The synthesis of a specific product via the Fischer-Tropsch synthesis remains challenging due to the uncontrollable coupling of CH on active sites. Isoparaffins, essential high-quality petroleum additives for improving octane numbers, are primarily derived from petroleum or natural gas. With petroleum reserves dwindling and the associated low selectivity, the direct conversion of syngas to isoparaffins has emerged as a promising alternative. This study presents a tandem catalyst comprising CoMnO and zeolites for catalyzing the direct conversion of syngas to C-C isoparaffins. The relay catalyst exhibited an impressive selectivity of 55.6% toward the desired products while maintaining a low CO selectivity of approximately 20%. Notably, the selectivity of isobutane reached 43.5%, exceeding predictions based on the Anderson-Schulz-Flory distribution. Syngas undergoes conversion into olefins on CoMnO nanocomposites, diffuses into microporous zeolites, and interacts with Brønsted acids to produce isoparaffins. The stability of the relay catalyst relied significantly on the pore characteristics and acidic density of the zeolites.
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http://dx.doi.org/10.1021/acs.inorgchem.4c02142 | DOI Listing |
Sci Adv
January 2025
Institute of Energy, School of Earth and Space Sciences, Peking University, Beijing 100871, China.
The origins of natural hydrogen in natural gas systems of sedimentary basins and the capacity of these systems to store hydrogen remain inadequately understood, posing crucial questions for the large-scale exploration of natural hydrogen. This study reports on the natural gas composition, stable carbon and hydrogen isotopic values, and helium isotopic values of gas samples collected from the Qingshen gas deposit within volcanic rocks of the Songliao Basin. Natural hydrogen primarily originates from water radiolysis, water-rock interactions (WRI), and mantle.
View Article and Find Full Text PDFNat Commun
January 2025
Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
Angew Chem Int Ed Engl
January 2025
Australian National University, Research School of Chemistry, AUSTRALIA.
Heterobimetallic μ-methylidyne complexes [WPt(μ2-CH)(CO)2L2(Tp*)], where L2 = (PPh3)2, (PPh3)(CO), (dppe), (PPh3)(CNC6H2Me3), have been obtained via the intermediacy of transient hydrido-μ-carbido complexes that undergo carbido-hydrido coupling to model a fundamental step in the proposed mechanism for Fischer-Tropsch synthesis.
View Article and Find Full Text PDFChem Soc Rev
January 2025
Interdisciplinary Institute of NMR and Molecular Sciences, School of Chemistry and Chemical Engineering, The State Key Laboratory of Refractories and Metallurgy, Hubei Province for Coal Conversion and New Carbon Materials, Wuhan University of Science and Technology, Wuhan 430081, P. R. China.
The thermocatalytic conversion of CO with green or blue hydrogen into valuable energy and commodity chemicals such as alcohols, olefins, and aromatics emerges as one of the most promising strategies for mitigating global warming concerns in the future. This process can follow either a CO-modified Fischer-Tropsch synthesis route or a methanol-mediated route, with the latter being favored for its high product selectivity beyond the Anderson-Schulz-Flory distribution. Despite the progress of the CO-led methanol-mediated route over bifunctional metal/zeolite catalysts, challenges persist in developing catalysts with both high activity and selectivity due to the complexity of CO hydrogenation reaction networks and the difficulty in controlling C-O bond activation and C-C bond coupling on multiple active sites within zeolites.
View Article and Find Full Text PDFAcc Chem Res
January 2025
Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
ConspectusFor chemical reactions with complex pathways, it is extremely difficult to adjust the catalytic performance. The previous strategies on this issue mainly focused on modifying the fine structures of the catalysts, including optimization of the geometric/electronic structure of the metal nanoparticles (NPs), regulation of the chemical composition/morphology of the supports, and/or adjustment of the metal-support interactions to modulate the reaction kinetics on the catalyst surface. Although significant advances have been achieved, the catalytic performance is still unsatisfactory.
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