2D MOFs and their derivatives for electrocatalytic applications: Recent advances and new challenges

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 472, P. 214777 - 214777

Published: Aug. 19, 2022

Language: Английский

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Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(11), P. 4714 - 4758

Published: Jan. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Language: Английский

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p–d Orbital Hybridization Induced by p-Block Metal-Doped Cu Promotes the Formation of C₂₊ Products in Ampere-Level CO₂ Electroreduction

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(8), P. 4675 - 4682

Published: Feb. 17, 2023

Large-current electrolysis of CO2 to multi-carbon (C2+) products is critical realize the industrial application conversion. However, poor binding strength *CO intermediates on catalyst surface induces multiple competing pathways, which hinder C2+ production. Herein, we report that p-d orbital hybridization induced by Ga-doped Cu (CuGa) could promote efficient electrocatalysis at ampere-level current density. It was found CuGa exhibited highest productivity with a remarkable Faradaic efficiency (FE) 81.5% density 0.9 A/cm2, and potential such high -1.07 V versus reversible hydrogen electrode. At 1.1 still maintained an FE 76.9%. Experimental theoretical studies indicated excellent performance results from Ga, not only enriches reactive sites but also enhances intermediate facilitates C-C coupling. The strategy can be extended other p-block metal-doped catalysts, as CuAl CuGe, boost electroreduction for As far know, this first work electrochemical reduction reaction generate product interaction using catalyst.

Language: Английский

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Metal–organic frameworks and derived materials as photocatalysts for water splitting and carbon dioxide reduction

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 469, P. 214664 - 214664

Published: June 24, 2022

Language: Английский

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Recent progress in electrocatalytic nitrogen reduction to ammonia (NRR)

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 478, P. 214981 - 214981

Published: Dec. 25, 2022

Language: Английский

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Operando Spectroscopic Analysis of Axial Oxygen-Coordinated Single-Sn-Atom Sites for Electrochemical CO₂ Reduction

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(13), P. 7242 - 7251

Published: March 6, 2023

Sn-based materials have been demonstrated as promising catalysts for the selective electrochemical CO2 reduction reaction (CO2RR). However, detailed structures of catalytic intermediates and key surface species remain to be identified. In this work, a series single-Sn-atom with well-defined is developed model systems explore their reactivity toward CO2RR. The selectivity activity formic acid on Sn-single-atom sites are shown correlated Sn(IV)-N4 moieties axially coordinated oxygen (O-Sn-N4), reaching an optimal HCOOH Faradaic efficiency 89.4% partial current density (jHCOOH) 74.8 mA·cm-2 at -1.0 V vs reversible hydrogen electrode (RHE). Employing combination operando X-ray absorption spectroscopy, attenuated total reflectance surface-enhanced infrared Raman 119Sn Mössbauer surface-bound bidentate tin carbonate captured during Moreover, electronic coordination under conditions determined. Density functional theory (DFT) calculations further support preferred formation Sn-O-CO2 over O-Sn-N4 sites, which effectively modulates adsorption configuration reactive lowers energy barrier hydrogenation *OCHO species, compared *COOH Sn-N4 thereby greatly facilitating CO2-to-HCOOH conversion.

Language: Английский

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Recent progress of metal single-atom catalysts for energy applications

Nano Energy, Journal Year: 2023, Volume and Issue: 111, P. 108404 - 108404

Published: April 5, 2023

Language: Английский

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C₂₊ Selectivity for CO₂ Electroreduction on Oxidized Cu-Based Catalysts

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(26), P. 14335 - 14344

Published: June 21, 2023

Design for highly selective catalysts CO2 electroreduction to multicarbon (C2+) fuels is pressing and important. There is, however, presently a poor understanding of selectivity toward C2+ species. Here we report the first time method judiciously combined quantum chemical computations, artificial-intelligence (AI) clustering, experiment development model relationship between product composition oxidized Cu-based catalysts. We 1) evidence that Cu surface more significantly facilitates C-C coupling, 2) confirm critical potential condition(s) this oxidation state under different metal doping components viaab initio thermodynamics computation, 3) establish an inverted-volcano experimental Faradaic efficiency using multidimensional scaling (MDS) results based on physical properties dopant elements, 4) demonstrate design electrocatalysts selectively generate product(s) through co-doping strategy early late transition metals. conclude combination theoretical AI can be used practically relationships descriptors complex reactions. Findings will benefit researchers in designing conversions products.

Language: Английский

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Ligand-free synthesis of noble metal nanocatalysts for electrocatalysis

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 451, P. 138668 - 138668

Published: Aug. 17, 2022

Language: Английский

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Sub-1 nm Cu₂O Nanosheets for the Electrochemical CO₂ Reduction and Valence State–Activity Relationship

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(48), P. 26133 - 26143

Published: Nov. 17, 2023

The copper-based (Cu-based) electrocatalytic materials effectively carry out the carbon dioxide reduction reaction (CO2RR) toward C2+ products, yet superiority and stability of oxidation state Cu are still worth studying. Herein, we designed prepared three Cu-based electrocatalysts with different states to study valence state-activity relationship. Among these electrocatalysts, Cu2O nanosheets thickness only 0.9 nm show an extremely high Faraday efficiency (FEC2+) ∼81%, FEC2+ has increase 37% compared traditional CuOx phase. ultrathin two-dimensional (2D) nanosheet structure abundant oxygen vacancies can stabilize improve selectivity for products in CO2RR. In situ Raman spectroscopy density functional theory calculations demonstrate that rich Cu+ 2D is most suitable *CO adsorption coverage on catalyst surface, which promotes C-C coupling This work provides excellent CO2RR products.

Language: Английский

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