Boosting CO₂ Hydrogenation to Methanol over Monolayer MoS₂ Nanotubes by Creating More Strained Basal Planes

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(14), С. 10032 - 10043

Опубликована: Апрель 2, 2024

The controlled creation, selective exposure, and activation of more basal planes while simultaneously minimizing the generation exposure edge sites are crucial for accelerating methanol synthesis from CO2 hydrogenation over MoS2 catalysts but remain a bottleneck. Here, we report facile method to fabricate heteronanotube with single-layer coaxially encapsulating carbon nanotubes (CNTs@MoS2) through host–guest chemistry. Inheriting long tubular structure CNTs, grown exhibit significantly than bulk crystals. More importantly, curvature not only promotes strain sulfur vacancy (Sv) also preferentially exposes in-plane Sv limiting which is conducive synthesis. Both layer number can be easily finely adjusted by altering CNT diameter quantity precursors. Remarkably, CNTs@MoS2 monolayer maximum displayed selectivity 78.1% space time yield 1.6 g gMoS2–1 h–1 at 260 °C GHSV 24000 mL gcat.–1 h–1, representing best results date among Mo-based catalysts. This study provides prospects novel catalyst design synthesizing coaxial heterostructure create additional catalytic ultimately enhance conversion selectivity.

Язык: Английский

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Mitigating the Poisoning Effect of Formate during CO₂ Hydrogenation to Methanol over Co-Containing Dual-Atom Oxide Catalysts

JACS Au, Год журнала: 2024, Номер 4(3), С. 1048 - 1058

Опубликована: Фев. 2, 2024

During the hydrogenation of CO2 to methanol over mixed-oxide catalysts, strong adsorption and formate poses a barrier for H2 dissociation, limiting selectivity productivity. Here we show that by using Co-containing dual-atom oxide poisoning effect can be countered separating site dissociation intermediates. We synthesized Co- In-doped ZrO2 catalyst (Co–In–ZrO2) containing atomically dispersed Co In species. Catalyst characterization showed atoms were in proximity each other owing random distribution. reaction, atom was responsible species, while nearby promoted adsorbed The cooperative increased 86% catalyst, productivity 2-fold comparison single-atom catalysts. This extended Co–Zn Co–Ga doped work presents different approach designing catalysts based on preferential substrates intermediates instead promoting mitigate poisonous effects

Язык: Английский

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NiGa nano-alloy for the dry reforming of methane: Influences of Ga alloying with Ni on the catalytic activity and stability

Chemical Engineering Journal, Год журнала: 2024, Номер 487, С. 150351 - 150351

Опубликована: Март 11, 2024

Язык: Английский

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Cu0 at the Cu/ZnO interface efficiently accelerate CO2 hydrogenation to methanol over Cu/ZnO/C–P catalysts

International Journal of Hydrogen Energy, Год журнала: 2024, Номер 58, С. 128 - 136

Опубликована: Янв. 20, 2024

Язык: Английский

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Oxygen vacancy engineering in MOF-derived AuCu/ZnO bimetallic catalysts for methanol synthesis via CO2 hydrogenation

Catalysis Today, Год журнала: 2024, Номер 434, С. 114702 - 114702

Опубликована: Апрель 5, 2024

Язык: Английский

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Gallium Cluster-Promoted In₂O₃ Catalyst for CO₂ Hydrogenation to Methanol

ACS Catalysis, Год журнала: 2024, Номер 14(18), С. 13958 - 13972

Опубликована: Сен. 6, 2024

Язык: Английский

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High-performance CuMgAl catalysts derived from hydrotalcite for CO2 hydrogenation to methanol: Effects of Cu-MgO interaction

Molecular Catalysis, Год журнала: 2024, Номер 558, С. 114002 - 114002

Опубликована: Март 7, 2024

Язык: Английский

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Insights into the Selectivity Determinant and Rate-Determining Step of CO₂ Hydrogenation to Methanol

The Journal of Physical Chemistry C, Год журнала: 2022, Номер 126(25), С. 10399 - 10407

Опубликована: Июнь 16, 2022

CO2 hydrogenation to methanol has attracted much attention. The mechanism, the factors affecting selectivity, and rate-determining step of reaction have not been clearly concluded. Here, mechanism on Cu/ZnO/Al2O3, Pd/ZnO, ZnZrOx catalysts was studied by in situ infrared spectroscopy HCOOH temperature-programmed surface (HCOOH-TPSR) experiment. It is shown that HCOO* a feasible more stable is, higher selectivity accompanied with less CO produced via decomposition HCOO*. H2–D2 isotope exchange inhibited presence CO2, which indicates H2 activation H* migration are adsorbed catalysts. As for methanol, orders close 0.5 0, respectively, indicating activated insufficient. Comparing reaction, their both two rates show linear relationship when temperature changes. considered

Язык: Английский

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Mononuclear Re sites on In2O3 catalyst for highly efficient CO2 hydrogenation to methanol

Journal of Catalysis, Год журнала: 2022, Номер 417, С. 462 - 472

Опубликована: Дек. 23, 2022

Язык: Английский

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Mechanism-Guided Catalyst Design for CO₂ Hydrogenation to Formate and Methanol

Accounts of Materials Research, Год журнала: 2023, Номер 4(9), С. 746 - 757

Опубликована: Июль 26, 2023

ConspectusCO2 to formate/formic acid and methanol has emerged as a promising method for utilizing CO2 in chemical fuel synthesis, well reducing emissions when H2 is produced through renewable energy sources. This reaction requires the activation of two chemically distinct molecules, H2, along with selective formation desired product. Creating efficient catalysts that surpass limitations existing remains significant challenge. Historically, development largely depended on trial error until successful outcomes are achieved. However, recent advances material synthesis well-defined structures, kinetics analysis, situ characterization techniques, computational studies have facilitated systematic understanding catalytic reactions enabled mechanism-guided catalyst development. innovative approach empowered researchers strategically design effective optimize target reaction, particularly rate-determining step, while tackling other limitations, such selectivity stability.This Account provides an overview our efforts hydrogenation engineering, which primarily divided into sections: (i) formic acid/formate (ii) production. For acid, we first discuss structure–activity correlation various metal/support systems, including different metal particle sizes, types support, crystalline morphologies support. These highlight crucial role electron-rich sites splitting adequate number weak basic activation, inform improved unique architectures. Notably, encapsulated cluster enhance utilization species synergistic interaction between active support material. The encapsulation strategy can also be applied inexpensive elements Ni, facilitating highly catalysts.Our primary focus CO2-to-methanol durable oxide-based catalysts. We identify critical limitation oxide their poor capability, based comprehensive review classical state-of-the-art Consequently, principal concept involves coupling promoters, provide high functionality, enable adsorption synthesis. An essential synthetic doping promoters surface Specifically, atomically dispersed significantly improve yield by maximizing interfacial synergy catalyst. A remarkable incorporation hydrogen dispenser, conductive carbon, promoter multicomponent composite dramatically enhances delivery from via long-range spillover, resulting accelerated overcomes conventional metal/oxide constrain movement across conclude discussing underlying implications these observations offering perspectives future research opportunities.

Язык: Английский

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