Heterogeneous Mn@CeO2 Catalyst for α-Alkylation of Ketones with Alcohols via Hydrogen-Borrowing Strategy DOI Creative Commons

Rajagopal Swaathy,

S. Karthikeyan

ACS Omega, Journal Year: 2025, Volume and Issue: 10(9), P. 9649 - 9660

Published: Feb. 24, 2025

Construction of a C-C bond via alkylation ketones with alcohol as the alkylating source by employing hydrogen-borrowing strategy is attracting significant attention and highly appealing due to its simplicity, cost-effectiveness, environmental benefits, fact that water only byproduct. The development heterogeneous catalysts based on nonprecious base metals progressing rapidly. Our newly disclosed manganese-doped cerium oxide nanocomposite (10 wt % Mn@CeO2) stands out cost-efficient air-stable catalyst, synthesized through straightforward coprecipitation method employed for α-alkylation primary alcohols strategy. X-ray diffraction (XRD) analysis confirms high crystallinity CeO2, while field emission scanning electron microscopy (FE-SEM) high-resolution transmission (HR-TEM) images reveal MnO2 nanoparticles, measuring 19 nm in size, uniformly decorated rod-shaped CeO2 which have size 33 nm. photoelectron spectroscopy (XPS) uncovers presence Mn4+ species embedded nanorods. Electron paramagnetic resonance (EPR) further indicates surface defects contribute impressive catalytic yield, ranges from 70 98% α-alkylated ketones. Thermogravimetric (TGA) demonstrates remarkable thermal stability maintaining up 800 °C. Additionally, inductively coupled plasma mass spectrometry (ICP-MS) no leaching Mn ions, emphasizing heterogeneity catalyst. Remarkably, 10 Mn@CeO2 recycled six cycles loss activity. This study underscores synergistic effect between metal redox pair key exceptional activity reactions, making promising catalyst sustainable efficient formation.

Language: Английский

Bio-Inspired Iron-Based Carbonic Anhydrase Mimic for CO2 Hydration and Conversion DOI

Fuying Zhu,

Haochen Qiu,

Fei Wang

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2023, Volume and Issue: 11(19), P. 7388 - 7397

Published: May 4, 2023

CO2 conversion by stable, cost-effective carbonic anhydrase (CA)-like nanozymes emerges as an efficient and sustainable approach for fixation. In this work, a novel iron-based nanomaterial (Fe10@CN-Mg) was first reported to be CA mimic, in which FeNx sites Mg(OH)2 play synergistically catalytic effect conversion. Although material has much lower metal content cost, it comparable kinetic constants (Km 6.37 mM Vmax 30.74 mM/min) significantly higher CaCO3 formation rate (20.60 g·g–1·h–1, the quality of produced per hour gram catalyst) than that mimics. Fe10@CN-Mg is stable when processed at extreme pH, high temperature, organic solvents, ionic strength also retains activity after long storage times (two months) seven cycles. addition, successfully applied convert into cyclic carbonates with economic efficiency.

Language: Английский

Citations

11
In Situ Fe/Co/B Codoped MoS2 Ultrathin Nanosheets Enable Efficient Electrocatalytic Nitrogen Reduction DOI

Jun‐Yang Ji,

Wei Zhang, Cong Li

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(32), P. 41734 - 41742

Published: Aug. 2, 2024

The development of sustainable and effective electrochemical nitrogen fixation catalysts is crucial for the mitigation terrible energy consumption resulting from Haber-Bosch process. Molybdenum disulfide (MoS2) exhibits promise toward reduction reaction (NRR) on account its similar structure to natural nitrogenases MoFe-co but still undergoes serious challenges with unsatisfactory catalytic performance resulted limited active sites, conductivity, selectivity. In this work, Fe/Co/B codoped MoS2 ultrathin nanosheets are synthesized verified as excellent NRR high activity, selectivity, durability. FeCoB-MoS2 demonstrates a ammonia yield 36.99 μg h–1 mgcat–1 at −0.15 V vs RHE Faraday efficiency (FE) 30.65% −0.10 in 0.1 M HCl. experimental results density functional theory (DFT) calculations emphasize that codoping Fe, Co, B into synergistically enhances conductivity optimizes electronic catalyst, which significantly improves electrocatalytic synthesis performance. This work broadens potential enlightens strategy designing efficient electrocatalysts field.

