Single-Atom Catalysts Based on the Metal–Oxide Interaction

Chemical Reviews, Год журнала: 2020, Номер 120(21), С. 11986 - 12043

Опубликована: Окт. 28, 2020

Metal atoms dispersed on the oxide supports constitute a large category of single-atom catalysts. In this review, supported catalysts are discussed about their synthetic procedures, characterizations, and reaction mechanism in thermocatalysis, such as water-gas shift reaction, selective oxidation/hydrogenation, coupling reactions. Some typical materials, including ferric oxide, cerium titanium dioxide, aluminum so on, intentionally mentioned for unique roles anchoring metal taking part catalytic The interactions between summarized to give picture how stabilize atomic centers, rationally tune geometric structures electronic states single atoms. Furthermore, several directions fabricating with improved performance proposed basis state-of-the-art understanding metal-oxide interactions.

Язык: Английский

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Hydrophobic zeolite modification for in situ peroxide formation in methane oxidation to methanol

Science, Год журнала: 2020, Номер 367(6474), С. 193 - 197

Опубликована: Янв. 10, 2020

Confining peroxide to make methanol In principle, hydrogen would be an efficient oxidant for the conversion of methane under mild conditions. practice, however, it is currently too expensive produce ahead time this purpose. Jin et al. report a catalyst system that generates and concentrates immediate reaction with methane. A hydrophobically coated zeolite keeps close gold palladium active site, where incoming then selectively oxidized methanol. Science , issue p. 193

Язык: Английский

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Direct Methane Conversion under Mild Condition by Thermo-, Electro-, or Photocatalysis

Chem, Год журнала: 2019, Номер 5(9), С. 2296 - 2325

Опубликована: Май 27, 2019

Язык: Английский

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Coupling of Solar Energy and Thermal Energy for Carbon Dioxide Reduction: Status and Prospects

Angewandte Chemie International Edition, Год журнала: 2019, Номер 59(21), С. 8016 - 8035

Опубликована: Июль 16, 2019

Enormous efforts have been devoted to the reduction of carbon dioxide (CO2 ) by utilizing various driving forces, such as heat, electricity, and radiation. However, efficient CO2 is still challenging because sluggish kinetics. Recent pioneering studies from several groups, including us, demonstrated that coupling solar energy thermal offers a novel promising strategy promote activity and/or manipulate selectivity in reduction. Herein, we clarify definition principles energy, comprehensively review status prospects energy. Catalyst design, reactor configuration, photo-mediated activity/selectivity, mechanism photo-thermo will be emphasized. The aim this Review understanding towards activation provide guidelines for design new catalysts .

Язык: Английский

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From Solar Energy to Fuels: Recent Advances in Light‐Driven C₁ Chemistry

Angewandte Chemie International Edition, Год журнала: 2019, Номер 58(49), С. 17528 - 17551

Опубликована: Март 2, 2019

Abstract Catalytic C 1 chemistry based on the activation/conversion of synthesis gas (CO+H 2 ), methane, carbon dioxide, and methanol offers great potential for sustainable development hydrocarbon fuels to replace oil, coal, natural gas. Traditional thermal catalytic processes used transformations require high temperatures pressures, thereby carrying a significant footprint. In comparison, solar‐driven catalysis greener more pathway manufacturing other commodity chemicals, although conversion efficiencies are currently too low justify industry investment. this Review, we highlight recent advances milestones in light‐driven chemistry, including solar Fischer–Tropsch synthesis, water‐gas‐shift reaction, CO hydrogenation, as well methane reactions. Particular emphasis is placed rational design catalysts, structure–reactivity relationships, reaction mechanisms. Strategies scaling up also discussed.

Язык: Английский

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Strategies and Challenges on Selectivity of Photocatalytic Oxidation of Organic Substances

Advanced Energy Materials, Год журнала: 2021, Номер 11(8)

Опубликована: Янв. 20, 2021

Abstract Most organic compounds are conventionally synthesized under high temperature and elevated pressure, resulting in significant energy consumption wastage. Heterogeneous photocatalytic oxidation has the potential to provide a green route for synthesis of majority industrially important chemicals. The major limiting factor affecting efficiency is lack selectivity; therefore, substantial effort been devoted solving this problem. Responding fast‐moving progress, review gives an overview fundamental understanding reactive oxygen species involved oxidations furthermore, general mechanisms few crucial reactions. focus critical on discussion diverse strategies improve selectivity value chemicals, including band engineering, metal loading, hybrid materials, defect with primary aim highlighting catalyst design protocols based reaction mechanism. Finally, difficulties challenges developing highly selective photocatalysts comprehensively discussed order help direct future research.

Язык: Английский

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Direct and Selective Photocatalytic Oxidation of CH₄ to Oxygenates with O₂ on Cocatalysts/ZnO at Room Temperature in Water

Journal of the American Chemical Society, Год журнала: 2019, Номер 141(51), С. 20507 - 20515

Опубликована: Дек. 13, 2019

Direct conversion of methane into methanol and other liquid oxygenates still confronts considerable challenges in activating the first C-H bond inhibiting overoxidation. Here, we report that ZnO loaded with appropriate cocatalysts (Pt, Pd, Au, or Ag) enables direct oxidation to formaldehyde water using only molecular oxygen as oxidant under mild light irradiation at room temperature. Up 250 micromoles ∼95% selectivity is achieved for 2 h over 10 mg 0.1 wt % Au. Experiments isotopically labeled reveal O2, rather than water, source CH4 oxidation. We find cocatalyst could concertedly activate O2 methyl radical mildly oxidative intermediate (hydroperoxyl radical) which are two key precursor intermediates generating oxygenated products Our study underlines equally significant aspects realizing selective photooxidation oxygenates, i.e., efficient activation controllable O2.

Язык: Английский

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Solar-Energy-Mediated Methane Conversion

Joule, Год журнала: 2019, Номер 3(7), С. 1606 - 1636

Опубликована: Июль 1, 2019

Язык: Английский

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Single-atom Cu anchored catalysts for photocatalytic renewable H2 production with a quantum efficiency of 56%

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Янв. 10, 2022

Abstract Single-atom catalysts anchoring offers a desirable pathway for efficiency maximization and cost-saving photocatalytic hydrogen evolution. However, the single-atoms loading amount is always within 0.5% in most of reported due to agglomeration at higher concentrations. In this work, highly dispersed large (>1 wt%) copper were achieved on TiO 2 , exhibiting H evolution rate 101.7 mmol g −1 h under simulated solar light irradiation, which than other photocatalysts reported, addition excellent stability as proved after storing 380 days. More importantly, it exhibits an apparent quantum 56% 365 nm, significant breakthrough field. The Cu incorporation enables efficient electron transfer via 2+ -Cu + process. present approach paves way design advanced materials remarkable activity durability.

Язык: Английский

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Two-dimensional photocatalyst design: A critical review of recent experimental and computational advances

Materials Today, Год журнала: 2019, Номер 34, С. 78 - 91

Опубликована: Дек. 20, 2019

Язык: Английский

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