Co-catalytic metal–support interactions in single-atom electrocatalysts

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(3), P. 173 - 189

Published: Jan. 10, 2024

Language: Английский

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Highly Efficient Electroreduction of CO₂ to Ethanol via Asymmetric C–C Coupling by a Metal–Organic Framework with Heterodimetal Dual Sites

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(49), P. 26783 - 26790

Published: Nov. 28, 2023

The electroreduction of CO2 into value-added liquid fuels holds great promise for addressing global environmental and energy challenges. However, achieving highly selective yielding multi-carbon oxygenates through the electrochemical reduction reaction (eCO2RR) is a formidable task, primarily due to sluggish asymmetric C-C coupling reaction. In this study, novel metal-organic framework (CuSn-HAB) with unprecedented heterometallic Sn···Cu dual sites (namely, pair SnN2O2 CuN4 bridged by μ-N atoms) was designed overcome limitation. CuSn-HAB demonstrated an impressive Faradic efficiency (FE) 56(2)% eCO2RR alcohols, current density 68 mA cm-2 at low potential -0.57 V (vs RHE). Notably, no significant degradation observed over continuous 35 h operation specified density. Mechanistic investigations revealed that, in comparison copper site, site exhibits higher affinity oxygen atoms. This enhanced plays pivotal role facilitating generation key intermediate *OCH2. Consequently, compared homometallic Cu···Cu (generally ethylene product), were proved be more thermodynamically favorable between *CO *OCH2, leading formation *CO-*OCH2, which ethanol product.

Language: Английский

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A covalent molecular design enabling efficient CO2 reduction in strong acids

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(10), P. 1231 - 1242

Published: June 25, 2024

Language: Английский

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Highly selective and low-overpotential electrocatalytic CO2 reduction to ethanol by Cu-single atoms decorated N-doped carbon dots

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 345, P. 123694 - 123694

Published: Jan. 4, 2024

Language: Английский

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Selective Increase in CO2 Electroreduction to Ethanol Activity at Nanograin‐Boundary‐Rich Mixed Cu(I)/Cu(0) Sites via Enriching Co‐Adsorbed CO and Hydroxyl Species

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: May 31, 2024

Selective producing ethanol from CO

Language: Английский

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Structural Design and Energy and Environmental Applications of Hydrogen‐Bonded Organic Frameworks: A Systematic Review

Advanced Science, Journal Year: 2024, Volume and Issue: 11(22)

Published: April 22, 2024

Abstract Hydrogen‐bonded organic frameworks (HOFs) are emerging porous materials that show high structural flexibility, mild synthetic conditions, good solution processability, easy healing and regeneration, recyclability. Although these properties give them many potential multifunctional applications, their unstable due to the presence of only weak reversible hydrogen bonds. In this work, development history synthesis methods HOFs reviewed, categorize design concepts strategies improve stability. More importantly, significant latest HOF‐related research for addressing energy environmental issues, work discusses advances in storage conversion, substance generation isolation, detection degradation transformation, biological applications. Furthermore, a discussion coupling orientation HOF cross‐cutting fields environment is presented first time. Finally, current challenges, opportunities, advance applications discussed.

Language: Английский

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Recent progress in Cu-based electrocatalysts for CO2 reduction

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159210 - 159210

Published: Jan. 1, 2025

Language: Английский

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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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Lattice Oxygen-Driven Co-Adsorption of Carbon Dioxide and Nitrate on Copper: A Pathway to Efficient Urea Electrosynthesis

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

Published: Feb. 10, 2025

The electrochemical coupling of CO2 and NO3– on copper-based catalysts presents a sustainable strategy for urea production while simultaneously addressing wastewater denitrification. However, the inefficient random adsorption copper surface limits interaction key carbon nitrogen intermediates, thereby impeding efficient C–N coupling. In this study, we demonstrate that residual lattice oxygen in oxide-derived nanosheets (OL-Cu) can effectively tune electron distribution, thus activating neighboring atoms generating electron-deficient (Cuδ+) sites. These Cuδ+ sites enhance stabilize *CO which enables directional at adjacent This mechanism shortens pathway achieves yield up to 298.67 mmol h–1 g–1 −0.7 V versus RHE, with an average Faradaic efficiency 31.71% high current density ∼95 mA cm–2. situ spectroscopic measurements confirmed formation tracked evolution intermediates (i.e., *CO, *NO, *OCNO, *NOCONO) during synthesis. Density functional theory calculations revealed promote coadsorption *NO3, as well *OCNO significantly improving kinetics. study underscores critical role facilitating selectivity.

Language: Английский

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Enhancing C-C Coupling in CO2 Electroreduction by Engineering Pore Size of Porous Carbon-Supported Cu Catalysts

Catalysts, Journal Year: 2025, Volume and Issue: 15(3), P. 199 - 199

Published: Feb. 20, 2025

The electroreduction of CO2 (CO2RR) is a promising and environmentally sustainable approach to closing the carbon cycle. However, achieving high activity selectivity for multicarbon (C2₊) products remains significant challenge due complexity reaction pathways. In this study, porous carbon-supported copper catalysts (CuHCS) with pore sizes 120 nm (CuHCS120) 500 (CuHCS500) were synthesized tailor microenvironment at electrode–electrolyte interface enhance product selectivity. CuHCS120 achieved maximum faradaic efficiency (FE) C2₊ 46%, double that CuHCS500 (23%). contrast, showed higher FE CO (36%) compared (14%) same potential. In-depth ex situ in investigations revealed smaller pores promote enrichment adsorption *CO intermediates, thereby enhancing C–C coupling formation products. These findings underscore critical role structural confinement modulating catalytic provide valuable insights rational design advanced CO2RR.

Language: Английский

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