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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Advances in the Design of Heterogeneous Catalysts and Thermocatalytic Processes for CO₂ Utilization

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(23), P. 14147 - 14185

Published: Nov. 20, 2020

Utilization of CO2 as feedstock to produce fine chemicals and renewable fuels is a highly promising field, which presents unique challenges in its implementation at scale. Heterogeneous catalysis with simple operation industrial compatibility can be an effective means achieving this challenging task. This review summarizes the current developments heterogeneous thermal for production carbon monoxide, alcohols, hydrocarbons from CO2. A detailed discussion provided regarding structure–activity correlations between catalyst surface intermediate species aid rational design future generation catalysts. Effects active metal components, supports, promoters are discussed each section, will guide researchers synthesize new catalysts improved selectivity stability. Additionally, brief overview process considerations has been provided. Future research directions proposed special emphasis on application scope catalytic materials possible approaches increase performance.

Language: Английский

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Applications of Zeolites to C1 Chemistry: Recent Advances, Challenges, and Opportunities

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(44)

Published: July 22, 2020

Abstract C1 chemistry, which is the catalytic transformation of molecules including CO, CO 2 , CH 4 3 OH, and HCOOH, plays an important role in providing energy chemical supplies while meeting environmental requirements. Zeolites are highly efficient solid catalysts used industry. The design development zeolite‐based mono‐, bi‐, multifunctional has led to a booming application chemistry. Combining advantages zeolites metallic species promoted production various hydrocarbons (e.g., methane, light olefins, aromatics, liquid fuels) oxygenates methanol, dimethyl ether, formic acid, higher alcohols) from molecules. key zeolite descriptors that influence performance, such as framework topologies, nanoconfinement effects, Brønsted acidities, secondary‐pore systems, particle sizes, extraframework cations atoms, hydrophobicity hydrophilicity, proximity between acid sites discussed provide deep understanding significance An outlook regarding challenges opportunities for conversion resources using meet emerging demands also presented.

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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Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels

ACS Central Science, Journal Year: 2020, Volume and Issue: 6(10), P. 1657 - 1670

Published: Sept. 18, 2020

Carbon dioxide (CO2) hydrogenation to liquid fuels including gasoline, jet fuel, diesel, methanol, ethanol, and other higher alcohols via heterogeneous catalysis, using renewable energy, not only effectively alleviates environmental problems caused by massive CO2 emissions, but also reduces our excessive dependence on fossil fuels. In this Outlook, we review the latest development in design of novel very promising catalysts for direct hydrocarbons, alcohols. Compared with methanol production, synthesis products two or more carbons (C2+) faces greater challenges. Highly efficient C2+ from can be achieved a reaction coupling strategy that first converts carbon monoxide then conducts C–C over bifunctional/multifunctional catalyst. Apart catalytic performance, unique catalyst ideas, structure–performance relationship, discuss current challenges perspectives industrial applications.

Language: Английский

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Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Nature Communications, Journal Year: 2020, Volume and Issue: 11(1)

Published: Feb. 11, 2020

Abstract Synthesis of ethanol from non-petroleum carbon resources via syngas (a mixture H 2 and CO) is an important but challenging research target. The current conversion to suffers low selectivity or multiple processes with high energy consumption. Here, we report a high-selective into by triple tandem catalysis. An efficient trifunctional system composed potassium-modified ZnO–ZrO , modified zeolite mordenite Pt–Sn/SiC working compatibly in stream one reactor can afford 90%. We demonstrate that the K + –ZnO–ZrO catalyses methanol eight-membered ring channels functions for carbonylation acetic acid, which then hydrogenated over catalyst. present work offers effective methodology leading selective decoupling single-catalyst-based complicated uncontrollable reaction well-controlled multi-steps reactor.

Language: Английский

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Tandem Catalysis for Hydrogenation of CO and CO₂ to Lower Olefins with Bifunctional Catalysts Composed of Spinel Oxide and SAPO-34

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(15), P. 8303 - 8314

Published: July 6, 2020

Transformation of syngas (H2/CO) and hydrogenation CO2 into lower olefins are attractive routes for chemical utilization various carbon resources CO2, but both suffer from limited product selectivity. Tandem catalysis that integrates the activation CO or to an intermediate subsequent controllable C–C bond formation form offers a promising approach. Here, we report over bifunctional catalysts composed spinel binary metal oxide SAPO-34. ZnAl2O4/SAPO-34 ZnGa2O4/SAPO-34 found be highly selective synthesis CO2. Our studies reveal oxygen vacancy site on oxides plays pivotal role in adsorption while −Zn–O– domain accounts H2 activation. We demonstrate methanol dimethyl ether formed reaction intermediates, which subsequently converted by Brønsted acid sites zeolite. The surfaces proceeds via same formate methoxide species. elucidate water–gas shift is responsible during conversion. cofeeding useful strategy inhibit formation.

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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Recent advances in carbon dioxide hydrogenation to produce olefins and aromatics

Chem, Journal Year: 2021, Volume and Issue: 7(9), P. 2277 - 2311

Published: March 20, 2021

Language: Английский

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Highly Selective Olefin Production from CO₂ Hydrogenation on Iron Catalysts: A Subtle Synergy between Manganese and Sodium Additives

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(48), P. 21736 - 21744

Published: Aug. 28, 2020

Mn and Na additives have been widely studied to improve the efficiency of CO2 hydrogenation valuable olefins on Fe catalysts, but their effects catalytic properties mechanism are still under vigorous debate. This study shows that Fe-based catalysts with moderate contents highly selective for olefins, together low selectivities both CO CH4 much improved space-time olefin yields compared state-of-the-art catalysts. Combined kinetic assessment quasi in situ characterizations further unveil sole presence suppresses activity because close contact between Mn, whereas introduction mediates Fe-Mn interaction provides strong basic sites. subtle synergy sheds light importance interplay multiple could bring an enabling strategy selectivity.

Language: Английский

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