Oxide–Zeolite-Based Composite Catalyst Concept That Enables Syngas Chemistry beyond Fischer–Tropsch Synthesis

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(11), P. 6588 - 6609

Published: May 25, 2021

Syngas chemistry has been under study since Fischer-Tropsch synthesis (FTS) was invented in the 1920s. Despite successful applications of FTS as core technology coal-to-liquid and gas-to-liquid processes industry, product selectivity control syngas conversion still remains a great challenge, particularly for value-added chemicals such light olefins. Recent studies show that catalyst design concept OXZEO (oxide-zeolite-based composite) enables direct to mixed olefins with reaching 80% ethylene 83% among hydrocarbons. They both well-surpass limits predicated by Anderson-Schultz-Flory model via conventional route (58% 30%, respectively). Furthermore, this allows one-step gasoline-range isoparaffins aromatic compounds, which is otherwise not possible FTS. A rapidly growing number demonstrate versatility may form platform utilization carbon resources including coal, natural gas, biomass variety basic fuels. However, mechanism far from being understood. Therefore, we focus mainly on catalytic roles bifunctionalities while reviewing development bifunctional catalysts selective taking syngas-to-light an example. With this, intend provide insights into order understand challenges prospects future much more active catalysts.

Language: Английский

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Towards the development of the emerging process of CO₂heterogenous hydrogenation into high-value unsaturated heavy hydrocarbons

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(19), P. 10764 - 10805

Published: Jan. 1, 2021

This review covers recent developments in the synthesis of α-olefins and aromatics from CO 2 hydrogenation via direct indirect routes.

Language: Английский

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CO2 towards fuels: A review of catalytic conversion of carbon dioxide to hydrocarbons

Journal of environmental chemical engineering, Journal Year: 2020, Volume and Issue: 9(2), P. 104756 - 104756

Published: Nov. 14, 2020

Language: Английский

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Advances in Catalytic Applications of Zeolite‐Supported Metal Catalysts

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(51)

Published: Oct. 5, 2021

Abstract Zeolites possessing large specific surface areas, ordered micropores, and adjustable acidity/basicity have emerged as ideal supports to immobilize metal species with small sizes high dispersities. In recent years, the zeolite‐supported catalysts been widely used in diverse catalytic processes, showing excellent activity, superior thermal/hydrothermal stability, unique shape‐selectivity. this review, a comprehensive summary of state‐of‐the‐art achievements applications are presented for important heterogeneous processes last five mainly including 1) hydrogenation reactions (e.g., CO/CO 2 hydrogenation, unsaturated compounds, nitrogenous compounds); 2) dehydrogenation alkane chemical hydrogen storage materials); 3) oxidation CO oxidation, methane alkene epoxidation); 4) other hydroisomerization reaction selective reduction NO x ammonia reaction). Finally, some current limitations future perspectives on challenge opportunity subject pointed out. It is believed that review will inspire more innovative research synthesis catalysis promote their developments meet emerging demands practical applications.

Language: Английский

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Photocatalytic and electrocatalytic transformations of C1 molecules involving C–C coupling

Energy & Environmental Science, Journal Year: 2020, Volume and Issue: 14(1), P. 37 - 89

Published: Oct. 31, 2020

Selective transformation of one-carbon (C1) molecules, which are abundant or easily available and inexpensive carbon feedstocks, into value-added multi-carbon (C2+) compounds is a very attractive but highly challenging research target. Photocatalysis electrocatalysis have offered great opportunities for the activation controllable C–C coupling C1 molecules under mild environmentally benign conditions. This article provides critical review on recent advances in photocatalytic electrocatalytic conversions major including CO, CO2, CH4, CH3OH HCHO, C2+ compounds, such as C2H4, C3H6, ethanol ethylene glycol, play essential roles current chemical energy industry. Besides photocatalysts electrocatalysts reported these conversions, structure–performance relationships key factors that control activity product selectivity analysed to provide insights rational design more efficient catalysts synthesis from feedstocks. The active species, reaction intermediates catalyst-functioning mechanism discussed deepen understanding chemistry selective presence solar electrical energy.

