Size-Dependent Fe-Based Catalysts for the Catalytic Transfer Hydrogenation of α,β-Unsaturated Aldehydes

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Фев. 2, 2025

Metal-based catalysts ranging from nanoparticles (NPs) to the atomic level usually exhibit varying catalytic performance. The underlying size effect is both fascinating and evident. This study thoroughly investigates size-dependent effects of Fe-based on transfer hydrogenation (CTH) furfural (FF) at level. Fe was precisely loaded onto N-doped porous carbon in three forms: single atoms (Fe-SAs/NC), clusters (Fe-ACs/NC), (Fe-NPs/NC). achieved through meticulous control iron precursor composition. Remarkably, Fe-SAs/NC exhibited exceptional efficiency, achieving an FF conversion 91.3% a turnover frequency (TOF) 262.3 h-1 110 °C, which 9.2 times higher than Fe-ACs/NC impressive 93.7 Fe-NPs/NC. high selectivity toward furfuryl alcohol further substantiated by theoretical calculations. These calculations indicated benefits η1(O)-aldehyde adsorption configuration, formed vertical molecules Fe-N4 active sites. Geometrical optimization catalyst scale enhances its intrinsic activity selectivity. proposed provides deeper insights into mechanism single-atom contributes exploration high-performance

Язык: Английский

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Sequestration and Degradation of Waterborne Pollutants in N-Doped Porous Carbon Decorated with Fe Single Sites

ACS ES&T Engineering, Год журнала: 2025, Номер unknown

Опубликована: Март 5, 2025

Recently, advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) have rapidly developed. However, the low concentrations of waterborne pollutants remain a significant obstacle to their effective removal. This study proposes "sequestration-degradation" strategy, utilizing catalyst with high adsorption and catalytic performance enrich low-concentration from water, followed by flushing packed column minimal amount PMS solution achieve pollutant degradation regeneration. Mesoporous carbon decorated single-atom iron (FeN4/NC) was prepared fully characterized. It demonstrated fast kinetics capacity for common pollutants. Additionally, due its activity in activation produce singlet oxygen (1O2) superoxide (O2•–), FeN4/NC can quickly degrade partially mineralize 4-chlorophenol (4-CP). We indicate that is bifunctional material, NC support serving as center 4-CP, while Fe sites serve centers PMS. A proof-of-concept design sequestration rhodamine B constructed using FeN4/NC, demonstrating current wastewater treatment approach concept feasible. Our findings provide new pathway improving efficiency AOPs practical applications.

Язык: Английский

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Rational Design of Carbon‐Based Electrocatalysts for H₂O₂ Production by Machine Learning and Structural Engineering

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Апрель 17, 2025

Abstract Electrochemical synthesis of hydrogen peroxide (H 2 O ) via two‐electron oxygen reduction reaction (2e − ORR) represents an economically viable alternative to conventional anthraquinone processes. While noble metal catalysts have dominated this field, carbon‐based materials are emerging as promising alternatives due their low cost, abundant reserves, and tunable properties. This mini‐review summarizes recent advances in computational methods, particularly the integration density functional theory (DFT) with machine learning (ML), accelerate rational design electrocatalysts by enabling rapid screening structure‐training predictions. Meanwhile, optimization strategies systematically investigated, focusing on four key aspects: atomic‐level heterochromatic doping, defect engineering, microenvironment control, morphological design. Despite significant progress achieving high selectivity activity, challenges remain scaling these for industrial applications. Moving H will require multidisciplinary efforts combining advanced situ characterization techniques, modeling, process engineering develop robust suitable diverse operating conditions.

Язык: Английский

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Optimizing Adsorption‐Catalysis Synergy to Accelerate Sulfur Conversion Kinetics in Room‐Temperature Na‐S Batteries

Small, Год журнала: 2025, Номер unknown

Опубликована: Апрель 25, 2025

Abstract Room‐temperature sodium‐sulfur (RT Na‐S) batteries are expected to become the next‐generation energy storage system due their ultrahigh theoretically density of 1274 Wh kg −1 , abundant sulfur resource, and low cost. However, practical application is hindered by challenges severe shuttle effect sluggish S conversion kinetics. In this study, a series nano‐sized nickel‐based chalcogenides designed fabricated as electrocatalysts for cathode. The p orbitals originated from different anions show great on partial‐filled d orbital metal Ni site, which further regulates electronic states catalytic site. Theoretical experimental results confirm excellent electrocatalytic performance NiSe electrocatalyst with reaction barriers, moderate adsorption capability, strong ability, consistent Sabatier's principle. optimized catalyst presents high reversible capacity 720.4 mAh g durability over 200 cycles at 0.2 A retained 401.4 after 1000 2 in RT Na‐S batteries. This work balancing toward polysulfides via modulation d/p active sites.

Язык: Английский

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Boosting Singlet Oxygen Oxidation of Micropollutants at an Enzyme-like Bifunctional Single-Atom Catalyst Interface

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 8174 - 8184

Опубликована: Май 1, 2025

Язык: Английский

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