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Reversible hydrogen uptake/release over a sodium phenoxide-cyclohexanolate pair

文献类型:期刊论文

作者Yu, Yang1,2; He, Teng1; Wu, Anan3; Pei, Qijun1,2; Karkamkar, Abhijeet4; Autrey, Tom4; Chen, Ping1,5,6
刊名Angewandte chemie-international edition
出版日期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
DOI10.1002/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.
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
WOS类目Chemistry, Multidisciplinary
语种英语
WOS记录号WOS:000459709300024
出版者WILEY-V C H VERLAG GMBH
URI标识http://www.irgrid.ac.cn/handle/1471x/2372751
专题大连化学物理研究所
通讯作者He, Teng; Wu, Anan; Chen, Ping
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Xiamen Univ, Fujian Prov Key Lab Theoret & Computat Chem, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
4.Pacific Northwest Natl Lab, Richland, WA 99352 USA
5.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
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
Yu, Yang,He, Teng,Wu, Anan,et al. Reversible hydrogen uptake/release over a sodium phenoxide-cyclohexanolate pair[J]. Angewandte chemie-international edition,2019,58(10):3102-3107.
APA Yu, Yang.,He, Teng.,Wu, Anan.,Pei, Qijun.,Karkamkar, Abhijeet.,...&Chen, Ping.(2019).Reversible hydrogen uptake/release over a sodium phenoxide-cyclohexanolate pair.Angewandte chemie-international edition,58(10),3102-3107.
MLA Yu, Yang,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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来源:大连化学物理研究所

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