Preventing Salt Formation in Zero-Gap CO₂ Electrolyzers by Quantifying Cation Accumulation

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 807 - 814

Published: Jan. 14, 2025

Language: Английский

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Modulating the Electronic Properties of Single Ni Atom Catalyst via First‐Shell Coordination Engineering to Boost Electrocatalytic Flue Gas CO₂ Reduction

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

Published: Jan. 10, 2025

Abstract Electrochemical converting CO 2 to via single atom catalyst is an effective strategy for reducing concentration in the atmosphere and achieving a carbon‐neutral cycle. However, relatively low industrial processes large energy barriers activating severely obstruct actual application. Reasonably modulating coordination shell of active center enhance activity catalysts. Herein, well‐designed single‐atom electrocatalyst Ni‐N 3 S 1 developed large‐scale synthesis strategy. The constructed S‐C exhibits superior catalytic than 4 ‐C conversion H‐type cells, industrial‐level current density with excellent durability at wide pH range can be achieved gas‐diffusion flow cells. Experimental results functional theory (DFT) calculation demonstrate that introducing electronegative significantly regulate electronic structure site, promoting adsorption capacity decreasing barrier *COOH formation, thus larger size flexibility sulfur mitigate nickel agglomeration stability catalyst. This work provides designing highly catalysts electrocatalysis reactive sites.

Language: Английский

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Reversible Angle Distortion-Dependent Electrochemical CO₂ Reduction on Cobalt Phthalocyanine

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 7, 2025

Deducing the local electronic and atomic structural changes in active sites during electrochemical carbon dioxide reduction is essential for elucidating intrinsic mechanisms developing highly catalysts that are stable a long duration. Herein, utilizing operando valence-to-core X-ray emission spectroscopy high energy-resolution fluorescence detected absorption near-edge structure, combined with spectroscopic calculations, structure evolutions of model cobalt phthalocyanine (CoPc) were quantitatively elucidated. Under real reaction conditions, CoPc undergoes reversible angle distortion while maintaining constant metal-ligand bond length, causing energy levels split d orbitals electron density molecular orbitals. The further influences interactions among ligands, intermediates, metal centers. change CO Faraday efficiency was also determined, demonstrating robustness. demonstrated findings serve as an important contribution to determine structure-performance relationship which enlightens rational design atomically dispersed site activity emphasize capabilities resolution toward analyzing metal-implanted N-doped catalysts.

Language: Английский

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Unraveling Dynamic Structural Evolution of Single Atom Catalyst via In Situ Surface-Enhanced Infrared Absorption Spectroscopy

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 7, 2025

Metal–nitrogen-carbon (M–N-C) single-atom catalysts (SACs) have been widely applied in catalyzing electrochemical redox reactions. However, their long-term catalytic stabilities greatly limit practical applications. This work investigates the dynamic evolution of two model Cu–N–C SACs with different Cu–N coordinations, namely Cu1/Npyri-C and Cu1/Npyrr-C, CO reduction reaction (CORR), based on a collection situ characterizations including attenuated total reflectance surface-enhanced infrared absorption spectroscopy, X-ray quasi-in electron paramagnetic resonance spectroscopy ultraviolet–visible complemented by theoretical calculations. Our findings reveal that Cu nanoparticle formation rate over Cu1/Npyrr-C is more than 6 times higher during CORR. Quasi-in UV–vis measurements demonstrate hydrogen radicals can be produced CORR, which will attack bonds SACs, causing leaching Cu2+ followed subsequent to form nanoparticles. Kinetic calculations show displays better stability resulting from stronger Cu–Npyri bonds. study deepens understanding deactivation mechanism reactions provides guidance for design next-generation enhanced durability.

Language: Английский

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Comprehensive Insight into External Field‐Driven CO₂ Reduction to CO: Recent Progress and Future Prospects

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

Published: March 19, 2025

Abstract Currently, thermal catalysis is the predominant method for achieving reverse water–gas shift (RWGS) reaction reduction of carbon dioxide (CO 2 ) to monoxide (CO), which a crucial intermediate in synthesis other high value‐added chemicals via Fischer–Tropsch synthesis. To extend applicability CO RR) CO, researchers have explored RR that utilizes external fields addition fields. This review commences by providing an overview research background pertinent and then primary mechanisms potential pathways associated with process are summarized. Furthermore, impact various fields, including traditional light photothermal coupling solar thermochemical laser electric photoelectric electromagnetic plasma on investigated. Finally, summary future perspectives as influenced presented. It anticipated this will provide valuable insights focused preparation high‐value‐added through enhanced

Language: Английский

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Low‐Coordinated Ni Single Atom Catalyst with Carbon Coordination for Efficient CO₂ Electroreduction

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

Published: March 21, 2025

Abstract In essence, electrocatalytic CO 2 reduction reaction (CO RR) process for the ‐to‐CO conversion involves two critical reactive intermediates: *COOH and *CO. The trade‐off between adsorption of desorption *CO is challenging Ni‐based RR catalysts. high‐valence Ni site inadequate in supplying sufficient electrons activation subsequent *COOH; conversely, metallic with abundant electron exhibits excessively strong π‐backbonding *CO, thus hindering its desorption. Here, study reports a low‐coordinated single atom catalyst (SAC) characterized by structure carbon coordination, thereby engineering moderate depletion at sites. This SAC achieves high selectivity production up to 99.1% H‐cell. Additionally, it maintains an ultrahigh near 100% across broad range current densities flow cell, coupled sustained stability large 250 mA cm −2 20 h. Both situ characterization results density functional theory (DFT) calculations confirm dual functionality this structure, as enhances while concurrently facilitating greatly promoting overall process.

Language: Английский

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In(OH)3-modified CuO nanosheets for CO2 electroreduction to promote C2 products and inhibit H2

Applied Surface Science, Journal Year: 2025, Volume and Issue: unknown, P. 163421 - 163421

Published: May 1, 2025

Language: Английский

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Regulating Adsorption of Intermediates via d–p Orbital Electron Coupling for Boosting CO₂RR

ACS Applied Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: May 14, 2025

Language: Английский

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Frontiers in Catalytic Technologies for Carbon Neutrality: Advances and Prospects

Chemical Research in Chinese Universities, Journal Year: 2025, Volume and Issue: unknown

Published: May 16, 2025

Language: Английский

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Porous nitrogen-doped carbon anchored with highly dispersed nickel active sites for efficient carbon dioxide electroreduction

Materials Today Communications, Journal Year: 2025, Volume and Issue: unknown, P. 112197 - 112197

Published: March 1, 2025

Language: Английский

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