Oxygen vacancy-dependent chemical intermediates on Ru/MnO catalysts dictate the selectivity of CO2 reduction

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 352, С. 124010 - 124010

Опубликована: Апрель 21, 2024

Язык: Английский

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

Chemical Reviews, Год журнала: 2024, Номер 124(21), С. 12006 - 12085

Опубликована: Окт. 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.

Язык: Английский

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A New Look at Catalyst Surfaces at Work: Introducing Mixed Isotope Operando Infrared Spectroscopy (MIOIRS)

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 1363 - 1386

Опубликована: Янв. 8, 2025

This Perspective focuses on the characterization of supported metal catalysts by operando and CO infrared (IR) spectroscopy. IR spectroscopy is a powerful technique for probing catalyst surfaces used to identify single-atom catalysts, estimate surface availability gas phase, measure Lewis acidity. However, interpretation spectra not trivial influenced dipole–dipole interactions among molecules at medium high coverage. Such phenomenon results in spectral distortions, such as intensity transfer bands, appearance spurious shifts band position. Dipole–dipole were widely investigated understood from 1950s 1990s, but implications have been seemingly overlooked literature, with few exceptions. Inspired seminal studies field, I propose here use mixed isotopic streams, diluted 13CO 12CO, reduce dipole coupling effects retrieve more information reactions involving CO, oxidation or hydrogenation reactions. Similarly, 13CO2/12CO2 streams may be applied CO2 hydrogenation, where adsorbed commonly observed. The proposed name Mixed Isotope Operando Spectroscopy, MIOIRS. In this Perspective, will first summarize nature layers their spectra. Then, briefly describe how mixtures can partially break adsorbates distortion. both sections, give showcases vibrational heterogeneous catalysts. Finally, discuss possible MIOIRS detection quantification defect sites nanoparticles, bimetallic nanoparticles surfaces, kinetics intermediates different active sites. Notably, expanded other which strong permanent dipoles, self-catalytic reduction NOx abatement.

Язык: Английский

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Highly stable FeNiMnCaO catalyst for integrated CO2 capture and hydrogenation to CO

Chemical Engineering Journal, Год журнала: 2024, Номер 482, С. 148948 - 148948

Опубликована: Янв. 29, 2024

Язык: Английский

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Reaction Mechanisms and Applications of Single Atom Catalysts for Thermal-Catalytic Carbon Dioxide Hydrogenation Toward Oxygenates

ACS Catalysis, Год журнала: 2024, Номер 14(21), С. 16434 - 16458

Опубликована: Окт. 23, 2024

Thermo-catalytic CO2 hydrogenation to high-value oxygenates has been regarded as one of the most powerful strategies that can potentially alleviate excessive emissions. However, due high chemical stability and variability pathways, it is still challenging achieve highly active selective hydrogenation. Single atom catalysts (SACs) with ultrahigh metal utilization efficiency extraordinary electronic features have displayed growing importance for thermo-catalytic multiple developed improve performances. Here, we review breakthroughs in developing SACs efficient toward common (CO, HCOOH, CH3OH, CH3CH2OH) following order: first, an analysis reaction mechanisms thermodynamics challenges reactions; second, a summary SAs designed by dividing them into two categories single- dual-sites; third, discussion support effects focus on approaches regulating strong metal–support interaction (MSI). Summarily, current future perspectives develop higher-performance are presented. We expect this bring more design inspiration trigger innovation catalytic evolution materials eventually benefit achievement carbon-neutrality goal.

Язык: Английский

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Kinetic and DRIFTS studies of the CO2 catalytic hydrogenation on Ru/SiO2: A comprehensive and strategic investigation of CO2 methanation mechanisms by kinetic modeling and data regression

Chemical Engineering Journal, Год журнала: 2024, Номер 485, С. 149716 - 149716

Опубликована: Фев. 22, 2024

Язык: Английский

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Deconvoluting the Individual Effects of Nanoparticle Proximity and Size in Thermocatalysis

ACS Nano, Год журнала: 2024, Номер 18(24), С. 15958 - 15969

Опубликована: Июнь 5, 2024

Nanoparticle (NP) size and proximity are two physical descriptors applicable to practically all NP-supported catalysts. However, with conventional catalyst design, independent variation of these investigate their individual effects on thermocatalysis remains challenging. Using a raspberry-colloid-templating approach, we synthesized well-defined series comprising Pd12Au88 alloy NPs three distinct sizes at different interparticle distances. We show that NP distance independently control activity selectivity, respectively, in the hydrogenation benzaldehyde benzyl alcohol toluene. Surface-sensitive spectroscopic analysis indicates surfaces smaller expose greater fraction reactive Pd dimers, compared inactive single atoms, thereby increasing intrinsic catalytic activity. Computational simulations reveal how larger improves selectivity by diminishing local concentration profile between NPs, thus suppressing its readsorption consequently, undesired formation Accordingly, yield is maximized using catalysts separated distances, overcoming activity–selectivity trade-offs. This work exemplifies high suitability modular method as model platform isolate establish clear structure–property relationships, bridging materials gap surface science technical

Язык: Английский

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Revisiting the influence of Ni particle size on the hydrogenation of CO2 to CH4 over Ni/CeO2

Journal of Catalysis, Год журнала: 2024, Номер 438, С. 115708 - 115708

Опубликована: Авг. 13, 2024

Язык: Английский

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Small Cobalt Nanoparticles Favor Reverse Water‐Gas Shift Reaction Over Methanation Under CO₂ Hydrogenation Conditions**

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(52)

Опубликована: Ноя. 13, 2023

Cobalt-based catalysts are well-known to convert syngas into a variety of Fischer-Tropsch (FTS) products depending on the various reaction parameters, in particular particle size. In contrast, reactivity these particles has been much less investigated context CO2 hydrogenation. that context, Surface organometallic chemistry (SOMC) was employed synthesize highly dispersed cobalt nanoparticles (Co-NPs) with sizes ranging from 1.6 3.0 nm. These SOMC-derived Co-NPs display significantly different catalytic performances under hydrogenation conditions: while smallest (1.6 nm) catalyze mainly reverse water-gas shift (rWGS) reaction, larger (2.1-3.0 favor expected methanation activity. Operando X-ray absorption spectroscopy shows smaller fully oxidized conditions, ones remain mostly metallic, paralleling observed difference performances. This fundamental selectivity, away for is noteworthy and correlates formation CoO conditions.

Язык: Английский

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Tuning Catalytic Activity of CO₂ Hydrogenation to C1 Product via Metal Support Interaction Over Metal/Metal Oxide Supported Catalysts

ChemSusChem, Год журнала: 2024, Номер 17(16)

Опубликована: Март 28, 2024

Abstract The metal supported catalysts are emerging that receiving a lot of attention in CO 2 hydrogenation to C1 products. Numerous experiments have demonstrated the support (usually an oxide) is crucial for catalytic performance. oxides used aid homogeneous dispersion particles, prevent agglomeration, and control morphology owing interaction (MSI). MSI can efficiently optimize structural electronic properties tune conversion key reaction intermediates involved hydrogenation, thereby enhancing There increasing being paid promotion effects process. However, systematically understanding about on products performance has not been fully studied yet due diversities conditions. Hence, characteristics modes elaborated detail our work.

Язык: Английский

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