ACS Catalysis
·
2026
·
IF 13.6
Yang Pan,Zhou Xiaomei,Hou Yufeng,Guan Qingxin,Li Wei
Competitive H 2 oxidation severely limits CO 2 selectivity (typically <50%) during preferential CO oxidation (CO-PROX) on Pt catalysts. While metal–oxide interfaces can potentially circumvent this trade-off, constructing architectures that spatially decouple CO and H 2 activation remains challenging. Here, we report a junction-confined FeO-Pt/SiO 2 catalyst in which FeO species selectively decorate Pt nanoparticles, creating well-defined and closely contacted interfacial sites. Unlike randomly distributed FeO in conventional catalysts, this configuration enables electron redistribution from Pt to FeO, as revealed by Bader charge analysis. This electronic effect preserves strong CO adsorption on Pt (required for CO activation) while dramatically enhancing O 2 activation at the interface. Consequently, CO oxidation proceeds via a dominant low-barrier interfacial pathway (0.20 eV), while weakened H 2 adsorption at the FeO–Pt junction mitigates competitive H 2 oxidation under H 2 -rich conditions. The catalyst achieves >70% CO 2 selectivity at complete CO conversion over 80–160 ° C and maintains stability for 100 h without noticeable deactivation under H 2 -rich conditions. This work demonstrates that precise spatial organization of metal–oxide interfaces can effectively decouple competitive reaction pathways, offering a generalizable strategy for designing selective oxidation catalysts beyond CO-PROX.
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THIN SOLID FILMS
·
2023
·
IF 2.1
Xinkuai He,Ruqing Guo,Qingtian Zou,Jingjing Yang,Zhousi Hu,Luye Wu
The co-deposition behavior of Co +2 and Fe +2 in ethylene glycol (EG) are investigated using cyclic voltammetry (CV) techniques. These results imply that Co +2 species can accelerate the Co-Fe co-deposition, while Fe +2 can inhibit the reduction of Co +2 . Moreover, the two effects can be improved as Co +2 or Fe +2 concentration increases. Microstructural and compositional characteristics of the samples show that Co-Fe deposits with various Fe content can be obtained from anhydrous FeCl 2 and CoCl 2 in EG. Scanning electron microscopy imaging of the surfaces of these Co-Fe alloy coatings shows that they present a dense structure with spherical “nodules”, the size of which is related to the Fe content. The electrocatalytic activity for hydrogen evolution reaction (HER) on the Co-Fe coatings is also investigated. These results indicate that its electrocatalytic activity can be improved as Fe contents increase from 2.2 to 9.8 wt.% and the Co-Fe alloy with 9.8 wt.% Fe exhibits the high electrocatalytic activity for HER with an overpotential of 124 mV at 10 mA cm −2 in 1 M KOH.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Luo Huihui,Tian Shuainan,Liang Hongliang,Wang He,Gao Shuang,Dai Wen
The cleavage and functionalization of C–S bonds have become a rapidly growing field for the design or discovery of new transformations. However, it is usually difficult to achieve in a direct and selective fashion due to the intrinsic inertness and catalyst-poisonous character. Herein, for the first time, we report a novel and efficient protocol that enables direct oxidative cleavage and cyanation of organosulfur compounds by heterogeneous nonprecious-metal Co-N-C catalyst comprising graphene encapsulated Co nanoparticles and Co-Nx sites using oxygen as environmentally benign oxidant and ammonia as nitrogen source. A wide variety of thiols, sulfides, sulfoxides, sulfones, sulfonamides, and sulfonyl chlorides are viable in this reaction, enabling access to diverse nitriles under cyanide-free conditions. Moreover, modifying the reaction conditions also allows for the cleavage and amidation of organosulfur compounds to deliver amides. This protocol features excellent functional group tolerance, facile scalability, cost-effective and recyclable catalyst, and broad substrate scope. Characterization and mechanistic studies reveal that the remarkable effectiveness of the synergistic catalysis of Co nanoparticles and Co-Nx sites is crucial for achieving outstanding catalytic performance.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
·
2023
·
IF 5
Pingfu Huang,Hui Yan,Hao Wu,Lulu Liu,Wenmin Niu,Bo Zhai,Ziwei Hu,Jingjuan Li,Qianming Du,Yang Zhou
The co-amorphous (CAM) system has attracted widely attention for improving the solubility of poor water solubility drug and provide a formulation strategy for combination administration system. Paclitaxel (PTX) belongs to biopharmaceutics classification system (BCS) class Ⅳ drug, with the poor water solubility and membrane permeability. This study aimed to preparing the CAM system between PTX and curcumin (CUR) by rotary evaporation method. The solid-state characterization of CAM indicated that the PTX and CUR presented as amorphous state, compared with crystalline PTX and CUR, the amorphous system could improve the saturated solubility and dissolution with significantly difference, besides, the PTX absorption permeability increased after amorphization with CUR, and the rat pharmacokinetic study exhibited that the PTX-CUR had a high C max and AUC 0-∞ compared with crystalline CUR and PTX, Furthermore, the amorphous CUR and PTX exhibited the stronger anti-tumor efficacy in A549 cell model in vivo . In addition, PTX-CUR exhibited physical stability under the long-term storage condition. In conclusion, amorphization of PTX and CUR provided a promising mothed to improve the anti-tumor efficacy and oral bioavailability of PTX.
