Technologies and perspectives for achieving carbon neutrality

The Innovation, Год журнала: 2021, Номер 2(4), С. 100180 - 100180

Опубликована: Окт. 30, 2021

Язык: Английский

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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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Identification of Halogen-Associated Active Sites on Bismuth-Based Perovskite Quantum Dots for Efficient and Selective CO₂-to-CO Photoreduction

ACS Nano, Год журнала: 2020, Номер 14(10), С. 13103 - 13114

Опубликована: Сен. 17, 2020

All-inorganic Pb-free bismuth (Bi) halogen perovskite quantum dots (PQDs) with distinct structural and photoelectric properties provide plenty of room for selective photoreduction CO2. However, the efficient conversion CO2-to-CO high selectivity on Bi-based PQDs driven by solar light remains unachieved, precise reaction path/mechanism promoted surface halogen-associated active sites is still poorly understood. Herein, we screen a series nontoxic stable Cs3Bi2X9 (X = Cl, Br, I) photocatalytic reduction at gas-solid interface. Among all reported pure-phase PQDs, as-synthesized Cs3Bi2Br9 exhibited highest efficiency generating 134.76 μmol g-1 CO yield 98.7% under AM 1.5G simulated illumination. The intermediates were dynamically monitored precisely unraveled based in situ DRIFTS investigation. In combination DFT calculation, it was revealed that Br allow optimizing coordination modes surface-bound intermediate species reducing energy rate-limiting step COOH- formation from •CO2-. This work presents mechanistic insight into halogen-involved catalytic mechanism fuel production.

Язык: Английский

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A Review on MXene Synthesis, Stability, and Photocatalytic Applications

ACS Nano, Год журнала: 2022, Номер 16(9), С. 13370 - 13429

Опубликована: Сен. 12, 2022

Photocatalytic water splitting, CO2 reduction, and pollutant degradation have emerged as promising strategies to remedy the existing environmental energy crises. However, grafting of expensive less abundant noble-metal cocatalysts on photocatalyst materials is a mandatory practice achieve enhanced photocatalytic performance owing ability extract electrons efficiently from enable rapid/enhanced catalytic reaction. Hence, developing highly efficient, inexpensive, noble-metal-free composed earth-abundant elements considered noteworthy step toward considering photocatalysis more economical strategy. Recently, MXenes (two-dimensional (2D) transition-metal carbides, nitrides, carbonitrides) shown huge potential alternatives for cocatalysts. several excellent properties, including atomically thin 2D morphology, metallic electrical conductivity, hydrophilic surface, high specific surface area. In addition, they exhibit Gibbs free intermediate H atom adsorption close zero than that commercial Pt-based cocatalyst, Fermi level position above H2 generation potential, an capture activate molecules. Therefore, there growing interest in MXene-based various events. this review, we focus recent advances synthesis with 0D morphologies, stability MXenes, photocatalysts evolution, degradation. The challenges possible future directions enhance are 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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Photocatalytic C–C Coupling from Carbon Dioxide Reduction on Copper Oxide with Mixed-Valence Copper(I)/Copper(II)

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(7), С. 2984 - 2993

Опубликована: Фев. 11, 2021

To realize the evolution of C2+ hydrocarbons like C2H4 from CO2 reduction in photocatalytic systems remains a great challenge, owing to gap between relatively lower efficiency multielectron transfer photocatalysis and sluggish kinetics C–C coupling. Herein, with Cu-doped zeolitic imidazolate framework-8 (ZIF-8) as precursor, hybrid photocatalyst (CuOX@p-ZnO) CuOX uniformly dispersed among polycrystalline ZnO was synthesized. Upon illumination, catalyst exhibited ability reduce 32.9% selectivity, rate 2.7 μmol·g–1·h–1 water hole scavenger high 22.3 presence triethylamine sacrificial agent, all which have rarely been achieved systems. The X-ray absorption fine structure spectra coupled situ FT-IR studies reveal that, original catalyst, Cu mainly existed form CuO, while unique Cu+ surface layer upon CuO matrix formed during reaction, this site is active anchor generated CO further perform coupling C2H4. intermediate *OC–COH experimentally identified by for first time reduction. Moreover, theoretical calculations showed critical role such sites strengthening binding *CO stabilizing intermediate. This work uncovers new paradigm achieve system.

Язык: Английский

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Photocatalytic CO2 reduction

Nature Reviews Methods Primers, Год журнала: 2023, Номер 3(1)

Опубликована: Авг. 10, 2023

Язык: Английский

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Photocatalytic CO₂Reduction: A Review of Ab Initio Mechanism, Kinetics, and Multiscale Modeling Simulations

ACS Catalysis, Год журнала: 2020, Номер 10(24), С. 14984 - 15007

Опубликована: Дек. 7, 2020

Climate change has prompted scientists to search for possible ways of reducing CO2 emissions or even capturing it from the atmosphere. Catalytic reduction into value-added chemicals been put forward as a viable strategy. While thermocatalytic routes producing CO, methanol, methane, and higher hydrocarbons have focus considerable research efforts, photocatalytic conversion is an emerging approach. Photoactivation potential greener process because could be carried out at lower temperatures pressures, decreasing energy consumption. The recent advent available computational power tools made study reaction in silico catalyst prediction mechanism elucidation. In this Review, we thus on ab initio comparison with experiments. most commonly used materials are variously doped TiO2, g-C3N4, perovskites, which favorable optical properties their own. Their efficiency mostly governed by band gap, charge separation, transfer. characteristics can improved, catalysts tailored specific use doping, introduction defects (such oxygen vacancies geometric effects), cocatalysts, using Z-scheme catalysts. Most theoretical studies calculations conduction valence bands, adsorption energies. Some try describe mechanism. Few go beyond hybrid-functional DFT approach explicitly model effect electron excitation. description excited states post-DFT methods, yet applied problem photoreduction larger scale. We conclude Review outlook how current state-of-the-art improving existing

Язык: Английский

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Insight on Reaction Pathways of Photocatalytic CO₂ Conversion

ACS Catalysis, Год журнала: 2022, Номер 12(12), С. 7300 - 7316

Опубликована: Июнь 3, 2022

Photocatalytic CO2 conversion to value-added chemicals is a promising solution mitigate the current energy and environmental issues but challenging process. The main obstacles include inertness of molecule, sluggish multi-electron process, unfavorable thermodynamics, selectivity control preferable products. Furthermore, lack fundamental understanding reaction pathways accounts for very moderate performance in field. Therefore, this Perspective, we attempt discuss possible mechanisms toward all C1 C2 products, taking into account experimental evidence theoretical calculation on surface adsorption, proton electron transfer, products desorption. Finally, remaining challenges field, including mechanistic understanding, reactor design, economic consideration, potential solutions, are critically discussed by us.

Язык: Английский

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S-scheme heterojunction photocatalysts for CO2 reduction

Matter, Год журнала: 2022, Номер 5(12), С. 4187 - 4211

Опубликована: Дек. 1, 2022

Язык: Английский

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