Atomically Dispersed Cu Active Centers: Local Structure and Mechanism Modulation for Carbon Dioxide Reduction

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 10, 2025

Abstract Reducing carbon dioxide （CO 2 ）to high‐value products using green renewable energy is a promising approach for addressing and greenhouse effect issues. Consequently, electrocatalytic CO reduction reaction (CO RR) technology has become current research hotspot. Since the discovery of high activity selectivity copper in RR, atomically dispersed Cu catalysts have garnered widespread attention due to their efficient atom utilization, unique electronic structure, outstanding catalytic performance. However, great challenge remains providing rational catalyst design principles achieve regulation product distribution. A clear understanding materials an in‐depth interpretation mechanism as well elucidation strategy progress toward different are keys building solving above problem. Therefore, this review starts with introduction advanced characterization techniques reveal structure mechanisms. Then, various optimization strategies applications producing targeted summarized discussed. Finally, perspectives on RR field future development offered.

Language: Английский

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A Perspective on the Reaction Mechanisms of CO₂ Electrolysis

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 2212 - 2227

Published: April 18, 2025

Language: Английский

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Cation Effects on the Adsorbed Intermediates of CO₂ Electroreduction Are Systematic and Predictable

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8814 - 8822

Published: May 23, 2024

The electrode–electrolyte interface, and in particular the nature of cation, has considerable effects on activity product selectivity electrochemical reduction CO2. Therefore, to improve electrocatalysis this challenging reaction, it is paramount ascertain whether cation adsorbed intermediates are systematic. Here, DFT calculations used show that K+, Na+, Mg2+, single carbon CO2 can either be stabilizing or destabilizing depending metal adsorbate. Because systematic trends observed, accurately predicted simple terms for a wide variety metals, cations species. These results then applied CO four different catalytic surfaces (Au, Ag, Cu, Pd) activation weak-binding metals consistently observed by virtue stabilization key intermediate *COOH.

Language: Английский

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Electrocatalytic reduction of carbon dioxide to C4+ products

Current Opinion in Electrochemistry, Journal Year: 2024, Volume and Issue: 46, P. 101534 - 101534

Published: May 10, 2024

Language: Английский

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Nanostructured DyFeO₃ photocatalyst: an authentic and effective approach for remediation of industrial and pharmaceutical wastewater

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(37), P. 25475 - 25490

Published: Jan. 1, 2024

Illustration of the photocatalytic degradation mechanism pollutants by DyFeO 3 under solar irradiation, emphasizing enhanced apparent quantum yield and reduction in activation energy facilitated .

Language: Английский

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Electrochemical Nitrogen Reduction: The Energetic Distance to Lithium

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(10), P. 4947 - 4952

Published: Sept. 19, 2024

Energy-efficient electrochemical reduction of nitrogen to ammonia could help in mitigating climate change. Today, only Li- and recently Ca-mediated systems can perform the reaction. These materials have a large intrinsic energy loss due need electroplate metal. In this work, we present series calculated energetics, formation energies, binding energies as fundamental features calculate energetic distance between Li Ca potential new systems. The featured increases with standard potential. However, dimensionality using principal component analysis provides an encouraging picture; are not exceptional feature space, other should be able carry out it becomes more challenging positive plating is.

Language: Английский

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Benchmarking ionomers for CO2 electroreduction to multicarbon products in zero-gap electrolyzers

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(32), P. 20990 - 20998

Published: Jan. 1, 2024

This work benchmarks ionomers for CO 2 electroreduction to multicarbon products. Ionomers with stronger hydrophobicity or having bulkier and less hydrated ionised side chains were found favour *CO adsorption product formation.

Language: Английский

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Refining Free-Energy Calculations for Electrochemical Reactions: Unveiling Corrections beyond Gas-Phase Errors for Solvated Species and Ions

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(33), P. 13732 - 13742

Published: Aug. 9, 2024

As much of the theory related to computational electrocatalysis has been adapted from thermodynamics gas-phase reactions, it demands careful treatment and implementation proper corrections when investigating electrochemical systems. In this article, we present a comprehensive thermodynamic framework that incorporates all potential phases (gaseous or aqueous) different forms (molecular ionic) reactants products under ambient conditions. This elucidates systematic relationships governing Gibbs free energy across diverse chemical species, employing Henry's volatility constant (KHor H), acid dissociation (Ka), pH. We introduce method for calculating both KH Ka, detailing associated challenges. Our study demonstrates calculation energies is influenced by Ka pH, primarily due occurrence unbalanced numbers electrons protons transfers during adsorption desorption ions. findings also highlight inclusion aqueous products, whether in molecular ionic form, significantly modifies free-energy landscapes. turn, reported solvation ion are imperative obtain correct activity predictions descriptors such as overpotential span model Gmax(η), deviations more than 0.3 eV observed if these contributions ignored.

Language: Английский

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Anionic Surfactant-Tuned Interfacial Water Reactivity Promoting Electrocatalytic CO₂ Reduction

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 18156 - 18166

Published: Nov. 23, 2024

The effects of the electrical double layer (EDL), which pertain to compositions and interactions among electrolyte species, significantly impact catalytic process. There is a pressing need investigate role components deepen our understanding EDL effects. In this study, we tune water activity within range anionic surfactants featuring different functional groups adjust H2 evolution CO2 reduction selectivity. We demonstrate that these are active in local reaction environment under cathodic potential. enhanced selectivity CO can be attributed robust interfacial hydrogen-bonding network reformed by surfactants. This diminishes dissociation promotes hydrogenation step reduction. Notably, incorporating improves performance, registering Faradaic efficiencies 89.7% (RSO3–, SDS), 97.5% (RSO4–, SLS), 98.4% (RPO42–, SMP), 98.9% (RCOO–, SL) at −1.2 V versus RHE, thereby outperforming blank KHCO3 (53.1%). research underscores crucial influence additives CO2RR.

Language: Английский

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Mechanistic insights into the enhanced photocatalytic efficiency of MoS₂-tuned DyFeO₃ heterojunction for pollutants degradation

Nanoscale, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

In this study, DyFeO3-MoS2 heterojunction nanocomposites were synthesized by integrating porous DyFeO3 nanoparticles (an n-type semiconductor) with MoS2 nanosheets (a p-type semiconductor). The resulting p-n substantially improved the photocatalytic efficiency for degrading methylene blue (MB) and levofloxacin (LFX). This design introduces a built-in electric field at interface, promoting efficient charge separation suppressing electron-hole recombination, thereby significantly enhancing performance under solar irradiation compared to alone. Characterization studies, including XRD, FESEM, TEM, XPS, UV-visible absorbance, photoluminescence, Mott-Schottky analysis, confirmed nanocomposites' crystalline structure, well-dispersed nanosheets, oxygen vacancies, enhanced visible light absorption, favorable band positions. incorporation of increased separation, surface area mitigating aggregation, leading higher degradation rates. Among tested compositions, (80 : 20) nanocomposite, containing 20 wt% MoS2, exhibited highest efficiencies, 96.5% MB 88.7% LFX. Further analyses, activation energy determination, quantum yield measurement, scavenger tests, reusability assessments, optimized nanocomposite's durability. reduced energies high yields (35.5% MB, 25.8% LFX) indicate photon conversion radical generation, superoxide radicals (˙O2-) identified as primary reactive species. Stability tests revealed over 85% retention activity after four cycles, underscoring composite's robustness. Moreover, mechanism key insights into pathways pollutants. investigation demonstrates viable solar-driven solution pollutant in wastewater treatment incorporating nanostructures.

Language: Английский

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