Recent advancements and perspectives of the CO2 hydrogenation reaction

Green Carbon, Journal Year: 2023, Volume and Issue: 1(2), P. 133 - 145

Published: Oct. 23, 2023

Owing to excessive carbon dioxide (CO2) emissions, which cause severe environmental issues, the conversion and utilization of CO2 have received increasing attention. its high efficiency potential for industrial applications, converting into value-added chemicals via thermocatalytic hydrogenation is a highly effective route among electrocatalytic, photocatalytic, conversion. In past two decades, our group has developed novel technologies produce such as aliphatic hydrocarbons, methanol (MeOH), ethanol, aromatics (especially para-xylene, PX). this review, we summarize strategy rational design catalysts, including low-temperature MeOH synthesis capsule catalysts tandem catalysis. We also discuss challenges opportunities hydrogenation, capture, H2 prices, taxes. hope inspire new ideas through exploration reaction paths.

Language: Английский

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Selectivity Control by Relay Catalysis in CO and CO₂ Hydrogenation to Multicarbon Compounds

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(5), P. 714 - 725

Published: Feb. 13, 2024

ConspectusThe hydrogenative conversion of both CO and CO2 into high-value multicarbon (C2+) compounds, such as olefins, aromatic hydrocarbons, ethanol, liquid fuels, has attracted much recent attention. The hydrogenation is related to the chemical utilization various carbon resources including shale gas, biomass, coal, carbon-containing wastes via syngas (a mixture H2 CO), while by green chemicals fuels would contribute recycling for neutrality. state-of-the-art technologies CO/CO2 C2+ compounds primarily rely on a direct route Fischer–Tropsch (FT) synthesis an indirect two methanol-mediated processes, i.e., methanol from compounds. be more energy- cost-efficient owing reduced operation units, but product selectivity FT limited Anderson–Schulz–Flory (ASF) distribution. Selectivity control compound one most challenging goals in field C1 chemistry, chemistry transformation one-carbon (C1) molecules.We have developed relay-catalysis strategy solve challenge arising complicated reaction network involving multiple intermediates channels, which inevitably lead side reactions byproducts over conventional heterogeneous catalyst. core relay catalysis design single tandem-reaction channel, can target controllably, choosing appropriate (or intermediate products) steps connecting these intermediates, arranging optimized yet matched catalysts implement like relay. This Account showcases representative systems our group past decade lower (C2–C4) aromatics, oxygenates with breaking limitation catalysts. These are typically composed metal or oxide CO/CO2/H2 activation zeolite C–C coupling reconstruction, well third even fourth catalyst component other functions if necessary. mechanisms oxides, distinct that transition noble surfaces, discussed emphasis role oxygen vacancies. Zeolites catalyze (including hydrocracking/isomerization heavier methanol-to-hydrocarbon reactions, carbonylation methanol/dimethyl ether) system, mainly controlled Brønsted acidity shape-selectivity confinement effect zeolites. We demonstrate thermodynamic/kinetic matching steps, proximity spatial arrangement components, transportation intermediates/products sequence key issues guiding selection each construction efficient system. Our methodology also useful molecules coupling, inspiring efforts toward precision catalysis.

Language: Английский

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Direct conversion of CO and H2O to hydrocarbons at atmospheric pressure using a TiO2−x/Ni photothermal catalyst

Nature Energy, Journal Year: 2024, Volume and Issue: 9(2), P. 154 - 162

Published: Jan. 5, 2024

Language: Английский

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Opening Direct Electrochemical Fischer–Tropsch Synthesis Path by Interfacial Engineering of Cu Electrode with P-Block Elements

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(3), P. 3368 - 3387

Published: Jan. 12, 2024

The electrochemical synthesis of syngas (CO and H2) has garnered considerable attention in the context Fischer–Tropsch (FT) employing thermal catalysts. Nonetheless, need for a novel, cost-effective technique persists. In this investigation, we introduce direct (dEC) approach FT that functions under ambient conditions by utilizing p-block element (Sn In) overlaid Cu electrode. Surface *CO H* species were obtained an electrolytic medium through CO2 + H+ e– → HOOCad (or CO adsorption) reactions, respectively. We have observed C2–7 long-chain hydrocarbons with CnH2n+2/CnH2n ratio 1–3, observation can be explained process C–C coupling chain growth conventional synthesis, based on linearity Anderson-Schulz–Flory equation plots. Thick Sn overlayers resulted dominant production formate, while C2H4 found to proportional inversely correlated H2, C2H6, C3–7 hydrocarbon production. EC CO2/CO reduction used dEC offers valuable insights into mechanism C2+ holds promise as eco-friendly producing energy environmental purposes.

Language: Английский

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Crystal-Phase Engineering in Heterogeneous Catalysis

Chemical Reviews, Journal Year: 2023, Volume and Issue: 124(1), P. 164 - 209

Published: Dec. 4, 2023

The performance of a chemical reaction is critically dependent on the electronic and/or geometric structures material in heterogeneous catalysis. Over past century, Sabatier principle has already provided conceptual framework for optimal catalyst design by adjusting structure catalytic via change composition. Beyond composition, it essential to recognize that atomic catalyst, encompassing terraces, edges, steps, kinks, and corners, have substantial impact activity selectivity reaction. Crystal-phase engineering capacity bring about alterations configurations enabling control over coordination numbers, morphological features, arrangement surface atoms. Modulating crystallographic phase therefore an important strategy improving stability, activity, materials. Nonetheless, complete understanding how depends crystal remains elusive, primarily due absence molecular-level view active sites across various phases. In this review, we focus assessing dependence phases elucidate challenges complexities inherent catalysis, ultimately aiming improved design.

