Integration of ultrafine CuO nanoparticles with two-dimensional MOFs for enhanced electrochemical CO2 reduction to ethylene

Wang, Linlin; Li, Xin; Hao, Leiduan; Hong, Song; Robertson, Alex W.; Sun, Zhenyu

doi:10.1016/s1872-2067(21)63947-5

Cited by 42 publications

(35 citation statements)

References 35 publications

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“…To evaluate the intrinsic catalytic properties of the samples, we first conducted the ECR in CO 2 ‐saturated 0.1 mol/L KHCO 3 aqueous electrolyte (pH 6.8) using an H‐cell with continuous CO 2 flow 20 . All potentials mentioned are hereafter with respect to reversible hydrogen electrode.…”

Section: Resultsmentioning

confidence: 99%

“…Strikingly, the incorporation of single Sb atoms on the surface of CuO could effectively hamper hydrogen evolution and greatly facilitate CO 2 reduction (Figure ). The FE and yield rate of each reduction product were determined according to gas chromatography and proton nuclear magnetic resonance measurements 20 . CO, HCOOH, and C 2 H 4 were found to be the major reduction products within the switching voltages from −0.75 to −1.2 V (Figure 4B).…”

Section: Resultsmentioning

confidence: 99%

“…To evaluate the intrinsic catalytic properties of the samples, we first conducted the ECR in CO 2 -saturated 0.1 mol/L KHCO 3 aqueous electrolyte (pH 6.8) using an H-cell with continuous CO 2 flow. 20 All potentials mentioned are hereafter with respect to reversible hydrogen electrode. The potential-dependent geometric current densities of Sb/CuO (V O ) and bare CuO(V O ) were recorded by linear sweep voltammetry (LSV).…”

Section: Electrocatalytic Property For Co 2 Reductionmentioning

confidence: 99%

“…Hence, optimizing the population and binding of the *CO intermediate and concurrently reducing the relative ratio of adsorbed H (to impede the undesired HER) are necessary to accelerate the ECR to C 2 H 4 . To achieve this purpose, previous works have been devoted to the modification of Cu catalysts by heteroatom doping, 13,14 alloying, 15 morphology and facet control, 16,17 mixed oxidation states, 18 and interface engineering 19,20 . However, the C 2 H 4 production efficiency remains insufficient, mostly due to the large C–C coupling barriers.…”

Section: Introductionmentioning

confidence: 99%

“…To achieve this purpose, previous works have been devoted to the modification of Cu catalysts by heteroatom doping, 13,14 alloying, 15 morphology and facet control, 16,17 mixed oxidation states, 18 and interface engineering. 19,20 However, the C 2 H 4 production efficiency remains insufficient, mostly due to the large C-C coupling barriers. To overcome this issue, the design and development of a synergistic catalytic system that enables enhancement of both CO 2 activation and C-C coupling offer a promising avenue.…”

Section: Introductionmentioning

confidence: 99%

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Single atom and defect engineering of CuO for efficient electrochemical reduction of CO₂ to C₂H₄

et al. 2022

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Electrochemical CO2 transformation to high‐value ethylene (C2H4) at high currents and efficiencies is desired and yet remains a grand challenge. We show for the first time that coupling single Sb atoms and oxygen vacancies of CuO enable synergistic electrocatalytic reduction of CO2 to C2H4 at low overpotentials. Highly dispersed Sb atoms occupying metal substitutional sites of CuO are synthesized under mild conditions. The overall CO2 reduction faradaic efficiency (FE) reaches 89.3 ± 1.1% with an FE toward C2H4 exceeding 58.4% at a high‐current density of 500 mA/cm2. Addition of the p‐block metal is found to induce transformation of CuO from flakes to nanoribbons rich in nanoholes and oxygen vacancies, greatly enhancing CO2 adsorption and activation while suppressing hydrogen evolution. Further density functional theory calculations with in situ X‐ray diffraction reveal that combining Sb sites and oxygen vacancies prominently lessen the dimerization energy of adsorbed CO intermediate, thus boosting the conversion of CO2 to produce C2H4. This study provides a new perspective for promoting selective C–C coupling for electrochemical CO2 reduction.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Electrocatalytic Property For Co 2 Reductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Single atom and defect engineering of CuO for efficient electrochemical reduction of CO₂ to C₂H₄

et al. 2022

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Heterogeneous Nanosized Metal (Metallic Compound)@Metal‐Organic Framework Composites: Recent Advances in the Preparation and Applications

