Reversible Hydrogen Uptake/Release over a Sodium Phenoxide-Cyclohexanolate Pair | |
Chen, Ping1,2,6; Yu, Yang2,3; He, Teng2; Wu, Anan4; Pei, Qijun2,3; Karkamkar, Abhijeet5; Autrey, Tom5 | |
刊名 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION |
2019-03-04 | |
卷号 | 58期号:10页码:3102-3107 |
关键词 | hydrogen storage materials metalation organic hydrides thermodynamic modification |
ISSN号 | 1433-7851 |
DOI | 10.1002/anie.201810945 |
通讯作者 | He, Teng(heteng@dicp.ac.cn) ; Wu, Anan(ananwu@xmu.edu.cn) ; Chen, Ping(pchen@dicp.ac.cn) |
英文摘要 | Hydrogen uptake and release in arene-cycloalkane pairs provide an attractive opportunity for on-board and off-board hydrogen storage. However, the efficiency of arene-cycloalkane pairs currently is limited by unfavorable thermodynamics for hydrogen release. It is shown here that the thermodynamics can be optimized by replacement of H in the -OH group of cyclohexanol and phenol with alkali or alkaline earth metals. The enthalpy change upon dehydrogenation decreases substantially, which correlates with the delocalization of the oxygen electron to the benzene ring in phenoxides. Theoretical calculations reveal that replacement of H with a metal leads to a reduction of the HOMO-LUMO energy gap and elongation of the C-H bond in the alpha site in cyclohexanolate, which indicates that the cyclohexanol is activated upon metal substitution. The experimental results demonstrate that sodium phenoxide-cyclohexanolate, an air- and water-stable pair, can desorb hydrogen at ca. 413 K and 373 K in the solid form and in an aqueous solution, respectively. Hydrogenation, on the other hand, is accomplished at temperatures as low as 303 K. |
资助项目 | National Natural Science Foundation of China[21875246] ; National Natural Science Foundation of China[51671178] ; National Natural Science Foundation of China[51472237] ; DICP[DICP ZZBS201616] ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology[2016YFE0118300] ; National Science Foundation of China (NSFC)[21773193] ; Fundamental Research Funds for the Central Universities[20720160031] ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; U.S. Department of Energy[DE-AC05-76RL01830] ; iChEM2011 |
WOS关键词 | ACCEPTORLESS DEHYDROGENATION ; NITROGEN-HETEROCYCLES ; CHEMICAL HYDRIDES ; STORAGE MATERIALS ; N-HETEROCYCLES ; SYSTEM ; DISSOCIATION ; PERFORMANCE ; CATALYSIS ; RELEASE |
WOS研究方向 | Chemistry |
语种 | 英语 |
出版者 | WILEY-V C H VERLAG GMBH |
WOS记录号 | WOS:000459709300024 |
资助机构 | National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; U.S. Department of Energy ; U.S. Department of Energy ; iChEM2011 ; iChEM2011 ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; U.S. Department of Energy ; U.S. Department of Energy ; iChEM2011 ; iChEM2011 ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; U.S. Department of Energy ; U.S. Department of Energy ; iChEM2011 ; iChEM2011 ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; DICP ; DICP ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; Sino-Japanese Research Cooperative Program of the Ministry of Science and Technology ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Fundamental Research Funds for the Central Universities ; Fundamental Research Funds for the Central Universities ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; Hydrogen Materials-Advanced Research Consortium (HyMARC), as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office ; U.S. Department of Energy ; U.S. Department of Energy ; iChEM2011 ; iChEM2011 |
内容类型 | 期刊论文 |
源URL | [http://cas-ir.dicp.ac.cn/handle/321008/165964] |
专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
通讯作者 | Chen, Ping; He, Teng; Wu, Anan |
作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Xiamen Univ, Fujian Prov Key Lab Theoret & Computat Chem, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China 5.Pacific Northwest Natl Lab, Richland, WA 99352 USA 6.Xiamen Univ, Collaborat Innovat Ctr Chem Energy Mat iChEM 2011, Xiamen 361005, Fujian, Peoples R China |
推荐引用方式 GB/T 7714 | Chen, Ping,Yu, Yang,He, Teng,et al. Reversible Hydrogen Uptake/Release over a Sodium Phenoxide-Cyclohexanolate Pair[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2019,58(10):3102-3107. |
APA | Chen, Ping.,Yu, Yang.,He, Teng.,Wu, Anan.,Pei, Qijun.,...&Autrey, Tom.(2019).Reversible Hydrogen Uptake/Release over a Sodium Phenoxide-Cyclohexanolate Pair.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,58(10),3102-3107. |
MLA | Chen, Ping,et al."Reversible Hydrogen Uptake/Release over a Sodium Phenoxide-Cyclohexanolate Pair".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 58.10(2019):3102-3107. |
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