In-situ N-defect and single-metal atom synergetic engineering of high-efficiency Ag–N–C electrocatalysts for CO2 reduction

Liao, Luliang; Xia, Guomin; Wang, Yigang; Ye, Guigui; Wang, Hongming

doi:10.1016/j.apcatb.2022.121826

Cited by 24 publications

(12 citation statements)

References 42 publications

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“…Single-atom catalysts (SACs), which have uniform active sites and geometric structure as well as close to 100% of metal utilization efficiency, have been regarded as the ideal metal catalysts and showed great potential for high efficiency and selectivity in the CO 2 RR. − However, only a few literature studies of Ag SACs have been reported up to now, − which are much less related to the electrocatalytic CO 2 RR. − The CO faradaic efficiency (FE CO ) is >95%, while the best CO partial current density ( j CO ) is lower than 15 mA cm –2 catalyzed by Ag-based SACs. Although atom efficiency is greatly improved compared with Ag nanocatalysts, Ag SACs with large current density at high faradaic efficiency are rarely reported.…”

Section: Introductionmentioning

confidence: 99%

Ag Single Atoms Anchored on CeO₂ with Interfacial Oxygen Vacancies for Efficient CO₂ Electroreduction

Liang

Meng

et al. 2023

ACS Appl. Mater. Interfaces

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Ag single-atom catalysts (SACs) have great potential in selective electrocatalysis of the CO2 reduction reaction (CO2RR) to CO, while it is still a challenge to achieve high current density and high atom efficiency simultaneously. Here, we present a new and simple in situ adsorption–reduction method to prepare Ag SACs supported on CeO2 (Ag1/CeO2). It is found that Ag single atoms are anchored on CeO2 through strong metal–support interaction (SMSI), and each Ag atom is accompanied with three interfacial oxygen vacancies. This Ag1/CeO2 exhibits high performance in the electrocatalytic CO2RR with a high CO faradaic efficiency (FE) of >95% under a wide potential range. The turnover frequency (TOF) value can reach 50,310 h–1 at FECO = 99.5% in H-cells. Notably, Ag1/CeO2 achieves an industrial-grade current density of 403 mA cm–2 with a high FECO of 97.2% in flow cells. Experimental results combined with density functional theory calculation revealed that this superior performance was mainly ascribed to the existence of interfacial oxygen vacancies, which lead to the formation of Ag–O–Ce3+ atomic interfaces, and activates the Ce3+–O structures as the synergistic active center of Ag, thus promoting CO2 adsorption and activation and reducing the reaction potential barrier of *COOH-to-*CO.

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Section: Introductionmentioning

confidence: 99%

Ag Single Atoms Anchored on CeO₂ with Interfacial Oxygen Vacancies for Efficient CO₂ Electroreduction

Liang

Meng

et al. 2023

ACS Appl. Mater. Interfaces

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“…[10][11] Second, the metal atom active centers can generate unique coordination structures with other non-metal atoms. [12][13] In particular, the low coordination structure can effectively modulate the electronic structure of the metal atom center, thus enhancing the catalytic activity and achieving satisfactory catalytic effects. [14][15] Third, similar to homogeneous catalysts, single-atom catalysts have highly homogeneous active sites and geometric configurations, which enable them to have similar electronic structures and spatial interactions with substrate molecules, thus improving catalytic selectivity.…”

Section: Introductionmentioning

confidence: 99%

Customization from Single to Dual Atomic Sites for Efficient Electrocatalytic CO₂ Reduction to Value‐added Chemicals

Wei

Pan

et al. 2023

Chemistry An Asian Journal

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In recent years, single‐atom catalysts (SACs) have received increasing attention in the field of electrochemical CO2RR with their efficient atom utilization efficiency and excellent catalytic performance. However, their low metal loading and the presence of linear relationships for single active sites with simple structures possibly restrict their activity and practical applications. Active site tailoring at the atomic level is a visionary approach to break the existing limitations of SACs. This paper first briefly introduces the synthesis strategies of SACs and DACs. Then, combining previous experimental and theoretical studies, this paper introduces four optimization strategies, namely spin‐state tuning engineering, axial functionalization engineering, ligand engineering, and substrate tuning engineering, for improving the catalytic performance of SACs in the electrochemical CO2RR process by combining previous experimental and theoretical studies. Then it is introduced that DACs exhibit significant advantages over SACs in increasing metal atom loading, promoting the adsorption and activation of CO2 molecules, modulating intermediate adsorption, and promoting C−C coupling. At the end of this paper, we briefly and succinctly summarize the main challenges and application prospects of SACs and DACs in the field of electrochemical CO2RR at present.