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DALTON TRANSACTIONS
·
2018
·Vol. 48
·期 2
·468-477
·
IF 4.099
Zhiyin Xiao,Ran Jiang,Jing Jin,Xiuqin Yang,Binyu Xu,Xiaoming Liu,Yabing He,Yi He
Four diiron(II) carbonyl complexes, [Fe2(μ-SR)3(CO)5X] (X− = Br−, I−; R = CH2CH3, CH2CH2CH3) were facilely synthesized by reacting [Fe(CO)4X2] with monothiolates. Their potential as carbon monoxide-releasing molecules (CORMs) was systematically investigated, revealing that their CO-releasing behaviour is highly solvent-dependent. Specifically, in dimethyl sulfoxide (DMSO), the CO-releasing kinetics were fast. Intermediates with a lower oxidation state might be involved in the reaction. By contrast, in less polar solvents such as methanol, acetonitrile and dichloromethane, intermediates featuring the triiron carbonyl cation, [Fe3(μ-SCH2CH3)6(CO)6]+, were isolated. The triiron intermediate underwent further decomposition to liberate CO. One of the iodo complexes was also examined for its CO-release in PBS solution when solubilised with DMSO in the presence of deoxy-Mb and the CO-release was found to be quantitative. Furthermore, kinetic analyses were performed and the CO-release in general obeyed a first-order kinetic model. Plausible CO-releasing pathways are proposed for the parent complexes and the triiron intermediate. Assessments in cytotoxicity indicated that the cytoxicity of the diiron(II) complexes varied with both the halide and thiolate and those bearing bromide and the thiolate with longer chains were more biocompatible.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yang Li,Xuemei Diao,Peicheng Li,Panpan Liu,Yan Gao,Zhiyong Zhao,Xiao Chen,Ge Wang
To cope with the complex and changeable extreme environments, extending multifunctionality is crucial for potable smart wearable composite phase change materials (PCMs). Herein, we developed advanced Co/N co-doped carbon foam-based multifunctional “five-in-one” composite PCMs integrating dual-temperature thermal management, light-triggered heating, waterproof, flame retardant, and microwave absorption through high-temperature calcination of melamine foam@ZIF67 and melting encapsulation of paraffin wax (PW). Benefiting from the strong full-spectrum absorption, fast photon and phonon transport, and local surface plasmon resonance effect, our designed foam-based composite PCMs exhibited an ultrahigh photothermal conversion efficiency of 95.17 %. More importantly, foam-based composite PCMs demonstrated excellent thermal management, structural stability and thermal storage stability after undergoing 300 heating–cooling cycles. Furthermore, foam-based composite PCMs showed superior microwave absorption (RL min = -57.93 dB), good flame retardancy and satisfactory hydrophobicity (contact angle > 100°). Thus, our developed multifunctional foam-based composite PCMs provide great potential for personalized thermal management and anti-radiation smart wearables even in harsh environments (e.g., rain, snow, sweat, fire, extreme cold, extreme heat and electromagnetic interference), creating a versatile platform for smart wearable light-triggered phase change heater with on-demand properties.
