Defect-Mediated Cu–S Pair Active Sites Modulating Proton Supply to Facilitate Overall CO<sub>2</sub> Photoreduction with H<sub>2</sub>O

Cao, Heng; Zhu, Xiaodi; Xue, Jiawei; Wang, Ruyang; Shang, Jiusi; Ma, Peiyu; Liu, Chengyuan; Bao, Jun

doi:10.1021/acscatal.4c02857

ACS Catal.

2024

DOI: 10.1021/acscatal.4c02857

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Defect-Mediated Cu–S Pair Active Sites Modulating Proton Supply to Facilitate Overall CO₂ Photoreduction with H₂O

Heng Cao,

Xiaodi Zhu,

Jiawei Xue

et al.

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Cited by 5 publications

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Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO₂ Reduction to Propylene Under Visible Light Illumination

Huang,

Chen,

Xie

et al. 2024

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The use of sunlight to convert CO2 into multi‐carbon fuels, particularly propylene, is considered a sustainable carbon cycle pathway, but propylene requires a multi‐electron‐coupled proton reaction process that has not been reported. Herein, two covalent organic frameworks (DA‐COF and DP‐COF) are prepared by varying the bridging positions of anthraquinone conjugated units. The experimental results show that the neighbouring bridge in DA‐COF forms a unique cleavage structure like an enzyme catalyst, which can provide an efficient microenvironment for the reduction reaction to trap protons. At the same time, the neighbor bridging in DA‐COF can form an electron donor‐electron acceptor structure to accelerate the photogenerated carrier migration. As a result, DA‐COF exhibits excellent visible light propylene production with a yield of 270.54 µmol g−1 and no C₃H₆ product is detected by the DP‐COF during the reduction process. This study presents a novel avenue for the production of high value‐added multi‐carbon products using photocatalysis.

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Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO₂ Reduction to Propylene Under Visible Light Illumination

Huang,

Chen,

Xie

et al. 2024

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Single‐Atom Pt Anchored Polyoxometalate as Electron‐Proton Shuttle for Efficient Photoreduction of CO₂ to CH₄ Catalyzed by NiCo Layered Doubled Hydroxide

Cai,

Hu,

Chen

et al. 2024

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The crucial role of active hydrogen (H*) in photocatalytic CO2 methanation has long been overlooked, although recently, accelerating proton‐coupled electron transfer (PCET) processes to enhance CH4 productivity and selectivity has garnered significant attention. Herein, a single‐atom Pt‐anchored H3PMo12O40 (Pt1‐PMo12) is applied as an efficient proton–electron shuttle to facilitate the photocatalytic performance of NiCo layered double hydroxide (NiCo‐LDH). The resultant Pt1‐PMo12@NiCo‐LDH exhibited superior CH4 productivity (723 µmol g−1 h−1) with CH4 selectivity of 82.3%, showcasing a 24.9 times productivity enhancement over NiCo‐LDH (29 µmol g−1 h−1). Systematic investigations revealed that abundant H* is generated by the dissociation of H2O on Pt1 sites and stored within Pt1‐PMo12. Subsequently, the multiple H* rapidly migrated from Pt1‐PMo12 to the catalytic sites on NiCo‐LDH by the engineered strong Mo─O─Ni/Co bonds, thereby significantly expediting the PCET process. The in situ DRIFTS and theoretical calculations elucidated that the Pt1‐PMo12 decreased the energy barrier for *CO protonation to *CHO (0.38–0.18 eV) and optimized the rate‐determining step of *CH3 to *CH4 (0.64 eV), thus promoting highly active and selective CH4 generation. This work provided novel insights into achieving efficient photocatalytic CO2 methanation by modulating the fast generation and transport of active H*.

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Two-dimensional QDs-Co-CuS1-x/Ti3C2/TiO2 heterojunction with synergistic unsaturated bimetal sites and sulfur vacancies for highly selective photocatalytic CO2 reduction

Shao,

Yang,

Kan

et al. 2025

Journal of Colloid and Interface Science

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Defect-Mediated Cu–S Pair Active Sites Modulating Proton Supply to Facilitate Overall CO₂ Photoreduction with H₂O

Cited by 5 publications

References 31 publications

Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO₂ Reduction to Propylene Under Visible Light Illumination

Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO₂ Reduction to Propylene Under Visible Light Illumination

Single‐Atom Pt Anchored Polyoxometalate as Electron‐Proton Shuttle for Efficient Photoreduction of CO₂ to CH₄ Catalyzed by NiCo Layered Doubled Hydroxide

Two-dimensional QDs-Co-CuS1-x/Ti3C2/TiO2 heterojunction with synergistic unsaturated bimetal sites and sulfur vacancies for highly selective photocatalytic CO2 reduction

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Defect-Mediated Cu–S Pair Active Sites Modulating Proton Supply to Facilitate Overall CO2 Photoreduction with H2O

Cited by 5 publications

References 31 publications

Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO2 Reduction to Propylene Under Visible Light Illumination

Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO2 Reduction to Propylene Under Visible Light Illumination

Single‐Atom Pt Anchored Polyoxometalate as Electron‐Proton Shuttle for Efficient Photoreduction of CO2 to CH4 Catalyzed by NiCo Layered Doubled Hydroxide

Two-dimensional QDs-Co-CuS1-x/Ti3C2/TiO2 heterojunction with synergistic unsaturated bimetal sites and sulfur vacancies for highly selective photocatalytic CO2 reduction

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Defect-Mediated Cu–S Pair Active Sites Modulating Proton Supply to Facilitate Overall CO₂ Photoreduction with H₂O

Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO₂ Reduction to Propylene Under Visible Light Illumination

Covalent Organic Frameworks with Tunable Bridge Positions for Photocatalytic CO₂ Reduction to Propylene Under Visible Light Illumination

Single‐Atom Pt Anchored Polyoxometalate as Electron‐Proton Shuttle for Efficient Photoreduction of CO₂ to CH₄ Catalyzed by NiCo Layered Doubled Hydroxide