Solar fuels: research and development strategies to accelerate photocatalytic CO₂ conversion into hydrocarbon fuels

Energy & Environmental Science, Год журнала: 2021, Номер 15(3), С. 880 - 937

Опубликована: Ноя. 16, 2021

Photocatalytic CO 2 conversion is vital technology to realize global carbon neutrality and generate future energy supplies. This review proposes fundamentals, challenges, strategies, prospects for photocatalytic research.

Язык: Английский

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Synergistic Effect of Cu Single Atoms and Au–Cu Alloy Nanoparticles on TiO₂ for Efficient CO₂ Photoreduction

ACS Nano, Год журнала: 2021, Номер 15(9), С. 14453 - 14464

Опубликована: Сен. 1, 2021

The synergy between metal alloy nanoparticles (NPs) and single atoms (SAs) should maximize the catalytic activity. However, there are no relevant reports on photocatalytic CO2 reduction via utilizing SAs NPs. Herein, we developed a facile photodeposition method to coload Cu Au–Cu NPs TiO2 for synthesis of solar fuels with H2O. optimized photocatalyst achieved record-high performance formation rates 3578.9 CH4 369.8 μmol g–1 h–1 C2H4, making it significantly more realistic implement sunlight-driven value-added fuels. combined in situ FT-IR spectra DFT calculations revealed molecular mechanisms C–C coupling form C2H4. We proposed that synergistic function could enhance adsorption activation H2O lower overall energy barrier (including rate-determining step) C2H4 formation. These factors all enable highly efficient stable production concept alloys cocatalysts can be extended other systems, thus contributing development effective cocatalysts.

Язык: Английский

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Engineering Single-Atom Active Sites on Covalent Organic Frameworks for Boosting CO₂ Photoreduction

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(37), С. 17097 - 17109

Опубликована: Сен. 6, 2022

Solar carbon dioxide (CO2) conversion is an emerging solution to meet the challenges of sustainable energy systems and environmental/climate concerns. However, construction isolated active sites not only influences catalytic activity but also limits understanding structure-catalyst relationship CO2 reduction. Herein, we develop a universal synthetic protocol fabricate different single-atom metal (e.g., Fe, Co, Ni, Zn, Cu, Mn, Ru) anchored on triazine-based covalent organic framework (SAS/Tr-COF) backbone with bridging structure metal-nitrogen-chlorine for high-performance Remarkably, as-synthesized Fe SAS/Tr-COF as representative catalyst achieved impressive CO generation rate high 980.3 μmol g-1 h-1 selectivity 96.4%, over approximately 26 times higher than that pristine Tr-COF under visible light irradiation. From X-ray absorption fine analysis density functional theory calculations, superior photocatalytic performance attributed synergic effect atomically dispersed host, decreasing reaction barriers formation *COOH intermediates promoting adsorption activation well desorption. This work affords rational design state-of-the-art catalysts at molecular level provides in-depth insights efficient conversion.

Язык: Английский

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ZnSe Nanorods–CsSnCl₃ Perovskite Heterojunction Composite for Photocatalytic CO₂ Reduction

ACS Nano, Год журнала: 2022, Номер 16(2), С. 3332 - 3340

Опубликована: Фев. 4, 2022

Utilizing sunlight to convert CO2 into chemical fuels could simultaneously address the greenhouse effect and fossil fuel crisis. ZnSe nanocrystals are promising candidates for photocatalysis because of their low toxicity excellent photoelectric properties. However, pristine generally has catalytic activities due serious charge recombination lack efficient sites reduction. Herein, a nanorods-CsSnCl3 perovskite (ZnSe-CsSnCl3) type II heterojunction composite is designed prepared photocatalytic The ZnSe-CsSnCl3 exhibits enhanced activity reduction with respect nanorods. experimental characterizations theoretical calculations reveal that separation lowered free energy facilitate conversion on composite. This work presents photocatalyst based ecofriendly metal chalcogenides halide perovskites. Our study also promoted understanding mechanisms nanocrystals, which be valuable development photocatalysts.

