TY - JOUR
T1 - Direct, nonoxidative conversion of methane to ethylene, aromatics, and hydrogen
AU - Guo, Xiaoguang
AU - Fang, Guangzong
AU - Li, Gang
AU - Ma, Hao
AU - Fan, Hongjun
AU - Yu, Liang
AU - Ma, Chao
AU - Wu, Xing
AU - Deng, Dehui
AU - Wei, Mingming
AU - Tan, Dali
AU - Si, Rui
AU - Zhang, Shuo
AU - Li, Jianqi
AU - Sun, Litao
AU - Tang, Zichao
AU - Pan, Xiulian
AU - Bao, Xinhe
PY - 2014
Y1 - 2014
N2 - The efficient use of natural gas will require catalysts that can activate the first C-H bond of methane while suppressing complete dehydrogenation and avoiding overoxidation. We report that single iron sites embedded in a silica matrix enable direct, nonoxidative conversion of methane, exclusively to ethylene and aromatics. The reaction is initiated by catalytic generation of methyl radicals, followed by a series of gas-phase reactions. The absence of adjacent iron sites prevents catalytic C-C coupling, further oligomerization, and hence, coke deposition. At 1363 kelvin, methane conversion reached a maximum at 48.1% and ethylene selectivity peaked at 48.4%, whereas the total hydrocarbon selectivity exceeded 99%, representing an atom-economical transformation process of methane. The lattice-confined single iron sites delivered stable performance, with no deactivation observed during a 60-hour test.
AB - The efficient use of natural gas will require catalysts that can activate the first C-H bond of methane while suppressing complete dehydrogenation and avoiding overoxidation. We report that single iron sites embedded in a silica matrix enable direct, nonoxidative conversion of methane, exclusively to ethylene and aromatics. The reaction is initiated by catalytic generation of methyl radicals, followed by a series of gas-phase reactions. The absence of adjacent iron sites prevents catalytic C-C coupling, further oligomerization, and hence, coke deposition. At 1363 kelvin, methane conversion reached a maximum at 48.1% and ethylene selectivity peaked at 48.4%, whereas the total hydrocarbon selectivity exceeded 99%, representing an atom-economical transformation process of methane. The lattice-confined single iron sites delivered stable performance, with no deactivation observed during a 60-hour test.
UR - https://www.scopus.com/pages/publications/84900318624
U2 - 10.1126/science.1253150
DO - 10.1126/science.1253150
M3 - 文章
AN - SCOPUS:84900318624
SN - 0036-8075
VL - 344
SP - 616
EP - 619
JO - Science
JF - Science
IS - 6184
ER -