Mechanism and Kinetics of Methane Oxidation to Methanol Catalyzed by AuPd Nanocatalysts at Low Temperature

Rui  Serra-Maia; F. Marc  Michel; Temple A.  Douglas; Yijin  Kang; Eric A.  Stach

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Mechanism and Kinetics of Methane Oxidation to Methanol Catalyzed by AuPd Nanocatalysts at Low Temperature

机译：低温Aupd纳米催化剂催化甲烷氧化机理和动力学

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The selective oxidation of methane to methanol at ambient conditions has the potential to enable the use of natural gas obtained in remote areas. We performed multivariate statistical analysis of 137 laboratory experiments to show that gold–palladium nanocatalysts unlock the reaction pathway that forms methanol, but the overall rate of methane oxidation does not correlate with the total number of active sites because the catalyst does not participate in the rate limiting step of the reaction. Using an H_(2)O_(2) concentration below 2.5 × 10~(–5) mol/L reduces the H_(2)O_(2) overuse up to 10,000 times and promotes a methanol selectivity greater than 0.8 without compromising the reaction productivity. These results have enormous practical importance for methane utilization because they explain the poor methane conversion rates obtained thus far and show the path to increase the methanol productivity and reduce the overuse of industrially expensive H_(2)O_(2).

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《ACS catalysis》 |2021年第5期|共9页
作者
Rui Serra-Maia; F. Marc Michel; Temple A. Douglas; Yijin Kang; Eric A. Stach;
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作者单位

Department of Materials Sciences Engineering University of Pennsylvania;

Department of Geosciences Virginia Polytechnic Institute and State University;

Pathology and Laboratory Science Perelman School of Medicine University of Pennsylvania;

Institute for Sustainability and Energy Northwestern University;

Department of Materials Sciences Engineering University of Pennsylvania;

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正文语种 eng
中图分类物理化学（理论化学）、化学物理学;
关键词
methanol; methane oxidation; AuPd nanocatalysts; selectivity; productivity; energy conversion;

机译：甲醇;甲烷氧化;AUPD纳米催化剂;选择性;生产率;能量转换;

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2. A simple kinetic model for oxidative coupling of methane over La0.6Sr0.4Co0.8Fe0.2O3-δ nanocatalyst [J] . Ali Farsi, Sattar Ghader, Ali Moradi, 天然气化学（英文版） . 2011,第003期
3. Kinetics and Mechanism Modeling of Liquid-Phase Toluene Oxidation to Benzaldehyde Catalyzed by Mn-Mo Oxide [J] . Wang Li, Qingjun Zhang, Aiwu Zeng 天津大学学报（英文版） . 2019,第001期
4. The kinetic studies of direct methane oxidation to methanol in the plasma process [J] . INDARTO Antonius, CHOI Jae-Wook, LEE Hwaung, 中国科学通报：英文版 . 2008,第018期
5. Decomposition of Hydrogen Peroxide Catalyzed by AuPd Nanocatalysts during Methane Oxidation to Methanol [J] . Serra-Maia Rui, Michel F. Marc, Kang Yijin, ACS catalysis . 2020,第9期

机译：Aupd纳米催化剂在甲醇氧化过程中催化的过氧化氢的分解
6. Ultra-low temperature carbon (di)oxide hydrogenation catalyzed by hybrid ruthenium-nickel nanocatalysts: towards sustainable methane production [J] . Green chemistry . 2020,第15期

机译：杂交钌 - 镍纳催化剂催化的超低温度碳（DI）氧化氢：促进可持续甲烷生产
7. Comparative study of Co-rich and Ce-rich oxide nanocatalysts (CoxCe1-xOy) for low-temperature total oxidation of methanol [J] . Dziembaj R., Chojnacka A., Piwowarska Z., Catalysis Today . 2019,第期

机译：富含Ce的富含CE氧化物纳米催化剂（COXCE1-XOY）对甲醇的低温总氧化的比较研究
8. HIGH YIELD, LOW TEMPERATURE OXIDATION OF METHANE TO METHANOL [C] . NATO advanced study institute on catalytic activation and functionalisation of light alkanes . 1998

机译：高产，低温氧化甲烷至甲醇
9. Development of Detailed, Reduced and Skeletal Kinetic Mechanisms for Hydrocarbon Oxidation at Low and Intermediate Temperatures. [D] . Gupta, Ashutosh. 2011

机译：低温和中温下烃氧化的详细，还原和骨架动力学机理的发展。
10. High H2O2 Utilization Promotes Selective Oxidation of Methane to Methanol at Low Temperature [O] . Yang Yan, Changlei Chen, Shihui Zou, 2020

机译：高H2O2利用率促进甲烷在低温下选择性氧化为甲醇
11. Decomposition of hydrogen peroxide catalyzed by AuPd nanocatalysts during methane oxidation to methanol [O] . -1

机译：Aupd纳米催化剂在甲烷氧化过程中催化过氧化氢的分解甲醇
12. KINETICS OF THE CATALYZED OXIDATION OF HYDROGEN, CARBON MONOXIDE, AND METHANE BY OXYGEN IN A FLOWING STREAM OF HELIUM [R] . C. D. Scott 1961

机译：氦气流中氧气催化氧化氢，一氧化碳和甲烷的动力学

Mechanism and Kinetics of Methane Oxidation to Methanol Catalyzed by AuPd Nanocatalysts at Low Temperature

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