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“…3,4 Up to now, massive endeavors have been devoted to designing high-performance catalysts with Au, 5,6 Ag, 7,8 and Pd 9,10 as active sites for CO 2 -to-CO transformation. Further studies have demonstrated that the adjustment of the coordination number of the active sites and the local electronic structure through crystal facets, 11 grain boundaries, 12,13 and defects 14,15 at the nanoscale and the regulation of mass transfer of substrates and electrochemically active surface area through the particle size, 16,17 morphology, 7,18 and porosity 19,20 at the mesoscale greatly influence the catalytic activity and selectivity.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Electrochemical reduction reaction of CO 2 (CO 2 RR) is an ideal solution to alleviate the greenhouse effect among different CO 2 fixation methods for its high environmental compatibility. , Among various CO 2 RR pathways, electrochemical CO 2 reduction to CO is considered one of the most promising approaches due to its considerable technical and economic feasibility. , Up to now, massive endeavors have been devoted to designing high-performance catalysts with Au, , Ag, , and Pd , as active sites for CO 2 -to-CO transformation. Further studies have demonstrated that the adjustment of the coordination number of the active sites and the local electronic structure through crystal facets, grain boundaries, , and defects , at the nanoscale and the regulation of mass transfer of substrates and electrochemically active surface area through the particle size, , morphology, , and porosity , at the mesoscale greatly influence the catalytic activity and selectivity.…”

Section: Introductionmentioning

confidence: 99%

Covalent Organic Frameworks Boost the Silver-Electrocatalyzed Reduction of CO₂: The Electronic and Confinement Effect

Yang

et al. 2023

ACS Appl. Mater. Interfaces

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The electrocatalytic reduction of CO2 to CO with high efficiency is one of the most promising approaches for CO2 conversion due to its considerable economic feasibility and broad application prospects. In this study, three Ag@COF-R (R = −H, −OCH3, −OH) hybrids were facilely fabricated by impregnating silver acetate (AgOAc) into respective covalent organic frameworks (COFs) prepared in advance. They differ significantly in the crystallinity, porosity, distribution, size, and electronic configuration of AgOAc species, which thereby influences both the activity and the selectivity of electrolytic CO2-to-CO transformation. Impressively, Ag@COF-OCH3 provided a high FECO of 93.0% with a high j CO of 213.9 mA cm–2 at −0.87 V (vs reversible hydrogen electrode, RHE) in 1 M KOH using a flow cell. In addition, it exhibited long-term durability at 100 mA cm–2 for 30 h.

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In-situ N-defect and single-metal atom synergetic engineering of high-efficiency Ag–N–C electrocatalysts for CO2 reduction

Cited by 24 publications

References 42 publications

Ag Single Atoms Anchored on CeO₂ with Interfacial Oxygen Vacancies for Efficient CO₂ Electroreduction

Ag Single Atoms Anchored on CeO₂ with Interfacial Oxygen Vacancies for Efficient CO₂ Electroreduction

Customization from Single to Dual Atomic Sites for Efficient Electrocatalytic CO₂ Reduction to Value‐added Chemicals

Covalent Organic Frameworks Boost the Silver-Electrocatalyzed Reduction of CO₂: The Electronic and Confinement Effect

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In-situ N-defect and single-metal atom synergetic engineering of high-efficiency Ag–N–C electrocatalysts for CO2 reduction

Cited by 24 publications

References 42 publications

Ag Single Atoms Anchored on CeO2 with Interfacial Oxygen Vacancies for Efficient CO2 Electroreduction

Ag Single Atoms Anchored on CeO2 with Interfacial Oxygen Vacancies for Efficient CO2 Electroreduction

Customization from Single to Dual Atomic Sites for Efficient Electrocatalytic CO2 Reduction to Value‐added Chemicals

Covalent Organic Frameworks Boost the Silver-Electrocatalyzed Reduction of CO2: The Electronic and Confinement Effect

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Product

Resources

About

Ag Single Atoms Anchored on CeO₂ with Interfacial Oxygen Vacancies for Efficient CO₂ Electroreduction

Ag Single Atoms Anchored on CeO₂ with Interfacial Oxygen Vacancies for Efficient CO₂ Electroreduction

Customization from Single to Dual Atomic Sites for Efficient Electrocatalytic CO₂ Reduction to Value‐added Chemicals

Covalent Organic Frameworks Boost the Silver-Electrocatalyzed Reduction of CO₂: The Electronic and Confinement Effect