Catalysis Science & Technology最新文献

As the combination of Co with other non-noble metals is a viable way to improve the catalytic properties of Co in methane dry reforming (DRM), we studied an impregnated Co₃O₄/β-Ga₂O₃ powder catalyst to understand the influence of Ga and the catalytic role of the Co-Ga₂O₃ interface and the intermetallic compound CoGa in DRM. Co₃O₄/β-Ga₂O₃ undergoes a series of structural transformations during activation by reduction in hydrogen and under DRM conditions. Contact to the CO₂/CH₄ mixture without hydrogen pre-reduction yields CoGa₂O₄ spinel particles encrusting β-Ga₂O₃ without significant DRM activity. Hydrogen reduction transforms Co₃O₄/β-Ga₂O₃ initially to α-Co/β-Ga₂O₃, before it induces reactive metal-support interaction leading to the formation of bimetallic CoGa particles on β-Ga₂O₃. Subsequent improved DRM activity can be correlated to the decomposition of the intermetallic compound CoGa: according to operando X-ray diffraction CoGa re-transforms into α-Co/β-Ga₂O₃ during DRM. Hydrogen pre-reduction is a prerequisite for high DRM activity on Co₃O₄/β-Ga₂O₃, where intermediarily formed CoGa is decomposed under reaction conditions yielding a pronounced increase in the activity rivalling established noble metal and non-noble metal catalysts. A particular advantage of β-Ga₂O₃ is the suppression of coking and Co deactivation, as observed on a Ga-free Co/SiO₂ catalyst.

Correction for ‘Surface analysis of thermally stable Pt loaded CeO₂–ZrO₂ using colloidal Pt for TWC application’ by Hiroki Tanaka et al., Catal. Sci. Technol., 2025, 15, 1473–1481, https://doi.org/10.1039/D4CY01364F.

The conversion of CO₂ to value-added chemical products is one of the hottest scientific topics that is receiving considerable interest. Oxazolidinone, a product derived from CO₂, has received widespread attention due to its potential applications in the preparation of natural products. Here, we report a new heterogeneous polymer-supported magnesium–porphyrin as a photocatalyst for the conversion of CO₂ and aziridines to oxazolidinones under ambient conditions (room temperature and 1 atmosphere CO₂ pressure). We further studied the scope of oxazolidinone synthesis using various aziridines, and the catalyst was successfully reused several times.

The selective hydrogenolysis of C–O bonds in furfuryl alcohol (FFA) into high-value pentanediols is of great significance to the production of bio-based polyesters and polyurethanes. Herein, a supported 5Co/CeO₂ catalyst was designed to facilitate the selective conversion of FFA to 1,5-pentanediol (1,5-PeD). Complete conversion of FFA was achieved within 1 h at 170 °C and 4 MPa H₂, with a 54% selectivity to 1,5-PeD. The production rate reached 13 mol_1,5-PeD mol_Co⁻¹ h⁻¹, the highest value reported so far. The kinetic studies revealed that the reaction rate had a first order dependence on both hydrogen pressure and FFA concentration, with an apparent activation energy of 76 kJ mol⁻¹. Characterization using H₂-TPR, H₂-TPD, and XPS revealed that compared with 5Co/MgO and 5Co/ZrO₂, the 5Co/CeO₂ catalyst had the highest Co⁰/Co²⁺ ratio (0.69) and abundant oxygen vacancies. Moreover, the oxygen vacancy concentration increased with the reduction temperature of 5Co/CeO₂, and linearly correlated with the reaction rate. Raman, FFA-DRIFTS, and substrate control experiments showed that FFA was adsorbed on oxygen vacancies with both the furan oxygen and hydroxyl oxygen atoms. This unique adsorption mode facilitated the ring opening reactions. Co⁰ was responsible for hydrogen activation while the oxygen vacancies from both the interfacial Co²⁺ and CeO₂ were responsible for FFA adsorption. The good synergy between the Co⁰ and the adjacent oxygen vacancies allows the efficient conversion of FFA to 1,5-PeD. This study provides a useful guideline for the design of non-precious metal catalysts for upgrading other biomass-derived molecules via selective hydrogenolysis of C–O bonds.

