Atomically Dispersed Ga Synergy Lewis Acid‐Base Pairs in F‐doped Mesoporous Cu₂O for Efficient Eletroreduction of CO₂ to C₂₊ Products

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: April 22, 2024

Abstract Electroreduction of CO 2 into high‐value chemicals and fuels driven is an effective way to alleviate the environmental crisis, but it suffers from poor activity low selectivity catalyst. Single‐atom catalysts have excellent highest atomic efficiency, are widely used in 2‐electron transfer produce CO. However, electroreduction C 2+ products involves complex processes such as multi‐electron reaction competitive adsorption, so single‐atom catalysis often powerless. Herein, a Ga‐anchored F‐doped Cu O catalyst with dual active sites reported. The Lewis acid‐base pairs Ga single atom promote adsorption/activation dissociation water molecules, respectively, enhance coverage *CO *H, their synergy optimizes path. At high current density 600 mA cm −2 , FE C2+ reached 72.8 ± 3.2% remarkable stability. Experiments theory calculations demonstrate that increase key intermediate transformed *CHO through protonation reaction, which changes path C─C coupling (*OCCO) followed by (*OCCHO) energy barrier, greatly improving for products.

Language: Английский

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Heteroatoms Modulate the Copper Single Atom Catalytic Host Materials for Promoting the Redox Reaction in Aqueous Zinc‐Selenium Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract Aqueous zinc‐selenium (Zn‐Se) batteries have garnered much attention due to their inherent safety and high specific capacity. Unfortunately, the problem of sluggish redox reaction represents a significant obstacle development aqueous Zn‐Se batteries. Here, nitrogen‐phosphorus asymmetrically coordinated copper single atom catalytic host material (CuN 3 P 1 @C) is synthesized for an battery. The CuN @C exhibits rich porous structure, high‐loading Cu atoms, unique asymmetric coordination environment, which significantly reduces energy barrier between Se Zn, enhancing electrochemical performance Consequently, Se/CuN cathode achieves capacity 756 mAh g −1 at 0.2 A cycling stability 4 000 cycles 5.0 (capacity decay 0.0044% per cycle). Meanwhile, conversion mechanism battery systematically explored via systematical characteristics density functional theory calculations. This work opens up novel approach boosting by modulating atom‐based materials heteroatoms.

Language: Английский

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Site-designed dual-active-center catalysts for co-catalysis in advanced oxidation processes

npj Materials Sustainability, Journal Year: 2025, Volume and Issue: 3(1)

Published: Jan. 7, 2025

Abstract Advanced Oxidation Processes (AOPs) are promising for treating persistent pollutants, yet challenges arise due to the step-wise oxidants activation process, which traditional single-active-center catalysts struggle facilitate effectively. Recently, dual-active-center have emerged as a solution by enabling synergistic reactions. This review covers advances in these catalysts, their co-catalytic mechanisms, and applications electro-Fenton, photocatalytic, peroxymonosulfate-, pollutant-as-electron-donor based Fenton-like processes, along with active site design considerations future challenges.

Language: Английский

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Tailoring CO₂ Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate

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

Published: Feb. 5, 2025

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) orientate the transition adsorption configuration from C,O-side O-end, which triggers a shift activated first-step protonation C–C coupling, thus switching target product HCOOH in Faraday efficiency (FE: 90.6%) on FeN2S2 CH3COOH 82.3%) Fe4S4/FeN2S2. The strength *OCHO upon solitary site is linearly related coordination number Fe–S, with predominantly produced over single-atom (ortho-substituted S atoms). Fe4S4 cluster functions as switch reduction product, can not only optimize electronic structure neighboring but also impel complete hydrocarbon intermediate *CH3, followed coupling CO2* *CH3 via synergistic catalysis This strategy provides new avenue modulate reactant model desirable pathways, potential applications diverse multistep electrochemical processes controlled selectivity.

