Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution

能源化学(英文版) ›› 2019, Vol. 39 ›› Issue (12): 244-248.

Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution

Yang Yu^a,b, Qijun Pei^a,b, Teng He^a, Ping Chen^a,c,d

a Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China;
c State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
d Collaborative Innovation Center of Chemistry for Energy Materials(iChEM·2011), Xiamen University, Xiamen 361005, Fujian, China

收稿日期:2019-02-20 修回日期:2019-04-05 出版日期:2019-12-15 发布日期:2020-12-18
通讯作者: Teng He, heteng@dicp.ac.cn
基金资助:
The author acknowledges financial support from the project of the National Natural Science Foundation of China (51671178, 21875246) and the project from DICP (DICP ZZBS201616). We would like to thank the support from Sino-Japanese Research Cooperative Program of Ministry of Science and Technology (2016YFE0118300) and iChEM·2011.

Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution

Yang Yu^a,b, Qijun Pei^a,b, Teng He^a, Ping Chen^a,c,d

a Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b University of Chinese Academy of Sciences, Beijing 100049, China;
c State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
d Collaborative Innovation Center of Chemistry for Energy Materials(iChEM·2011), Xiamen University, Xiamen 361005, Fujian, China

Received:2019-02-20 Revised:2019-04-05 Online:2019-12-15 Published:2020-12-18
Contact: Teng He, heteng@dicp.ac.cn
Supported by:
The author acknowledges financial support from the project of the National Natural Science Foundation of China (51671178, 21875246) and the project from DICP (DICP ZZBS201616). We would like to thank the support from Sino-Japanese Research Cooperative Program of Ministry of Science and Technology (2016YFE0118300) and iChEM·2011.

摘要/Abstract

摘要： With reduced dehydrogenation enthalpy change and reduced dehydrogenation temperature compared with its phenol-cyclohexanol pair, sodium phenoxide-cyclohexanolate pair developed recently is promising for large-scale energy storage and long-distance hydrogen transportation. In the present work, we investigate the kinetic behavior of the pair in the hydrogenation and dehydrogenation in water over three commercial catalysts. It is shown that 5% Ru/Al₂O₃ and 5% Pt/C perform well in the hydrogenation and dehydrogenation, respectively. Kinetic analyses show that the hydrogenation of sodium phenoxide is of first-order with respect to H₂ pressure and zero-order to the concentration of sodium phenoxide in the presence of Ru/Al₂O₃ catalyst.>99% conversion of cyclohexanol and>99% selectivity to phenoxide can be achieved in the dehydrogenation catalyzed by Pt/C catalyst and in the presence of NaOH at 100℃, where cyclohexanone was observed as an intermediate. According to the kinetic analysis, the hydrogenation of sodium phenoxide may undergo the hydrolysis and hydrogenation pathway. For the dehydrogenation, an intermediate, i.e., cyclohexanone, was detected and two possible pathways are proposed accordingly.

关键词: Hydrogen storage, Hydrogenation, Dehydrogenation, Sodium phenoxide, Kinetic analysis

Abstract: With reduced dehydrogenation enthalpy change and reduced dehydrogenation temperature compared with its phenol-cyclohexanol pair, sodium phenoxide-cyclohexanolate pair developed recently is promising for large-scale energy storage and long-distance hydrogen transportation. In the present work, we investigate the kinetic behavior of the pair in the hydrogenation and dehydrogenation in water over three commercial catalysts. It is shown that 5% Ru/Al₂O₃ and 5% Pt/C perform well in the hydrogenation and dehydrogenation, respectively. Kinetic analyses show that the hydrogenation of sodium phenoxide is of first-order with respect to H₂ pressure and zero-order to the concentration of sodium phenoxide in the presence of Ru/Al₂O₃ catalyst.>99% conversion of cyclohexanol and>99% selectivity to phenoxide can be achieved in the dehydrogenation catalyzed by Pt/C catalyst and in the presence of NaOH at 100℃, where cyclohexanone was observed as an intermediate. According to the kinetic analysis, the hydrogenation of sodium phenoxide may undergo the hydrolysis and hydrogenation pathway. For the dehydrogenation, an intermediate, i.e., cyclohexanone, was detected and two possible pathways are proposed accordingly.

Key words: Hydrogen storage, Hydrogenation, Dehydrogenation, Sodium phenoxide, Kinetic analysis

Yang Yu, Qijun Pei, Teng He, Ping Chen. Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution[J]. 能源化学(英文版), 2019, 39(12): 244-248.

Yang Yu, Qijun Pei, Teng He, Ping Chen. Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution[J]. Journal of Energy Chemistry, 2019, 39(12): 244-248.

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Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution

Kinetic studies of reversible hydrogen storage over sodium phenoxide-cyclohexanolate pair in aqueous solution

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