Язык: Английский

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2D/2D BiVO4/CsPbBr3 S-scheme heterojunction for photocatalytic CO2 reduction: Insights into structure regulation and Fermi level modulation

Applied Catalysis B Environment and Energy, Год журнала: 2021, Номер 304, С. 120979 - 120979

Опубликована: Дек. 4, 2021

Язык: Английский

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Dual‐Single‐Atom Tailoring with Bifunctional Integration for High‐Performance CO₂ Photoreduction

Advanced Materials, Год журнала: 2021, Номер 33(49)

Опубликована: Окт. 7, 2021

Single-atom photocatalysis has been demonstrated as a novel strategy to promote heterogeneous reactions. There is diversity of monoatomic metal species with specific functions; however, integrating representative merits into dual-single-atoms and regulating cooperative remain pressing challenge. For dual-single-atom catalysts, enhanced photocatalytic activity would be realized through bifunctional properties tuning the synergistic effect. Herein, supported on conjugated porous carbon nitride polymer are developed for effective CO2 reduction, featuring function cobalt (Co) ruthenium (Ru). A series in situ characterizations theoretical calculations conducted quantitative analysis structure-performance correlation. It concluded that active Co sites facilitate dynamic charge transfer, while Ru selective surface-bound interaction during photoreduction. The combination atom-specific traits synergy between lead high conversion corresponding apparent quantum efficiency (AQE) 2.8% at 385 nm, along turnover number (TON) more than 200 without addition any sacrificial agent. This work presents an example identifying roles different single-atom metals synergy, where two unique collaborate further boost performance.

Язык: Английский

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Selective photocatalytic CO2 reduction in aerobic environment by microporous Pd-porphyrin-based polymers coated hollow TiO2

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

Опубликована: Март 17, 2022

Abstract Direct photocatalytic CO 2 reduction from primary sources, such as flue gas and air, into fuels, is highly desired, but the thermodynamically favored O almost completely impedes this process. Herein, we report on efficacy of a composite photocatalyst prepared by hyper-crosslinking porphyrin-based polymers hollow TiO surface subsequent coordinating with Pd(II). Such exhibits high resistance against inhibition, leading to 12% conversion yield air after 2-h UV-visible light irradiation. In contrast, over Pd/TiO without polymer severely inhibited presence ( ≥ 0.2 %). This study presents feasible strategy, building Pd(II) sites -adsorptive surface, for realizing H in an aerobic environment /O adsorption selectivity efficient charge separation oxidation , respectively.

Язык: Английский

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Interfacial Engineering of Bi₁₉Br₃S₂₇ Nanowires Promotes Metallic Photocatalytic CO₂ Reduction Activity under Near-Infrared Light Irradiation

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(17), С. 6551 - 6559

Опубликована: Апрель 14, 2021

Developing highly efficient photocatalysts to utilize solar radiation for converting CO2 into fuels is of great importance energy sustainability and carbon neutralization. Herein, through an alkali-etching-introduced interface reconstruction strategy, a nanowire photocatalyst denoted as V–Bi19Br3S27, with rich Br S dual-vacancies surface Bi–O bonding introduced significant near-infrared (NIR) light response, has been developed. The as-obtained V–Bi19Br3S27 nanowires exhibit metallic photocatalytic reduction property CH3OH when excited solely under NIR irradiation. Free any cocatalyst sacrificial agent, defective shows 2.3-fold higher generation than Bi19Br3S27 nanowires. detailed interfacial structure evolution reaction mechanism have carefully illustrated down the atomic scale. This work provides unique engineering strategy developing high-performance sulfur-based photon reducing alcohol achieving high-value fuel chemicals, which paves way efficiently using extending range achieve neutralization goal.

Язык: Английский

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A-site perovskite oxides: an emerging functional material for electrocatalysis and photocatalysis

Journal of Materials Chemistry A, Год журнала: 2021, Номер 9(11), С. 6650 - 6670

Опубликована: Янв. 1, 2021

This review summarizes the recent progress of A-site perovskite oxides as an emerging functional material for electrocatalysis and photocatalysis applications.

Язык: Английский

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Graphene aerogel-based NiAl-LDH/g-C3N4 with ultratight sheet-sheet heterojunction for excellent visible-light photocatalytic activity of CO2 reduction

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 306, С. 121065 - 121065

Опубликована: Янв. 21, 2022

Язык: Английский

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