Toward solar-driven carbon recycling

Joule, Год журнала: 2022, Номер 6(2), С. 294 - 314

Опубликована: Янв. 31, 2022

Carbon recycling will become a dominant trend toward alleviating extreme climate change and coping with the increasing energy demand in coming years. Solar-driven strategies have potential to convert CO2 solar fuels chemicals. In this forward-looking perspective, framework is outlined achieve "net-zero emission" blueprint by sorting out raw sources, products, feasible pathways, practical implementation through photocatalysis, photothermal catalysis, photoelectrochemical catalysis techniques. We comprehensively inspect compare state-of-art works framework, including solar-driven C1 fuel production from CO2, as well direct stepwise C2+ involving conversion. This analysis aspires provide most pathway forward finds that converting renewable H2 into can currently obtain best solar-to-fuel conversion efficiency target products high selectivity. Future visions on scientific, technological, economic issues are put determine what should be focus following decades.

Язык: Английский

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Developing Ni single-atom sites in carbon nitride for efficient photocatalytic H2O2 production

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 6, 2023

Photocatalytic two-electron oxygen reduction to produce high-value hydrogen peroxide (H2O2) is gaining popularity as a promising avenue of research. However, structural evolution mechanisms catalytically active sites in the entire photosynthetic H2O2 system remains unclear and seriously hinders development highly-active stable photocatalysts. Herein, we report high-loading Ni single-atom photocatalyst for efficient synthesis pure water, achieving an apparent quantum yield 10.9% at 420 nm solar-to-chemical conversion efficiency 0.82%. Importantly, using situ synchrotron X-ray absorption spectroscopy Raman directly observe that initial Ni-N3 dynamically transform into high-valent O1-Ni-N2 after O2 adsorption further evolve form key *OOH intermediate before finally forming HOO-Ni-N2. Theoretical calculations experiments reveal structure reduces formation energy barrier suppresses O=O bond dissociation, leading improved production activity selectivity.

Язык: Английский

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Thermo-photo catalysis: a whole greater than the sum of its parts

Chemical Society Reviews, Год журнала: 2022, Номер 51(9), С. 3609 - 3647

Опубликована: Янв. 1, 2022

This review provides an up-to-date understanding on emerging thermo-photo catalytic processes with emphasis the synergetic effects of thermal and photo energies.

Язык: Английский

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Active Site Engineering on Plasmonic Nanostructures for Efficient Photocatalysis

ACS Nano, Год журнала: 2023, Номер 17(5), С. 4193 - 4229

Опубликована: Фев. 20, 2023

Plasmonic nanostructures have shown immense potential in photocatalysis because of their distinct photochemical properties associated with tunable photoresponses and strong light–matter interactions. The introduction highly active sites is essential to fully exploit the plasmonic photocatalysis, considering inferior intrinsic activities typical metals. This review focuses on site-engineered enhanced photocatalytic performance, wherein are classified into four types (i.e., metallic sites, defect ligand-grafted interface sites). synergy between discussed detail after briefly introducing material synthesis characterization methods. Active can promote coupling solar energy harvested by metal catalytic reactions form local electromagnetic fields, hot carriers, photothermal heating. Moreover, efficient potentially regulates reaction pathway facilitating excited state formation reactants, changing status creating additional using photoexcited Afterward, application emerging summarized. Finally, a summary perspective existing challenges future opportunities presented. aims deliver some insights from expediting discovery high-performance photocatalysts.

Язык: Английский

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Mo₂TiC₂ MXene-Supported Ru Clusters for Efficient Photothermal Reverse Water–Gas Shift

ACS Nano, Год журнала: 2022, Номер 17(2), С. 1550 - 1559

Опубликована: Дек. 30, 2022

Driving metal-cluster-catalyzed high-temperature chemical reactions by sunlight holds promise for the development of negative-carbon-footprint industrial catalysis, which has yet often been hindered poor ability metal clusters to harvest and utilize full spectrum solar energy. Here, we report preparation Mo2TiC2 MXene-supported Ru (Ru/Mo2TiC2) with pronounced broadband absorption high sintering resistance. Under illumination focused sunlight, Ru/Mo2TiC2 can catalyze reverse water–gas shift (RWGS) reaction produce carbon monoxide from greenhouse gas dioxide renewable hydrogen enhanced activity, selectivity, stability compared their nanoparticle counterparts. Notably, CO production rate reached 4.0 mol·gRu–1·h–1, is among best reported so far photothermal RWGS catalysts. Detailed studies suggest that methane kinetically inhibited rapid desorption surface clusters.

