Predesign of Catalytically Active Sites via Stable Coordination Cluster Model System for Electroreduction of CO<sub>2</sub> to Ethylene

Lan, Ya‐Qian; Lu, Yunfeng; Dong, Long‐Zhang; Liu, Jiang; Yang, Ruiyue; Liu, Jingjing; Zhang, Lei; Wang, Yirong; Li, Shun-Li

doi:10.1002/ange.202111265

Cited by 9 publications

(2 citation statements)

References 52 publications

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“…Very recently, Lan and coworkers demonstrated that pyrazolate-bridged dicopper compounds (Scheme 1a) have ECR performances for yielding C 2+ products and show a Faradaic efficiency (FE) of ca. 60% under strong alkaline conditions, 20,31 though lower than those of the best Cu-based nanomaterials/nanocomposites (FE > 70%). 32,33 This might be ascribed to the higher Gibbs freeenergy barriers of hydrogenation of intermediates in ECR.…”

Section: ■ Introductionmentioning

confidence: 83%

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO₂ to C₂₊ Products

et al. 2022

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Crystalline porous materials sustained by supramolecular interactions (e.g., π−π stacking interactions) are a type of molecular crystals showing considerable stability, but their applications are rarely reported due to the high difficulty of their construction. Herein, a stable π−π stacking framework formed by a trinuclear copper(I) compound [Cu 3 (HBtz) 3 (Btz)Cl 2 ] (CuBtz, HBtz = benzotriazole) with pyrazolate-bridged dicopper(I) sites is reported and employed for electrochemical CO 2 reduction, showing an impressive performance of 73.7 ± 2.8% Faradaic efficiency for C 2+ products [i.e., ethylene (44%), ethanol (21%), acetate (4.7%), and propanol (4%)] with a current density of 7.9 mA cm −2 at the potential of −1.3 V versus RHE in an H-type cell and a Faradic efficiency (61.6%) of C 2+ products with a current density of ≈1 A cm −2 and a reaction rate of 5639 μmol m −2 s −1 at the potential of −1.6 V versus RHE in a flow cell device, representing an impressive performance reported to date. In-situ infrared spectroscopy, density functional theory calculations, and control experiments revealed that the uncoordinated nitrogen atoms of benzotriazolates in the immediate vicinity can act as proton relays and cooperate with the dicopper(I) site to promote the hydrogenation process of the *CO intermediate and the C−C coupling, resulting in the highly selective electroreduction of CO 2 to C 2+ products.

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Section: ■ Introductionmentioning

confidence: 83%

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO₂ to C₂₊ Products

et al. 2022

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“…Chemistry research has sought ‘green’ options that do not generate CO 2 , for both ammonia and hydrogen production [29–31], as well as methods by which CO 2 generated can be captured, either for long-term lock-in (e.g. as stable carbonates) or for use in other chemical and physical applications [32,33].…”

Section: How Does/can Chemistry Contribute To Resilience?mentioning

confidence: 99%

A shared future: chemistry's engagement is essential for resilience of people and planet

et al. 2022

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Strengthening resilience—elasticity or adaptive capacity—is essential in responding to the wide range of natural hazards and anthropogenic changes humanity faces. Chemistry's roles in resilience are explored for the first time, with its technical capacities set in the wider contexts of cross-disciplinary working and the intersecting worlds of science, society and policy. The roles are framed by chemistry's contributions to the sustainability of people and planet, examined via the human security framework's four material aspects of food, health, economic and environmental security. As the science of transformation of matter, chemistry is deeply involved in these material aspects and in their interfacing with human security's three societal and governance aspects of personal, community and political security. Ultimately, strengthening resilience requires making choices about the present use of resources as a hedge against future hazards and adverse events, with these choices being co-determined by technical capacities and social and political will. It is argued that, to intensify its contributions to resilience, chemistry needs to take action along at least three major lines: (i) taking an integrative approach to the field of ‘chemistry and resilience’; (ii) rethinking how the chemical industry operates; and (iii) engaging more with society and policy-makers.

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Experimental and Theoretical Insights into Single Atoms, Dual Atoms, and Sub‐Nanocluster Catalysts for Electrochemical CO₂ Reduction (CO₂RR) to High‐Value Products

Woldu,

Yohannes,

Huang

et al. 2024

Advanced Materials

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Electrocatalytic carbon dioxide (CO2) conversion into valuable chemicals paves the way for the realization of carbon recycling. Downsizing catalysts to single‐atom catalysts (SACs), dual‐atom catalysts (DACs), and sub‐nanocluster catalysts (SNCCs) has generated highly active and selective CO2 transformation into highly reduced products. This is due to the introduction of numerous active sites, highly unsaturated coordination environments, efficient atom utilization, and confinement effect compared to their nanoparticle counterparts. Herein, recent Cu‐based SACs are first reviewed and the newly emerged DACs and SNCCs expanding the catalysis of SACs to electrocatalytic CO2 reduction (CO2RR) to high‐value products are discussed. Tandem Cu‐based SAC–nanocatalysts (NCs) (SAC–NCs) are also discussed for the CO2RR to high‐value products. Then, the non‐Cu‐based SACs, DACs, SAC–NCs, and SNCCs and theoretical calculations of various transition‐metal catalysts for CO2RR to high‐value products are summarized. Compared to previous achievements of less‐reduced products, this review focuses on the double objective of achieving full CO2 reduction and increasing the selectivity and formation rate toward C–C coupled products with additional emphasis on the stability of the catalysts. Finally, through combined theoretical and experimental research, future outlooks are offered to further develop the CO2RR into high‐value products over isolated atoms and sub‐nanometal clusters.

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Predesign of Catalytically Active Sites via Stable Coordination Cluster Model System for Electroreduction of CO₂ to Ethylene

Cited by 9 publications

References 52 publications

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO₂ to C₂₊ Products

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO₂ to C₂₊ Products

A shared future: chemistry's engagement is essential for resilience of people and planet

Experimental and Theoretical Insights into Single Atoms, Dual Atoms, and Sub‐Nanocluster Catalysts for Electrochemical CO₂ Reduction (CO₂RR) to High‐Value Products

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Predesign of Catalytically Active Sites via Stable Coordination Cluster Model System for Electroreduction of CO2 to Ethylene

Cited by 9 publications

References 52 publications

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO2 to C2+ Products

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO2 to C2+ Products

A shared future: chemistry's engagement is essential for resilience of people and planet

Experimental and Theoretical Insights into Single Atoms, Dual Atoms, and Sub‐Nanocluster Catalysts for Electrochemical CO2 Reduction (CO2RR) to High‐Value Products

Contact Info

Product

Resources

About

Predesign of Catalytically Active Sites via Stable Coordination Cluster Model System for Electroreduction of CO₂ to Ethylene

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO₂ to C₂₊ Products

A Porous π–π Stacking Framework with Dicopper(I) Sites and Adjacent Proton Relays for Electroreduction of CO₂ to C₂₊ Products

Experimental and Theoretical Insights into Single Atoms, Dual Atoms, and Sub‐Nanocluster Catalysts for Electrochemical CO₂ Reduction (CO₂RR) to High‐Value Products