Language: Английский

Citations

4
Selective Synthesis of Amines by Heterogeneous Co Catalysts via Borrowing Hydrogen Protocols DOI
Endah Suarsih, Yusuke Kita, Keigo Kamata

et al.

Organic Letters, Journal Year: 2025, Volume and Issue: 27(4), P. 1024 - 1029

Published: Jan. 21, 2025

Developed Co-MgO/TiO2 was applicable to C-N bond formation by direct amination of primary and secondary alcohols with NH3 via a borrowing hydrogen protocol. Selective synthesis primary, secondary, tertiary amines achieved controlling the reaction conditions. Asymmetric can be synthesized coupling amines.

Language: Английский

Citations

0
Selective Hydrodeoxygenation of Lignin‐Derived Phenolic Monomers to Cyclohexanol over Tungstated Zirconia Supported Ruthenium Catalysts DOI
Quan Gan, Weihao Zhou, Xueping Zhang

et al.

ChemSusChem, Journal Year: 2024, Volume and Issue: unknown

Published: June 24, 2024

Abstract The selective hydrodeoxygenation (HDO) of lignin‐derived methoxyphenols to cyclohexanol is one the most significant transformation in biomass conversion since an important industrial raw material. This study has disclosed a series tungstated zirconia with different Zr/W ratio supported Ru catalysts (Ru/xZrW, x means molar ration Zr/W) for guaiacol cyclohexanol. Among these catalysts, Ru/16ZrW best catalytic activity, which can achieve 92 % yield under conditions 180 °C and 1 MPa H 2 pressure h (TOF 231 −1 ). Compared Ru/ZrO , smaller particles, more dispersed electron‐rich species, hydrogen spillover acid sites, are main reason its excellent performance on this reaction. Apart from guaiacol, other methoxy substitution phenols organosolv lignin also be converted into via reactions over catalyst.

Language: Английский

Citations

3
Heterogeneous Mn@CeO2 Catalyst for α-Alkylation of Ketones with Alcohols via Hydrogen-Borrowing Strategy DOI Creative Commons

Rajagopal Swaathy,

S. Karthikeyan

ACS Omega, Journal Year: 2025, Volume and Issue: 10(9), P. 9649 - 9660

Published: Feb. 24, 2025

Construction of a C-C bond via alkylation ketones with alcohol as the alkylating source by employing hydrogen-borrowing strategy is attracting significant attention and highly appealing due to its simplicity, cost-effectiveness, environmental benefits, fact that water only byproduct. The development heterogeneous catalysts based on nonprecious base metals progressing rapidly. Our newly disclosed manganese-doped cerium oxide nanocomposite (10 wt % Mn@CeO2) stands out cost-efficient air-stable catalyst, synthesized through straightforward coprecipitation method employed for α-alkylation primary alcohols strategy. X-ray diffraction (XRD) analysis confirms high crystallinity CeO2, while field emission scanning electron microscopy (FE-SEM) high-resolution transmission (HR-TEM) images reveal MnO2 nanoparticles, measuring 19 nm in size, uniformly decorated rod-shaped CeO2 which have size 33 nm. photoelectron spectroscopy (XPS) uncovers presence Mn4+ species embedded nanorods. Electron paramagnetic resonance (EPR) further indicates surface defects contribute impressive catalytic yield, ranges from 70 98% α-alkylated ketones. Thermogravimetric (TGA) demonstrates remarkable thermal stability maintaining up 800 °C. Additionally, inductively coupled plasma mass spectrometry (ICP-MS) no leaching Mn ions, emphasizing heterogeneity catalyst. Remarkably, 10 Mn@CeO2 recycled six cycles loss activity. This study underscores synergistic effect between metal redox pair key exceptional activity reactions, making promising catalyst sustainable efficient formation.

Language: Английский

Citations

0