Язык: Английский

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Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts

Nature Energy, Год журнала: 2023, Номер 8(9), С. 1013 - 1022

Опубликована: Авг. 17, 2023

Abstract Photocatalytic oxidative coupling of methane (OCM) produces C 2 molecules that can be used as building blocks for synthesis fuels and chemicals. However, the yield rate selectivity products are still moderate due to stable nature molecules. Here we develop a Au nanocluster-loaded TiO photocatalyst by sputtering approach, achieving high conversion 1.1 mmol h −1 , ~90% apparent quantum efficiency 10.3 ± 0.6%. The /C 2+ is on same order magnitude benchmark thermal catalysts in OCM processes operated at temperature (>680 °C). nanoparticles shown prolong photoelectron lifetimes factor 66 O reduction, together with acting hole acceptor catalytic centre promote adsorption, C–H activation C–C coupling. This work underscores importance multifunctional co-catalysts mechanistic understanding improve photocatalytic OCM.

Язык: Английский

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Spatial Decoupling of Redox Chemistry for Efficient and Highly Selective Amine Photoconversion to Imines

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(13), С. 7181 - 7189

Опубликована: Март 24, 2023

Light-driven primary amine oxidation to imines integrated with H2 production presents a promising means simultaneous of high-value-added fine chemicals and clean fuels. Yet, the effectiveness this strategy is generally limited by poor charge separation photocatalysts uncontrolled hydrogenation secondary amines. Herein, spatial decoupling proposed isolate redox chemistry at distinct sites photocatalysts, CoP core–ZnIn2S4 shell (CoP@ZnIn2S4) coaxial nanorods are assembled as proof-of-concept photocatalyst. Directional ultrafast carrier occurs between core ZnIn2S4 shell, confirmed in situ X-ray photoelectron spectroscopy, surface photovoltage transient absorption spectroscopy analyses. Toward photoconversion model substrate benzylamine N-benzylbenzaldimine, CoP@ZnIn2S4 exhibits 48-time higher rate >99% selectivity when compared (ca. 20% selectivity), detailed reaction mechanism has been verified diffuse reflectance infrared Fourier transform spectroscopy.

Язык: Английский

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Tailoring the oxidation state of metallic TiO through Ti3+/Ti2+ regulation for photocatalytic conversion of CO2 to C2H6

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 307, С. 121141 - 121141

Опубликована: Янв. 25, 2022

Язык: Английский

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Selective Photocatalytic Oxidative Coupling of Methane via Regulating Methyl Intermediates over Metal/ZnO Nanoparticles

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

Опубликована: Апрель 7, 2023

Abstract Methane conversion to higher hydrocarbons requires harsh reaction conditions due high energy barriers associated with C−H bond activation. Herein, we report a systematic investigation of photocatalytic oxidative coupling methane (OCM) over transition‐metal‐loaded ZnO photocatalysts. A 1 wt % Au/ZnO delivered remarkable C 2 ‐C 4 hydrocarbon production rate 683 μmol g −1 h (83 selectivity) under light irradiation excellent photostability two days. The metal type and its interaction strongly influence the selectivity toward C−C products. Photogenerated Zn + ‐O − sites enable CH activation methyl intermediates (*CH 3 ) migrating onto adjacent nanoparticles. nature *CH ‐metal controls OCM In case Au, strong d‐σ orbital hybridization reduces metal‐C−H angles steric hindrance, thereby enabling efficient coupling. Findings indicate center may be suitable descriptor for predicting product during metal/ZnO

Язык: Английский

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Catalyzing Artificial Photosynthesis with TiO₂ Heterostructures and Hybrids: Emerging Trends in a Classical yet Contemporary Photocatalyst

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Окт. 11, 2023

Titanium dioxide (TiO

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