen transportation. Herein, a novel alkali modification strategy for the thermodynamic optimization of cycloalkane-arene pairs is proposed and demonstrated. Our calculations and thermodynamic measurements show that the Na modified phenol-cyclohexanol pair has a dehydrogenation enthalpy change of 52 kJ mol-1 H2 which is significantly reduced by ca. 16 kJ mol-1 H2 from that of the pristine pair. 3 equivalents of H2 can be reversibly stored in the sodium modified phenol-cyclohexanol pair in aqueous solution, where the hydrogenation can take place at ambient temperature and 2 bar hydrogen pressure in the presence of commercial catalysts and, more importantly, dehydrogenation can be accomplished with >99% selectivity to H2 at 100°C.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1506689

Report Number(s):: PNNL-SA-132154

Journal Information:: Angewandte Chemie (International Edition), Vol. 58, Issue 10; ISSN 1433-7851

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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