Direct conversion of methane to formaldehyde and CO on B2O3 catalysts

Jinshu Tian, Jiangqiao Tan, Zhaoxia Zhang, Peijie Han, Min Yin, Shaolong Wan, Jingdong Lin, Shuai Wang () and Yong Wang ()
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Jinshu Tian: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Jiangqiao Tan: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Zhaoxia Zhang: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Peijie Han: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Min Yin: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Shaolong Wan: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Jingdong Lin: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Shuai Wang: State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, and College of Chemistry and Chemical Engineering, Xiamen University
Yong Wang: Washington State University

Nature Communications, 2020, vol. 11, issue 1, 1-7

Abstract: Abstract Direct oxidation of methane to value-added C1 chemicals (e.g. HCHO and CO) provides a promising way to utilize natural gas sources under relatively mild conditions. Such conversions remain, however, a key selectivity challenge, resulting from the facile formation of undesired fully-oxidized CO2. Here we show that B2O3-based catalysts are selective in the direct conversion of methane to HCHO and CO (~94% selectivity with a HCHO/CO ratio of ~1 at 6% conversion) and highly stable (over 100 hour time-on-stream operation) conducted in a fixed-bed reactor (550 °C, 100 kPa, space velocity 4650 mL gcat−1 h−1). Combined catalyst characterization, kinetic studies, and isotopic labeling experiments unveil that molecular O2 bonded to tri-coordinated BO3 centers on B2O3 surfaces acts as a judicious oxidant for methane activation with mitigated CO2 formation, even at high O2/CH4 ratios of the feed. These findings shed light on the great potential of designing innovative catalytic processes for the direct conversion of alkanes to fuels/chemicals.

Date: 2020
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DOI: 10.1038/s41467-020-19517-y

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