Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis

Chemical Reviews, Год журнала: 2024, Номер 124(20), С. 11348 - 11434

Опубликована: Окт. 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.

Язык: Английский

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Metal–N₄ model single‐atom catalyst with electroneutral quadri‐pyridine macrocyclic ligand for CO₂ electroreduction

Carbon Energy, Год журнала: 2024, Номер 6(8)

Опубликована: Фев. 15, 2024

Abstract Metal–N–C single‐atom catalysts, mostly prepared from pyrolysis of metal‐organic precursors, are widely used in heterogeneous electrocatalysis. Since metal sites with diverse local structures coexist this type material and it is challenging to characterize the structure, a reliable structure–property relationship difficult establish. Conjugated macrocyclic complexes adsorbed on carbon support well‐defined models mimic catalysts. Metal–N 4 site four electroneutral pyridine‐type ligands embedded graphene layer most commonly proposed structure active but its molecular counterpart has not been reported. In work, we synthesized conjugated center (Co, Fe, or Ni) coordinated pyridinic as model catalysts for CO 2 electroreduction. For comparison, anionic quadri‐pyridine ligand were also prepared. The Co complex expressed turnover frequency formation more than an order magnitude higher that ligand. Constrained ab initio dynamics simulations based indicate possesses stronger ability mediate electron transfer .

Язык: Английский

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Adjustable Selectivity for CO₂ Electroreduction to Ethylene or Ethanol by Regulating Interphases Between Copper and Tin Oxides

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 10, 2025

Abstract Enhancing the selectivity of C 2 products and revealing reaction mechanisms in CO electroreduction (CO RR) remain challenging. Regulating interphases catalysts is one most promising pathways. Herein, between copper (Cu) tin (Sn) oxides are regulated by controlling degree reduction during self‐assembly process, which exhibits obvious different to ethylene ethanol, respectively. The interphase Cu‐SnO ethanol as high 74.6%, while Cu O‐SnO shows 71.4% at –0.6 V versus RHE. In situ Fourier‐transform infrared spectroscopy measurements density functional theory calculations demonstrate that strong electron interaction, preferentially forming key *COH intermediates for asymmetrical C─C coupling produce ethanol. contrast, possesses oxygen vacancies both sites, thus enriching *CO symmetrical interphase. findings this work offer an advanced strategy regulating adjust RR.

Язык: Английский

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Planar chlorination engineering induced symmetry-broken single-atom site catalyst for enhanced CO2 electroreduction

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Фев. 15, 2025

Abstract Breaking the geometric symmetry of traditional metal-N 4 sites and further boosting catalytic activity are significant but challenging. Herein, planar chlorination engineering is proposed for successfully converting Zn-N site with low selectivity CO 2 reduction reaction (CO RR) into highly active 3 broken symmetry. The optimal catalyst Zn-SA/CNCl-1000 displays a highest faradaic efficiency (FE ) around 97 ± 3% good stability during 50 h test at high current density 200 mA/cm in zero-gap membrane electrode assembly (MEA) electrolyzer, promising application industrial catalysis. At -0.93 V vs. RHE, partial ( J turnover frequency (TOF) value catalyzed by 271.7 1.4 29325 151 -1 , as 29 times 83 those Zn-SA/CN-1000 without engineering. in-situ extended X-ray absorption fine structure (EXAFS) measurements functional theory (DFT) calculation reveal adjacent C-Cl bond induces self-reconstruction symmetry, strengthening adsorption * COOH intermediate, thus remarkably improving RR activity.

Язык: Английский

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In-situ characterization technologies and theoretical calculations in carbon dioxide reduction: In-depth understanding of reaction mechanisms and rational design of electrocatalysts

Coordination Chemistry Reviews, Год журнала: 2025, Номер 533, С. 216541 - 216541

Опубликована: Фев. 28, 2025

Язык: Английский

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