Experimental and theoretical study on dissociation thermodynamics and kinetics of hydrogen-propane hydrate

Wang, Pengfei1,2,3,4; Li, Kehan5; Yang, Jianyu6; Zhu, Jinlong1,2,3,4; Zhao, Yusheng1,2,3,4; Teng, Ying7,8

2021-12-15

10.1016/j.cej.2021.131279

CHEMICAL ENGINEERING JOURNAL   影响因子和分区

1385-8947

1873-3212

Hydrate-based hydrogen storage is a promising technology in the clean energy field. In this study, propane was selected as the accelerator guest molecule for hydrogen storage in hydrates. Hydrogen-propane (0.67/0.33, mole ratio) hydrate dissociation properties are investigated by experiment and molecular dynamics simulation. The hydrogen-propane hydrate phase equilibrium is measured by different methods and the average dissociation heat is 77.03 J/g under 0.98-1.72 MPa. While hydrate dissociation heat flow curves show the characteristic of two-step dissociation, which is further confirmed via Raman spectroscopy. Simultaneously, hydrogen-propane hydrate dissociation driven by depressurization and heating are also investigated by Raman spectroscopy. During dissociation, the Raman peak area of hydrogen in hydrate continues to decrease, whereas it is relatively stable for propane before the hydrate dissociation complete. In addition, hydrogen-propane hydrate reformation occurs more intensely during the heating process, especially when the temperature exceeds 273 K than with depressurization. This indicates that depressurization is more feasible for continuous hydrogen releasing, a concept of recycling hydrate clathrate structure was proposed to shorten hydrate formation time and accelerates hydrogen storage rate. In addition, the molecular dynamics simulation results confirmed that the hydrogen release rate from hydrate is higher than that of propane from the microscopic view point. The results of this study provide a potential pathway of hydrogen storage using hydrates.

Gas hydrate Hydrogen storage Hydrate dissociation heat Two-step dissociation

EI ; SCI

英语

第一 ; 通讯

Shenzhen Clean Energy Research Institute[CERI-KY-2019-003] ; Shenzhen Key Laboratory of Natural Gas Hydrates[ZDSYS20200421111201738] ; Department of Science and Technology of Guangdong Province[2019ZT08G315] ; Guangdong Province Basic and Applied Basic Research Fund[2019A1515110855] ; Young Innovative Talents Project in Ordinary Universities in Guangdong Province[2019KQNCX134] ; China Postdoctoral Science Foundation["2019M662195","2019TQ0302"] ; National Natural Science Foundation of China[11775011]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:000724625700004

ELSEVIER SCIENCE SA

20212910660055

Gas hydrates ; Hydration ; Hydrogen storage ; Molecular dynamics ; Propane ; Raman spectroscopy ; Thermodynamics

Natural Gas Deposits:512.2 ; Gas Fuels:522 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Chemical Reactions:802.2

ENGINEERING

Web of Science

1.Southern Univ Sci & Technol, Acad Adv Interdisciplinary Studies, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Shenzhen Key Lab Nat Gas Hydrates, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
4.Southern Marine Sci & Engn Guangdong Lab Guangzho, Guangzhou 511458, Peoples R China
5.Dalian Univ Technol, Key Lab Ocean Energy Utilizat & Energy Conservat, Minist Educ, Dalian 116024, Peoples R China
6.Southern Univ Sci & Technol, Dept Ocean Sci & Engn, Shenzhen 518055, Peoples R China
7.Shenzhen Univ, Coll Civil & Transportat Engn, Inst Deep Earth Sci & Green Energy, Shenzhen Key Lab Deep Engn Sci & Green Energy, Shenzhen 518060, Peoples R China
8.Shenzhen Univ, Guangdong Prov Key Lab Deep Earth Sci & Geotherma, Shenzhen 518060, Peoples R China

Wang, Pengfei,Li, Kehan,Yang, Jianyu,et al. Experimental and theoretical study on dissociation thermodynamics and kinetics of hydrogen-propane hydrate[J]. CHEMICAL ENGINEERING JOURNAL,2021,426.

Wang, Pengfei,Li, Kehan,Yang, Jianyu,Zhu, Jinlong,Zhao, Yusheng,&Teng, Ying.(2021).Experimental and theoretical study on dissociation thermodynamics and kinetics of hydrogen-propane hydrate.CHEMICAL ENGINEERING JOURNAL,426.

Wang, Pengfei,et al."Experimental and theoretical study on dissociation thermodynamics and kinetics of hydrogen-propane hydrate".CHEMICAL ENGINEERING JOURNAL 426(2021).