Recent advances of single-atom catalysts in CO₂conversion

Energy & Environmental Science, Год журнала: 2023, Номер 16(7), С. 2759 - 2803

Опубликована: Янв. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

Язык: Английский

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Co⁰−Co^δ+ Interface Double‐Site‐Mediated C−C Coupling for the Photothermal Conversion of CO₂ into Light Olefins

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(23)

Опубликована: Апрель 4, 2023

Solar-driven CO2 hydrogenation into multi-carbon products is a highly desirable, but challenging reaction. The bottleneck of this reaction lies in the C-C coupling C1 intermediates. Herein, we construct centre for intermediates via situ formation Co0 -Coδ+ interface double sites on MgAl2 O4 (Co-CoOx /MAO). Our experimental and theoretical prediction results confirmed effective adsorption activation by site to produce intermediates, while introduction electron-deficient state Coδ+ can effectively reduce energy barrier key CHCH* Consequently, Co-CoOx /MAO exhibited high C2-4 hydrocarbons production rate 1303 μmol g-1 h-1 ; total organic carbon selectivity 62.5 % under light irradiation with ratio (≈11) olefin paraffin. This study provides new approach toward design photocatalysts used conversion C2+ products.

Язык: Английский

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Manipulating the Spin State of Co Sites in Metal–Organic Frameworks for Boosting CO₂ Photoreduction

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(5), С. 3241 - 3249

Опубликована: Янв. 26, 2024

Photocatalytic CO2 reduction holds great potential for alleviating global energy and environmental issues, where the electronic structure of catalytic center plays a crucial role. However, spin state, key descriptor properties, is largely overlooked. Herein, we present simple strategy to regulate states Co centers by changing their coordination environment exchanging species into stable Zn-based metal–organic framework (MOF) afford Co-OAc, Co-Br, Co-CN photoreduction. Experimental DFT calculation results suggest that distinct sites give rise different charge separation abilities barriers adsorption/activation in photocatalysis. Consequently, optimized Co-OAc with highest spin-state presents an excellent photocatalytic activity 2325.7 μmol·g–1·h–1 selectivity 99.1% CO, which are among best all reported MOF photocatalysts, absence noble metal additional photosensitizer. This work underlines MOFs as ideal platform manipulation toward improved

Язык: Английский

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Cooperative Ni(Co)‐Ru‐P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self‐powered H₂ Production

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(35)

Опубликована: Июль 10, 2023

Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using thermodynamically more favorable hydrazine oxidation (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1 -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen (HER), realizing an ultralow working potential of -60 mV overpotential 32 current density 10 mA cm-2 , respectively. Inspiringly, two-electrode electrolyzer based on overall splitting (OHzS) demonstrates outstanding activity record-high 522 at cell voltage 0.3 V. DFT calculations elucidate cooperative Ni(Co)-Ru-P sites in Ru1 -NiCoP optimize H* adsorption, enhance adsorption *N2 significantly lower energy barrier dehydrogenation. Moreover, self-powered system utilizing OHzS device driven direct fuel (DHzFC) achieve satisfactory rate 24.0 mol h-1 m-2 .

Язык: Английский

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Interfacial oxygen vacancy modulated Ag3PO4 @MoS2 Z-scheme system for efficient photocatalytic hydrogen recovery from antibiotic wastewater

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 330, С. 122584 - 122584

Опубликована: Март 6, 2023

Язык: Английский

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Recent progress and challenges of photocatalytic CO2 conversion into value-added multi-carbon products

Coordination Chemistry Reviews, Год журнала: 2023, Номер 502, С. 215623 - 215623

Опубликована: Дек. 27, 2023

Язык: Английский

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Renaissance of elemental phosphorus materials: properties, synthesis, and applications in sustainable energy and environment

Chemical Society Reviews, Год журнала: 2023, Номер 52(16), С. 5388 - 5484

Опубликована: Янв. 1, 2023

This review summarizes the advancements in elemental phosphorus materials, focusing on fundamental physicochemical properties, synthesis, and applications sustainable energy environment.

Язык: Английский

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Unspecific peroxygenases immobilized on Pd-loaded three-dimensional ordered macroporous (3DOM) titania photocatalyst for photo-enzyme integrated catalysis

Applied Catalysis B Environment and Energy, Год журнала: 2023, Номер 330, С. 122622 - 122622

Опубликована: Март 13, 2023

Язык: Английский

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Ruthenium Single Atomic Sites Surrounding the Support Pit with Exceptional Photocatalytic Activity

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(21)

Опубликована: Апрель 1, 2024

Abstract Single‐metal atomic sites and vacancies can accelerate the transfer of photogenerated electrons enhance photocatalytic performance in photocatalysis. In this study, a series nickel hydroxide nanoboards (Ni(OH) x NBs) with different loadings single‐atomic Ru ( w ‐SA‐Ru/Ni(OH) ) were synthesized via photoreduction strategy. such catalysts, are anchored to surrounding pits. Notably, SA‐Ru/Ni(OH) 0.60 wt % loading (0.60‐SA‐Ru/Ni(OH) exhibits highest catalytic (27.6 mmol g −1 h during reduction CO 2 (CO RR). Either superfluous (0.64 %, 18.9 ; 3.35 9.4 or scarce (0.06 15.8 0.29 21.95 0.58 23.4 have negative effect on its properties. Density functional theory (DFT) calculations combined experimental results revealed that be adsorbed pits; help conversion as‐adsorbed lower energy *COOH formation accelerating reaction; excessive occupy retard completion RR.

Язык: Английский

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Insight into the Selectivity-Determining Step of Various Photocatalytic CO₂ Reduction Products by Inorganic Semiconductors

ACS Catalysis, Год журнала: 2024, Номер 14(14), С. 10760 - 10788

Опубликована: Июль 3, 2024

Язык: Английский

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