Language: Английский

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Perspectives and Outlook of E-fuels: Production, Cost Effectiveness, and Applications

Energy & Fuels, Journal Year: 2024, Volume and Issue: 38(9), P. 7665 - 7692

Published: April 23, 2024

With the introduction of EU's "ban on combustion" proposal in 2035, sale new fossil fuel vehicles will soon be comprehensively prohibited. The use e-fuels has become best means for survival and continuation internal combustion engines, while also responding to call carbon neutrality. This review studies how raw materials required different can obtained through assistance renewable energy or various net-zero emission routes, elaborates synthesis methods, economics, challenges faced by such as e-methanol e-ammonia. E-fuels have a wide range market applications, including but not limited road transportation, aviation, shipping, some transportation already chosen their fuel. By summarizing technoeconomic analysis e-fuels, this aims provide referable methods multiple options future large-scale production well insights subsequent application improvement e-fuels.

Language: Английский

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MXene-based catalysts: A review

Materials Today Catalysis, Journal Year: 2024, Volume and Issue: 5, P. 100054 - 100054

Published: May 27, 2024

Two-dimensional (2D) materials, such as graphene, hexagonal boron nitride, 2D metal–organic frameworks, layered double hydroxides, transition metal dichalcogenides, and MXenes, have garnered significant attention in catalysis due to their exceptional properties structures. Notably, recent studies revealed the promising catalytic activity of MXene-based catalysts for many reactions, including hydrogen evolution, oxygen reduction, nitrogen carbon dioxide alcohol oxidation, hydrogenation, dehydrogenation, methanol conversion, dry reforming methane, CO oxidation. This review offers a summary advances field, contextualizing progress made. Additionally, it delves into existing challenges while presenting prospects future developments this domain.

Language: Английский

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Understanding and Tuning the Effects of H₂O on Catalytic CO and CO₂ Hydrogenation

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(21), P. 12006 - 12085

Published: Oct. 31, 2024

Catalytic COx (CO and CO2) hydrogenation to valued chemicals is one of the promising approaches address challenges in energy, environment, climate change. H2O an inevitable side product these reactions, where its existence effect are often ignored. In fact, significantly influences catalytic active centers, reaction mechanism, performance, preventing us from a definitive deep understanding on structure-performance relationship authentic catalysts. It necessary, although challenging, clarify provide practical strategies tune concentration distribution optimize influence. this review, we focus how induces structural evolution catalysts assists processes, as well efforts understand underlying mechanism. We summarize discuss some representative tuning for realizing rapid removal or local enrichment around catalysts, along with brief techno-economic analysis life cycle assessment. These fundamental understandings further extended reactions CO CO2 reduction under external field (light, electricity, plasma). also present suggestions prospects deciphering controlling applications.

Language: Английский

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CuNiZn vs CuZn Electrodes: Electrochemical CO₂ Reduction, Role of Metal Elements, and Insights for C–C Coupling Chemistry

ACS Applied Energy Materials, Journal Year: 2024, Volume and Issue: 7(2), P. 614 - 628

Published: Jan. 3, 2024

Exploring bi- and trimetallic catalysts in electrochemical CO2 reduction (EC CO2R) has been a focal point for discovering products. This study investigates the distinct roles of metal elements CO2R using CuNiZn CuZn electrodes. Bimetallic exhibits superior activity, yielding substantial amounts CO, CH4, C2H4, various liquid products, including formate, ethanol, acetate, propanol, isopropanol. The on suggests potential connections to Fischer–Tropsch (FT) synthesis, indicating their capability produce long-chain hydrocarbons (CnH2n CnH2n+2, n = 2–7) from CO2. EC CO validated FT process over catalysts. discussion explores mechanisms formation C–C coupled C2+ considering potential- concentration-dependent Faradaic efficiencies (FEs). Recycling tests emphasize influence composition FEs. Surface analyses reveal oxidation states compositional changes, while dissolution metals during electrochemistry highlights dynamic surface characteristics. work provides insights into catalysts, states, conditions, advancing our understanding these electrodes role recycling through electrochemistry.

Language: Английский

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Harmonized Physical and Electrochemical Process Design for Densely Dispersed Cu Catalysts on Cu₂O Absorbers for Efficient Photoelectrochemical CO₂ Reduction Reaction

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(10)

Published: Jan. 9, 2024

Abstract The photoelectrochemical CO 2 reduction reaction (photo‐CO RR) is a promising technology to convert into high‐value‐added carbon‐based chemicals using relatively low voltage, which can economically solve the problem of emissions. Nevertheless, unlike conventional electrochemical RR approach, photo‐CO in its initial development stage. Particularly, when sunlight applied photoelectrodes for RR, severe photocorrosion unavoidable, resulting deterioration fundamental functions including device long‐term stability and conversion performance. This study proposes an innovative two‐step catalyst formation strategy enable efficient with Cu catalysts prepared intrinsic O absorption layer. approach based on harmonized process design i) growth physically generated nanoparticles ii) construction improved cluster catalysts. vacuum‐evaporated seeds are designed induce evenly dispersed electrical path O, selectively concentrated field from provides preferential sites metallic subsequent reduction. combination demonstrates synergistic performance −1.2 mA cm −2 at 0 V RHE suppression produces ≈95% product gas (0.4 ).

Language: Английский

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