Language: Английский

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Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Nature Nanotechnology, Journal Year: 2023, Volume and Issue: 18(3), P. 299 - 306

Published: Jan. 12, 2023

Language: Английский

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Aromatics Production via Methanol-Mediated Transformation Routes

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(13), P. 7780 - 7819

Published: June 14, 2021

The methanol-to-aromatics (MTA) process is regarded as a promising route to produce aromatic commodities through non-petroleum carbon resources, such biomass, waste, coal, natural gas, and CO2. In contrast with the industrially implemented methanol-to-olefin (MTO) process, most MTA studies are still in laboratory-scale stage. Recently, few demonstration plants of have been successfully launched, indicating importance gradual industrial maturity this technology. However, there many fundamental questions technological challenges that must be addressed. Review, we summarize recent advances mechanistic understanding on reaction catalyst deactivation during MTA, elaborate available strategies improve catalytic performance, correlate other important aromatization processes. With knowledge hand, share our views future research directions field.

Language: Английский

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Interfacing with Carbonaceous Potassium Promoters Boosts Catalytic CO₂ Hydrogenation of Iron

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(20), P. 12098 - 12108

Published: Aug. 26, 2020

Directly converting carbon dioxide into high-valued olefins (ethylene, propylene, and linear α-olefins) with regenerative hydrogen could be a way of reducing CO2 emissions replacing fossil fuels. However, precise control C–O activation subsequent C–C coupling toward those remain challenge, due to the unclear catalytic mechanism on active sites surrounding promoters. Herein, we demonstrate that carbonaceous series K-promoters from K2CO3, CH3COOK, KHCO3, KOH can induce Fe/C catalysts form more distinct Fe5C2–K2CO3 interface in nanoscale via hydrogenation, which boosts production by facilitating electron transfer potassium iron species. A high olefin selectivity near 75% hydrocarbons is realized at conversion than 32%. The maximum yield reaches up 20.1%, record-breaking highest value among all Fe based hydrogenation literature. More interestingly, appropriate proximity between catalyst endow system an outstanding stability. These findings enrich chemistry provide strategy design highly selective for chemicals.

Language: Английский

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Disentangling the activity-selectivity trade-off in catalytic conversion of syngas to light olefins

Science, Journal Year: 2023, Volume and Issue: 380(6646), P. 727 - 730

Published: May 18, 2023

Breaking the trade-off between activity and selectivity has been a long-standing challenge in field of catalysis. We demonstrate importance disentangling target reaction from secondary reactions for case direct syngas conversion to light olefins by incorporating germanium-substituted AlPO-18 within framework metal oxide-zeolite (OXZEO) catalyst concept. The attenuated strength catalytically active Brønsted acid sites allows enhancing targeted carbon-carbon coupling ketene intermediates form increasing site density while inhibiting that consume olefins. Thus, light-olefins 83% among hydrocarbons carbon monoxide 85% were obtained simultaneously, leading an unprecedented yield 48% versus current reported yields ≤27%.

Language: Английский

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Light olefin synthesis from a diversity of renewable and fossil feedstocks: state-of the-art and outlook

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(18), P. 7994 - 8044

Published: Jan. 1, 2022

Light olefins are important feedstocks and platform molecules for the chemical industry. Their synthesis has been a research priority in both academia There many different approaches to of these compounds, which differ by choice raw materials, catalysts reaction conditions. The goals this review highlight most recent trends light olefin perform comparative analysis synthetic routes using several quantitative characteristics: selectivity, productivity, severity operating conditions, stability, technological maturity sustainability. Traditionally, on an industrial scale, cracking oil fractions used produce olefins. Methanol-to-olefins, alkane direct or oxidative dehydrogenation technologies have great potential short term already reached scientific maturities. Major progress should be made field methanol-mediated CO CO2 hydrogenation electrocatalytic reduction is very attractive process long run due low temperature possible use sustainable electricity. application modern concepts such as electricity-driven intensification, looping, management nanoscale catalyst design lead near future more environmentally friendly, energy efficient selective large-scale synthesis.

Language: Английский

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