The electrochemical synthesis of dispersed hydrogen peroxide (H₂O₂) in acidic solutions is of significant interest for the electro-Fenton (EF) process. However, the development of robust and cost-effective catalysts for the selective two-electron oxygen reduction reaction (2e-ORR) remains a challenge. In this study, inspired by the hydrophobic surface of natural rose petals and mimicking their microstructure, we utilized the high adhesion property of polytetrafluoroethylene (PTFE) to bind highly conductive acetylene carbon black (ACET) onto the surface of graphite felt wire mesh. This formed a low-surface-energy, fluorine-doped hydrophobic cathode with a rough and defect-rich surface, optimized for gas diffusion. The cathode demonstrated an impressive H₂O₂ generation rate of 46.21 mg h⁻¹ cm⁻², meeting the requirements for the EF process. In continuous operation, the electrode exhibited exceptional catalytic performance and stability. This can be attributed to the variations in electron distribution density induced by F/C doping and surface defects, where high-density electron domains attract oxygen molecules at the interfaces of hydrated hydrogen ion (H₃O⁺) clusters, promoting the formation of the *OOH intermediate. The hydrophobicity of the interfaces weakly bind to *OOH, favouring desorption to enhance H₂O₂ generation and prevent the side reaction of hydrogen evolution on the wetted electrode surface and further reduction of generated H₂O₂ to H₂O. This study provides a new strategy for designing efficient and stable cathodes to guide future catalyst discovery.

A Pt-assisted MoO₃/g-C₃N₄ photocatalyst (Pt/5MoO₃/g-C₃N₄) was designed and synthesized for the selective photocatalytic reduction of CO₂ to CH₄. The structure, morphology, and chemical states of the catalyst were systematically analyzed using XRD, XPS, SEM, and TEM. The formation of an S-type heterojunction between MoO₃ and g-C₃N₄ effectively promoted charge separation and migration, enhancing photocatalytic efficiency. Pt, as a co-catalyst, facilitated charge transfer, reduced recombination, and improved CH₄ selectivity. The Pt/5MoO₃/g-C₃N₄ catalyst achieved a CH₄ production rate of 34.9 μmol g⁻¹ h⁻¹, 2.2 times higher than that of g-C₃N₄, with 100% CH₄ selectivity. In situ FTIR and XPS analyses confirmed that Pt⁰ acted as the primary catalytic site, while MoO₃ contributed to CO₂ adsorption and intermediate stabilization. Photoelectrochemical tests further demonstrated the synergistic effect of the S-type heterojunction and Pt co-catalyst, leading to enhanced charge separation and reduced interfacial charge transfer resistance. Moreover, Pt/5MoO₃/g-C₃N₄ exhibited excellent stability and recyclability. This study highlights the effectiveness of S-type heterojunction engineering and Pt co-catalysts in improving photocatalytic CO₂ reduction efficiency and selectivity.

Herein, we report an efficient methodology for the preparation of a heterogeneous sustainable magnetically separable Cu@PANI@Fe₃O₄ nanocomposite, and its catalytic efficiency in multicomponent reactions for the synthesis of triazolo quinolines and triazolyl benzamide derivatives is investigated. The Cu@PANI@Fe₃O₄ nanocomposite is characterized by several analytical techniques such as PXRD, FE-SEM, ICP-OES, HR-TEM, XPS, VSM, and TG-DTA to understand its crystallinity, chemical composition, morphology, and magnetic properties. A series of triazolo quinolines and triazolyl benzamide derivatives are synthesized in good to excellent yields under greener reaction conditions. A detailed mechanistic investigation by control experiments and DFT calculations has been performed to validate the proposed mechanism. Additionally, anti-cancer studies of the synthesized triazolo quinoline derivatives were performed and they were screened against colon carcinoma cell lines (HCT116) and subjected to MTT assay, showcasing good activity against the cells with IC₅₀ of 28–45 μM. Further, gram-scale synthesis, recyclability of the nanocomposite and its utility in up to five consecutive cycles were deliberated.

