Direct Conversion of Ethane to Oxygenates, Ethylene, and Hydrogen in a Noncatalytic Biphasic Plasma Microreactor

被引:6
作者
Cameli, Fabio [1 ]
Dimitrakellis, Panagiotis [1 ,2 ]
Vlachos, Dionisios G. [1 ,2 ]
机构
[1] Univ Delaware, Dept Chem & Biomol Engn, Newark, DE 19716 USA
[2] Delaware Energy Inst DEI, RAPID Mfg Inst, Catalysis Ctr Energy Innovat, Newark, DE 19716 USA
关键词
Gas-to-liquid transformation; liquid fuels; hydrogen; electrification; modular reactors; nonthermal plasma; CARBON-DIOXIDE; CO2; WATER; DEHYDROGENATION; TEMPERATURES; OXIDATION; MEMBRANES; CATALYSTS; METHANE; HEXANE;
D O I
10.1021/acssuschemeng.3c01594
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Modular, biphasic plasma reactor enablesupgrading of underutilizedgas streams into liquid fuels and hydrogen for electrified and decentralizedchemical processing. We selectively upgrade ethane (C2H6) to ethanol(C2H5OH), methanol (CH3OH), and aceticacid (CH3COOH) in a catalyst-free, continuous, argon/waterbiphasic plasma microreactor. The water (H2O) evaporatesand electron- dissociates into OH center dot radicals. OH center dot recombineswith alkyl radicals, produced via electron dissociation of ethane,to generate the oxygenates that absorb into H2O. A plasma-assistedpath, reminiscent of the low-temperature thermocatalytic ethane steamreforming, leads to significant H-2 coproduction. The gaseousstream also comprises CO2 and C2H4. Up to 1.3 and 1 mu mol min(-1) of liquid C2H5OH and CH3OH are attained, respectively.Compared to CO2-assisted ethane plasma conversion, whichproduces many oxygenates with low selectivity, the carbon selectivitycan range from >70% C2H5OH, CH3OH,and CH3COOH to 60% C2H4. The lowcarbon footprint, electrified, modular, intensified process usinga reactive evaporation and separation plasma could pave the way forthe valorization of underutilized shale gas resources in remote areas.
引用
收藏
页码:8003 / 8008
页数:6
相关论文
共 40 条
[1]   Gas-to-liquids process using multi-phase flow, non-thermal plasma microreactor [J].
Agiral, Anil ;
Nozaki, Tomohiro ;
Nakase, Masahiko ;
Yuzawa, Shuhei ;
Okazaki, Ken ;
Gardeniers, J. G. E. .
CHEMICAL ENGINEERING JOURNAL, 2011, 167 (2-3) :560-566
[2]   Oxygenate Production from Plasma-Activated Reaction of CO2 and Ethane [J].
Biswas, Akash N. ;
Winter, Lea R. ;
Loenders, Bjoern ;
Xie, Zhenhua ;
Bogaerts, Annemie ;
Chen, Jingguang G. .
ACS ENERGY LETTERS, 2022, 7 (01) :236-241
[3]   Plasma Technology for CO2 Conversion: A Personal Perspective on Prospects and Gaps [J].
Bogaerts, Annemie ;
Centi, Gabriele .
FRONTIERS IN ENERGY RESEARCH, 2020, 8
[4]   Oxidized Derivatives of n-Hexane from a Water/Argon Continuous Flow Electrical Discharge Plasma Reactor [J].
Bresch, Stefan ;
Wandell, Robert ;
Wang, Huihui ;
Alabugin, Igor ;
Locke, Bruce R. .
PLASMA CHEMISTRY AND PLASMA PROCESSING, 2016, 36 (02) :553-584
[5]   Modular Plasma Microreactor for Intensified Hydrogen Peroxide Production [J].
Cameli, Fabio ;
Dimitrakellis, Panagiotis ;
Chen, Tai-Ying ;
Vlachos, Dionisios G. .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2022, 10 (05) :1829-1838
[6]   Microflow chemistry and its electrification for sustainable chemical manufacturing [J].
Chen, Tai-Ying ;
Hsiao, Yung Wei ;
Baker-Fales, Montgomery ;
Cameli, Fabio ;
Dimitrakellis, Panagiotis ;
Vlachos, Dionisios G. .
CHEMICAL SCIENCE, 2022, 13 (36) :10644-10685
[7]   Recent progress in heterogeneous metal and metal oxide catalysts for direct dehydrogenation of ethane and propane [J].
Dai, Yihu ;
Gao, Xing ;
Wang, Qiaojuan ;
Wan, Xiaoyue ;
Zhou, Chunmei ;
Yang, Yanhui .
CHEMICAL SOCIETY REVIEWS, 2021, 50 (09) :5590-5630
[8]   Exceeding Equilibrium CO2 Conversion by Plasma-Assisted Chemical Looping [J].
Delikonstantis, Evangelos ;
Scapinello, Marco ;
Singh, Varun ;
Poelman, Hilde ;
Montesano, Cesare ;
Martini, Luca Matteo ;
Tosi, Paolo ;
Marin, Guy B. ;
Van Geem, Kevin M. ;
Galvita, Vladimir V. ;
Stefanidis, Georgios D. .
ACS ENERGY LETTERS, 2022, 7 (06) :1896-1902
[9]   Nanosecond pulsed discharge-driven non-oxidative methane coupling in a plate-to-plate electrode configuration plasma reactor [J].
Delikonstantis, Evangelos ;
Scapinello, Marco ;
Van Geenhoven, Orelie ;
Stefanidis, Georgios D. .
CHEMICAL ENGINEERING JOURNAL, 2020, 380
[10]   Low energy cost conversion of methane to ethylene in a hybrid plasma-catalytic reactor system [J].
Delikonstantis, Evangelos ;
Scapinello, Marco ;
Stefanidis, Georgios D. .
FUEL PROCESSING TECHNOLOGY, 2018, 176 :33-42