Isolated Cu Sites in CdS Hollow Nanocubes with Doping-Location-Dependent Performance for Photocatalytic CO₂ Reduction

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(3), P. 1468 - 1479

Published: Jan. 13, 2024

Doping engineering has enabled the construction of homogeneous and abundant atomic-level catalytic sites for photocatalytic CO2 reduction with improved selectivity target product. However, little is known about effect spatial position heteroatoms on activity semiconductors toward reduction. Herein, uniform Cu doping into bulk phase hollow CdS cubes (HCC) onto surface HCC, denoted as Cu/HCC HCC@Cu, respectively, are prepared by tuning introduction order sources. Experimental analysis shows that both methods can promote separation migration photoinduced charge carriers in CdS. Notably, HCC@Cu leads to much better proton H2 production performance but lower efficiency compared bare In sharp contrast, enhances CO2-to-CO conversion while mitigating evolution. This should be ascribed smaller overpotential saturated system than Ar system. addition, atoms shifts d band center upward near Fermi energy level, which promotes adsorption activation These results indicate photoelectrons a prolonged lifetime preferably reduce molecules rather protons. The density functional theory (DFT) calculation show desorption CO*, adaptable sulfur vacancies (Vs) produced situ techniques stimulate formation CO* intermediates, resulting high CO. work reveals different heteroatom locations will provide reference design efficient photocatalysts fine structure.

Language: Английский

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Solar-driven sugar production directly from CO2 via a customizable electrocatalytic–biocatalytic flow system

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 25, 2024

Abstract Conventional food production is restricted by energy conversion efficiency of natural photosynthesis and demand for resources. Solar-driven artificial synthesis from CO 2 provides an intriguing approach to overcome the limitations while promoting carbon-neutral economy, however, it remains very challenging. Here, we report design a hybrid electrocatalytic−biocatalytic flow system, coupling photovoltaics-powered electrocatalysis (CO formate) with five-enzyme cascade platform (formate sugar) engineered via genetic mutation bioinformatics, which achieves C 6 sugar (L-sorbose) solar-to-food 3.5%, outperforming over three-fold. This system can in principle be programmed diverse enzymes toward multifarious . work opens promising avenue under confined environments.

Language: Английский

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Challenges and Prospects in the Catalytic Conversion of Carbon Dioxide to Formaldehyde

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(46)

Published: Sept. 6, 2022

Formaldehyde (HCHO) is a crucial C

Language: Английский

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High entropy materials frontier and theoretical insights for logistics CO2 reduction and hydrogenation: Electrocatalysis, photocatalysis and thermo-catalysis

Journal of Alloys and Compounds, Journal Year: 2023, Volume and Issue: 969, P. 172232 - 172232

Published: Sept. 20, 2023

Language: Английский

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Donor‐Acceptor Activation of Carbon Dioxide

Chemistry - A European Journal, Journal Year: 2023, Volume and Issue: 29(61)

Published: July 26, 2023

Abstract The activation and functionalization of carbon dioxide entails great interest related to its abundance, low toxicity associated environmental problems. However, the inertness CO 2 has posed a challenge towards efficient conversion added‐value products. In this review we discuss one strategies that have been widely used capture activate dioxide, namely use donor‐acceptor interactions by partnering Lewis acidic basic fragment. This type resembles found in metalloenzymes, whose outstanding performance catalytically transforming encourages further bioinspired research. We divided into three general sections based on nature active sites: metal‐free examples (mainly formed frustrated pairs), main group‐transition metal combinations, transition heterobimetallic complexes. Overall, hundred compounds cooperatively interactions, revealing wide range structural motifs.

Language: Английский

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Rational Design of Heterogeneous Dual-Atom Catalysts for CO₂ Electroreduction Reactions

ACS Applied Energy Materials, Journal Year: 2023, Volume and Issue: 6(13), P. 6851 - 6882

Published: June 23, 2023

One of the strategies to mitigate concentration CO2 in atmosphere and reduce global warming effect is capture convert it synthetic fuels fine chemicals. Although structurally chemically stable, electrochemical transformation has attracted much attention because offers mild reaction conditions regarding temperature, pressure, process controllability. Among various electrocatalysts, dual-atom catalysts (DACs) have been extensively developed past few years due their unique features for reactions small molecules. The catalytic activity DACs reduction (eCO2RR) surpassed single-atom (SACs) by providing a higher metal loading, two active sites (cf. one site SACs), synergistic adjacent atoms, possibility tuning electronic state (adjusting d-band center), more possible configuration modes (side-on side-bridge) adsorption only end-on end-bridge SACs). As result, both reactivity selectivity eCO2RR can be achieved breaking scaling relationships with interactions between intermediates sites. This review highlights discusses recent progress applying homo- heteronuclear focusing on synthesis, characterization, performance.

Language: Английский

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The CO₂ Tree: The Potential for Carbon Dioxide Utilization Pathways

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 13(1), P. 5 - 29

Published: Dec. 13, 2024

Among the most active areas of chemistry research today is that carbon dioxide utilization: an area was viewed as futile and commercially impractical not so long ago due to energetic stability CO2 molecule. The breakthroughs largely began in earnest 1990s have accelerated now make up a diverse plentiful portfolio technological scientific advances commercialized technologies. Here, "The Tree" presented tool illustrate breadth potential products from utilization communicate these chemical address greatest challenge society faces today: climate change. It intended be useful for scientists, engineers, legislators, advocates, industrial decision-makers, policy makers, general public know what already possible may near future.

Language: Английский

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Theory-guided development of homogeneous catalysts for the reduction of CO₂to formate, formaldehyde, and methanol derivatives

Chemical Science, Journal Year: 2023, Volume and Issue: 14(11), P. 2799 - 2807

Published: Jan. 1, 2023

Computational volcano plots are used to predict selectivity in the context of (first-row) transition metal-catalyzed CO 2 reduction. The expected trends were tested experimentally and allowed for systematic improvement catalyst.

Language: Английский

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Paired Electrosynthesis of Formaldehyde Derivatives from CO₂ Reduction and Methanol Oxidation

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(2)

Published: Nov. 29, 2023

Abstract Utilizing CO 2 ‐derived formaldehyde derivatives for fuel additive or polymer synthesis is a promising approach to reduce net carbon dioxide emissions. Existing methodologies involve converting methanol by thermal hydrogenation, followed electrochemical thermochemical oxidation produce formaldehyde. Adding the conventional pathway, we propose new simultaneously generate at both electrodes partial and direct reduction of . To achieve this, method directly cathode required. Still, it has been scarcely reported previously due acidity formic acid intermediate facile over‐reduction methanol. By enabling activation subsequent stabilization respectively in solvent, were able implement strategy where generated alongside anode. Further mechanism studies revealed that protons supplied from anodic reaction contribute product. Additionally, was found cathodic derivative Faradaic efficiency can be further increased through prolonged electrolysis time up 50 % along with maximum 90 %.

Language: Английский

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Biotransforming CO2 into valuable chemicals

Journal of Cleaner Production, Journal Year: 2023, Volume and Issue: 434, P. 140185 - 140185

Published: Dec. 15, 2023

Language: Английский

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