Plasma catalysis is recognized as a promising technology for the elimination of methane. However, co-existence of moisture in flue gas reduces significantly the adsorption capacity of catalysts toward CH₄. Herein, Ni–Mn/SiO₂ catalysts were tuned by controlling the Ni/Mn molar ratio and subjected to hydrophobic treatment using myristic acid to promote methane oxidation under humid conditions. The plasma–catalytic system demonstrated a substantial improvement in CH₄ conversion and CO₂ selectivity compared to the plasma-only system owing to the synergistic effects of plasma and catalysis on methane degradation. The increase in the Mn/Ni molar ratio promotes the formation of Mn⁴⁺ on the catalyst surface and increases the specific surface area, facilitating the migration and adsorption of reactive oxygen species, which further improves the catalytic activity of methane oxidation reaction. In the presence of 5% water vapor, Ni–Mn(1 : 1)/SiO₂–MA exhibited the highest CH₄ conversion of 93.5% at 40 W. Due to the introduction of myristic acid with non-polar alkyl groups, a highly hydrophobic surface was obtained on modified catalysts, preventing the coverage of the active sites and promoting CH₄ adsorption. This study provides a new and viable solution to improve the performance of catalysts in methane oxidation under high-humidity conditions.

Efficient and selective catalytic hydrogenation of amides to amines is highly significant but extremely challenging. Here, a series of Ru/TiO₂ catalysts were prepared with the impregnation method at different calcination and reduction temperatures. Multiple characterization tools were used to characterize the physicochemical properties of the catalysts. The hydrogenation of butyramide to butylamine as a model reaction was used to evaluate the catalytic performance. The catalytic activity of the Ru catalyst supported on rutile TiO₂ was superior to that on anatase TiO₂. As the calcination temperature increased from 200 °C to 600 °C, the catalytic performance of Ru/rutile catalysts monotonously decreased. With the reduction temperature increasing from 200 °C to 600 °C, Ru/rutile catalysts displayed a volcano-like trend of catalytic activity. The Ru/rutile catalyst calcined at 200 °C and reduced at 500 °C exhibited the highest catalytic performance, with 93% butyramide conversion and 65% selectivity to butylamine at 150 °C with 5 MPa H₂. The evaluation and characterization results suggested that the lattice match between RuO₂ and rutile TiO₂ prevented Ru particle aggregation under high-temperature calcination, and smaller Ru particles were in favor of the amide hydrogenation reaction. The coverage of the TiO_x overlayer on Ru nanoparticles and the Ru–TiO_x boundary perimeter were effectively modulated by the strong metal–support interaction under different catalyst reduction temperatures, resulting in the optimization of the amide hydrogenation reactivity over Ru/rutile catalysts. This study facilitates the understanding of the influence of strong metal–support interaction on the catalytic hydrogenation of amide.

TiO₂-supported Au nanocatalysts are highly attractive for visible light photocatalysis owing to their efficient surface plasmon resonance (SPR) and superior intrinsic catalytic activity. The prevailing strategies to prepare high-performance plasmonic Au/TiO₂ include constructing highly active Au–TiO₂ interfaces by modulating the electronic and geometric properties of Au nanoparticles or the TiO₂ support. Herein, we report a synergism of an Fe-doped TiO₂ (Fe@TiO₂) support and cold plasma treatment for the preparation of an Au/Fe@TiO₂–P catalyst, enabling this Au nanocatalyst to outperform samples fabricated via classical methods for the visible light photocatalytic oxidation of CO. The key to this collaborative preparation is treating the Au species on Fe@TiO₂ derived from hydrothermal synthesis with cold plasma, which constructs large numbers of Au–Fe@TiO₂ interfaces by generating unique interactions between Au nanoparticles and the support. The Au/Fe@TiO₂–P catalyst features high dispersion of Au and abundant surface oxygen species, thus accelerating the visible light photocatalytic oxidation of CO along the hot-electron transfer reaction pathway. This investigation demonstrates a promising approach to design and construct high-performance supported Au nanocatalysts for visible light photocatalysis.