Cui

Zhao

Wang

et al. 2023

Adv Funct Materials

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Metal‐organic framework (MOF) composites based on MOFs‐wrapped metals or metallic compounds (denoted as M/MC@MOFs) are an important class of materials that integrate M/MCs and MOFs. MOFs can fix and confine M/MCs to regulate their size, prevent uncontrollable aggregation, and enhance the exposure and ordered arrangement of active sites. In turn, M/MCs support the MOFs to enhance their stability and realize more targeted properties. In this review, the features and application scope of different M/MC@MOF synthesis methods are explored, considering the influential factors and regulation modes of the M/MC–MOFs integration. Additionally, the performances of the M/MC@MOF composites are comprehensively discussed, and the underlying mechanisms are clarified. The performance of M/MC@MOFs is dependent on the orderly synergy between the MOFs and M/MCs. MOFs can sieve and transfer specific molecules to the M/MC surface, whereas the robust interface provides new charge/energy‐transfer pathways, which enhance the activity and selectivity of the composites for diverse molecules. Furthermore, the challenges facing this field are analyzed, and the recommendations for advancing the development of M/MC@MOF composites are presented.

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Self‐Polarization Triggered Multiple Polar Units Toward Electrochemical Reduction of CO₂ to Ethanol with High Selectivity

et al. 2023

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Electrochemical conversion of CO2 to highly valuable ethanol has been considered a intriguring strategy for carbon neutruality. However, the slow kinetics of coupling carbon‐carbon (C−C) bonds, especially the low selectivity ethanol than ethylene in neutral conditions, is a significant challenge. Herein, the asymmetrical refinement structure with enhanced charge polarization is built in the vertically oriented bimetallic organic frameworks (NiCu‐MOF) nanorod array with encapsulated Cu2O (Cu2O@MOF/CF), which can induce an intensive internal electric field to increase the C−C coupling for producing ethanol in neutral electrolyte. Particularly, when directly employed Cu2O@MOF/CF as the self‐supporting electrode, the ethanol faradaic efficiency (FEethanol) could reach maximum 44.3 % with an energy efficiency of 27 % at a low working‐potential of −0.615 V versus the reversible hydrogen electrode (vs. RHE) using CO2‐saturated 0.5 M KHCO3 as the electrolyte. Experimental and theoretical studies suggest that the polarization of atomically localized electric fields derived from the asymmetric electron distribution can tune the moderate adsorption of *CO to assist the C−C coupling and reduce the formation energy of H2CCHO*‐to‐*OCHCH3 for the generation of ethanol. Our research offers a reference for the design of highly active and selective electrocatalysts for reducing CO2 to multicarbon chemicals.

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Integration of ultrafine CuO nanoparticles with two-dimensional MOFs for enhanced electrochemical CO2 reduction to ethylene

Cited by 42 publications

References 35 publications

Single atom and defect engineering of CuO for efficient electrochemical reduction of CO₂ to C₂H₄

Single atom and defect engineering of CuO for efficient electrochemical reduction of CO₂ to C₂H₄

Heterogeneous Nanosized Metal (Metallic Compound)@Metal‐Organic Framework Composites: Recent Advances in the Preparation and Applications

Self‐Polarization Triggered Multiple Polar Units Toward Electrochemical Reduction of CO₂ to Ethanol with High Selectivity

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Integration of ultrafine CuO nanoparticles with two-dimensional MOFs for enhanced electrochemical CO2 reduction to ethylene

Cited by 42 publications

References 35 publications

Single atom and defect engineering of CuO for efficient electrochemical reduction of CO2 to C2H4

Single atom and defect engineering of CuO for efficient electrochemical reduction of CO2 to C2H4

Heterogeneous Nanosized Metal (Metallic Compound)@Metal‐Organic Framework Composites: Recent Advances in the Preparation and Applications

Self‐Polarization Triggered Multiple Polar Units Toward Electrochemical Reduction of CO2 to Ethanol with High Selectivity

Contact Info

Product

Resources

About

Single atom and defect engineering of CuO for efficient electrochemical reduction of CO₂ to C₂H₄

Single atom and defect engineering of CuO for efficient electrochemical reduction of CO₂ to C₂H₄

Self‐Polarization Triggered Multiple Polar Units Toward Electrochemical Reduction of CO₂ to Ethanol with High Selectivity