TY - JOUR
T1 - Long-Chain Hydrocarbons from Nonthermal Plasma-Driven Biogas Upcycling
AU - Knezevic, Josip
AU - Zhang, Tianqi
AU - Zhou, Renwu
AU - Hong, Jungmi
AU - Zhou, Rusen
AU - Barnett, Christopher
AU - Song, Qiang
AU - Gao, Yuting
AU - Xu, Wanping
AU - Liu, Dingxin
AU - Proschogo, Nicholas
AU - Mohanty, Biswaranjan
AU - Strachan, Jyah
AU - Soltani, Behdad
AU - Li, Fengwang
AU - Maschmeyer, Thomas
AU - Lovell, Emma C.
AU - Cullen, Patrick J.
N1 - Publisher Copyright:
© 2024 The Authors.
PY - 2024/5/8
Y1 - 2024/5/8
N2 - The burgeoning necessity to discover new methodologies for the synthesis of long-chain hydrocarbons and oxygenates, independent of traditional reliance on high-temperature, high-pressure, and fossil fuel-based carbon, is increasingly urgent. In this context, we introduce a nonthermal plasma-based strategy for the initiation and propagation of long-chain carbon growth from biogas constituents (CO2 and CH4). Utilizing a plasma reactor operating at atmospheric room temperature, our approach facilitates hydrocarbon chain growth up to C40 in the solid state (including oxygenated products), predominantly when CH4 exceeds CO2 in the feedstock. This synthesis is driven by the hydrogenation of CO2 and/or amalgamation of CHx radicals. Global plasma chemistry modeling underscores the pivotal role of electron temperature and CHx radical genesis, contingent upon varying CO2/CH4 ratios in the plasma system. Concomitant with long-chain hydrocarbon production, the system also yields gaseous products, primarily syngas (H2 and CO), as well as liquid-phase alcohols and acids. Our finding demonstrates the feasibility of atmospheric room-temperature synthesis of long-chain hydrocarbons, with the potential for tuning the chain length based on the feed gas composition.
AB - The burgeoning necessity to discover new methodologies for the synthesis of long-chain hydrocarbons and oxygenates, independent of traditional reliance on high-temperature, high-pressure, and fossil fuel-based carbon, is increasingly urgent. In this context, we introduce a nonthermal plasma-based strategy for the initiation and propagation of long-chain carbon growth from biogas constituents (CO2 and CH4). Utilizing a plasma reactor operating at atmospheric room temperature, our approach facilitates hydrocarbon chain growth up to C40 in the solid state (including oxygenated products), predominantly when CH4 exceeds CO2 in the feedstock. This synthesis is driven by the hydrogenation of CO2 and/or amalgamation of CHx radicals. Global plasma chemistry modeling underscores the pivotal role of electron temperature and CHx radical genesis, contingent upon varying CO2/CH4 ratios in the plasma system. Concomitant with long-chain hydrocarbon production, the system also yields gaseous products, primarily syngas (H2 and CO), as well as liquid-phase alcohols and acids. Our finding demonstrates the feasibility of atmospheric room-temperature synthesis of long-chain hydrocarbons, with the potential for tuning the chain length based on the feed gas composition.
UR - https://www.scopus.com/pages/publications/85192084298
U2 - 10.1021/JACS.4C01641
DO - 10.1021/JACS.4C01641
M3 - 文章
C2 - 38687243
AN - SCOPUS:85192084298
SN - 0002-7863
VL - 146
SP - 12601
EP - 12608
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 18
ER -