Language: Английский

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Enigma of Sustainable CO₂ Conversion to Renewable Fuels and Chemicals Through Photocatalysis, Electrocatalysis, and Photoelectrocatalysis: Design Strategies and Atomic Level Insights

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

Published: Jan. 2, 2025

Growing global population, escalating energy consumption, and climate change threaten future security. Fossil fuel combustion, primarily coal, oil, natural gas, exacerbates the greenhouse effect driving warming through CO

Language: Английский

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Metal‐Organic Frameworks‐Based Copper Catalysts for CO₂ Electroreduction Toward Multicarbon Products

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

Published: Feb. 12, 2025

ABSTRACT Copper (Cu) is the most promising catalyst for electrochemical CO 2 ‐to‐C 2+ conversion, whereas performance remains below practical thresholds due to high energy barrier of C−C coupling and lack effective approaches steer reaction pathway. Recent advances show that metal‐organic frameworks (MOF) could be a platform as support, pre‐catalyst, co‐catalyst modify electronic structure local environment Cu catalysts promoting reduction by virtue their great tunability over compositions pore architectures. In this review, we discussed general design principles, catalytic mechanisms, achievements MOF‐based catalysts, aiming boost refinement steering pathway C products. The fundamentals challenges are first introduced. Then, summarized conceptions from three aspects: engineering properties Cu, regulating environment, managing site exposure mass transport. Further, latest progress products namely Cu‐based MOF, MOF‐derived Cu@MOF hybrid discussed. Finally, future research opportunities strategies suggested innovate rational advanced electrifying transformation.

Language: Английский

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Theoretical research on efficient electrocatalysis of CO2 reduction reaction by borophene loaded transition metals

Surfaces and Interfaces, Journal Year: 2024, Volume and Issue: 49, P. 104454 - 104454

Published: May 9, 2024

Language: Английский

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Boron-Doped Dinickel Phosphide to Enhance Polysulfide Conversion and Suppress Shuttling in Lithium–Sulfur Batteries

ACS Nano, Journal Year: 2024, Volume and Issue: 18(27), P. 17774 - 17785

Published: June 28, 2024

Lithium–sulfur (Li–S) batteries are promising for next-generation high-energy energy storage systems. However, the slow reaction kinetics render mobile polysulfides hardly controlled, yielding shuttling effects and eventually damaging Li metal anodes. To improve cyclability of Li–S batteries, high-efficiency catalysts desired to accelerate polysulfide conversion suppress effect. Herein, we studied a doping system with Ni2P Ni2B as end members found B-doped catalyst that demonstrates high activity batteries. As anionic dopants, B an interesting reverse electron transfer P tunes electronic structure dramatically. The resultant exhibits short Ni–B bonds strong Ni–S interaction, donation further enhances adsorption on catalysts. S–S were activated appropriately, therefore decreasing low barrier reactions.

Language: Английский

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Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(20), P. 11348 - 11434

Published: Oct. 9, 2024

Environmental catalysis has emerged as a scientific frontier in mitigating water pollution and advancing circular chemistry reaction microenvironment significantly influences the catalytic performance efficiency. This review delves into engineering within liquid-phase environmental catalysis, categorizing microenvironments four scales: atom/molecule-level modulation, nano/microscale-confined structures, interface surface regulation, external field effects. Each category is analyzed for its unique characteristics merits, emphasizing potential to enhance efficiency selectivity. Following this overview, we introduced recent advancements advanced material system design promote (e.g., purification, transformation value-added products, green synthesis), leveraging state-of-the-art technologies. These discussions showcase was applied different reactions fine-tune regimes improve from both thermodynamics kinetics perspectives. Lastly, discussed challenges future directions engineering. underscores of intelligent materials drive development more effective sustainable solutions decontamination.

Language: Английский

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Improved performances toward electrochemical carbon dioxide and oxygen reductions by iron-doped stannum nanoparticles

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

Published: Jan. 1, 2025

We have designed a catalyst that can efficiently convert CO 2 into through Zn–CO batteries and the electrochemical RR, addressing both energy conversion environmental concerns simultaneously.

Language: Английский

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