Dataset Information

Direct conversion of methane to formaldehyde and CO on B₂O₃ catalysts.

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 g_cat^-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.

SUBMITTER: Tian J

PROVIDER: S-EPMC7655938 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature

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Direct conversion of methane to formaldehyde and CO on B2O3 catalysts.

Tian Jinshu J Tan Jiangqiao J Zhang Zhaoxia Z Han Peijie P Yin Min M Wan Shaolong S Lin Jingdong J Wang Shuai S Wang Yong Y

Nature communications 20201110 1

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% conv ...[more]

PMID: 33173054

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Project description:The development of efficient catalysts is one of the main challenges in CO2 conversion to valuable chemicals and fuels. Herein, inspired by the knowledge of the thermocatalytic (TC) processes, Cu/ZnO and bare Cu catalysts enriched with Cu+1 were studied to convert CO2 via the electrocatalytic (EC) pathway. Integrating Cu with ZnO (a CO-generation catalyst) is a strategy explored in the EC CO2 reduction to reduce the kinetic barrier and enhance C-C coupling to obtain C2+ chemicals and energy carriers. Herein, ethanol was produced with the Cu/ZnO catalyst, reaching a productivity of about 5.27 mmol·gcat-1·h-1 in a liquid-phase configuration at ambient conditions. In contrast, bare copper preferentially produced C1 products like formate and methanol. During CO2 hydrogenation, a methanol selectivity close to 100% was achieved with the Cu/ZnO catalysts at 200 °C, a value that decreased at higher temperatures (i.e., 23% at 300 °C) because of thermodynamic limitations. The methanol productivity increased to approximately 1.4 mmol·gcat-1·h-1 at 300 °C. Ex situ characterizations after testing confirmed the potential of adding ZnO in Cu-based materials to stabilize the Cu1+/Cu0 interface at the electrocatalyst surface because of Zn and O enrichment by an amorphous zinc oxide matrix; while in the TC process, Cu0 and crystalline ZnO prevailed under CO2 hydrogenation conditions. It is envisioned that the lower *CO binding energy at the Cu0 catalyst surface in the TC process than in the Cu1+ present in the EC one leads to preferential CO and methanol production in the TC system. Instead, our EC results revealed that an optimum local CO production at the ZnO surface in tandem with a high amount of superficial Cu1+ + Cu0 species induces ethanol formation by ensuring an appropriate local amount of *CO intermediates and their further dimerization to generate C2+ products. Optimizing the ZnO loading on Cu is proposed to tune the catalyst surface properties and the formation of more reduced CO2 conversion products.

Dataset Information

Direct conversion of methane to formaldehyde and CO on B₂O₃ catalysts.

Publications

Direct conversion of methane to formaldehyde and CO on B<sub>2</sub>O<sub>3</sub> catalysts.

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