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DALTON TRANSACTIONS
·
2013
·Vol. 42
·期 44
·15663-15669
·
IF 3.806
Li Long,Xiujuan Jiang,Xiu Wang,Zhiyin Xiao,Xiaoming Liu
A water soluble diiron hexacarbonyl complex, [Fe2{μ-SCH2CH(OH)CH2(OH)}2(CO)6] (1), was synthesised by reacting thioglycol with Fe3(CO)12 in THF. This diiron complex was employed as carbon monoxide releasing molecule (CO-RM). The CO-releasing was initiated via substitution of the bound CO by cysteamine (CysA, a clinic medicine). Further decomposition of the substituted products led to at least partially the formation of monoiron(II) dicarbonyl species via oxidative process while releasing more CO under inert atmosphere. Three intermediates generated in the CO-releasing process were spectroscopically identified. The kinetics of the decomposition of complex 1 was first-order process for both the complex and CysA, respectively. Under open atmosphere, the CO-releasing mechanism altered due to the involvement of oxygen in the decomposition of complex 1. The system showed minimal cytotoxicity in two selected arbitrarily cell lines, QSG-7701 and HepG2, with IC50 at the scale of 100 μmol L−1.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Peiyan Lin,Renhong Chen,Sheng Xu,Xia Xia,Fang Zhao,Xuefeng Ren,Yumeng Lu,Liguo Gao,Junjiang Bao,Anmin Liu
Electrocatalytic nitrate (NO3−) reduction to ammonia (NH3) has emerged as an environmentally friendly method for ammonia production due to its clean, efficient, and sustainable attributes. In this study, we prepared Co-doped TiO2 materials with graphene oxide (GO), Co–TiO2/GO, as potential NO3−RR electrocatalysts. Scanning electron microscopy (SEM) images revealed a spherical structure for the catalysts. Following a series of electrochemical tests, our findings indicated that Co-doping significantly enhances the NO3−RR activity of TiO2. Furthermore, incorporating GO notably diminishes the initial potential of titania-based catalysts, thereby strengthening the NO3−RR performance of TiO2. The engineered Co–TiO2/GO exhibits superior NO3−RR electrochemical properties, achieving an NH3 yield of up to 7.424 mg h−1 cm−2 and a Faraday efficiency of up to 56.5% at −1.1 V vs. RHE potential. This performance surpasses that of Co–TiO2, with minimal by-product NO2− generation. We also conducted tests without the catalyst and in the absence of NO3− in the electrolyte, confirming that the nitrogen in the synthesized ammonia was not derived from impurities in the catalyst or the electrolyte. Furthermore, Co–TiO2/GO demonstrated robust stability during eight cycles and 24 hours of continuous testing for the NO3−RR performance. Theoretical calculations suggest that doping TiO2 with Co and GO can enhance its electronic structure and conductivity, thereby facilitating the electrochemical synthesis of ammonia.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Yifeng Zhang,Meidong Lang
As the prevalence of bacterial infections on diverse material surfaces continues to rise globally, the demand for the development of surfaces with durable and effective antibacterial properties becomes more imperative. Herein, we developed a cationic polymer coating consisting of quaternized 4-vinylpyridine groups, 4-vinylpyridine groups, and butyl acrylate groups. Quaternized 4-vinylpyridine groups were utilized to confer antibacterial properties, while butyl acrylate groups were incorporated to enhance adherence to the substrate and flexibility of the material. The presence of the quaternary 4-vinylpyridine endowed the coating with excellent broad-spectrum antibacterial properties, with a maximum sterilization rate above 99%. The antibacterial properties assay revealed that the content of cationic group, the kind of substrates, as well as the length and type of alkyl chains significantly influenced the effectiveness and stability of antibacterial properties of cationic coatings. Cationic polymers can efficiently disrupt the integrality of the bacterial cell membrane, leading to the death of bacteria, which can be observed by scanning electron microscopy. In summary, the obtained cationic polymers that serve as effective, durable, and environmentally friendly antibacterial coatings without releasing harmful substances will have a much broader application potential in diverse application fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Bincheng Xu,Zexi Luo,Tao Tao,Ying Wang
Co-based nanomaterials have been proven as excellent catalysts in activating peroxymonosulfate (PMS), owing to the high adsorption ability and efficient electron transfer toward PMS molecules. However, the slow Co sites regeneration induced by HSO 5 − /SO 5 – redox cycle alone not only deteriorates the utilization efficiency of PMS, but also restricts the overall catalytic reaction rate. Herein, we report a novel S-FeCoO nano-catalyst to active PMS for chloramphenicol (CAP) degradation. As a result, up to 97.73 % of removal efficiency was achieved within 30 min even with an initial CAP concentration of 50 mg/L, which is substantially superior to other Co or Fe-based PMS activation systems. More importantly, synergistic effects arising from the coexisting Fe and S species were identified by the control experiments and characterization results. Co served as the primary active site, while Fe(II) and S 2− /S 2 2− greatly accelerated Co(III)/Co(II) redox cycle by donating electrons. The proposed strategy of dual acceleration of Co(III)/Co(II) redox cycle, as well as its mechanism insights, is expected to provide important implications on the rational design of advanced catalysts for PMS activation.
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Catalysts
·
2025
·Vol. 15
·期 4
·322
·
IF 4
Xianglong Meng,Ranran Song,Junjie Bian
In this study, natural clay-like silicate minerals were used as precursors to prepare highly acid-catalytic hydrophobic catalysts. A series of sulfonic acid-functionalized attapulgite catalysts, SO3H-APG, were fabricated by the ball-milling–oxidation method. The catalytic performance in the co-liquefaction and co-pyrolysis ofChlorellaand oil shale was investigated. The catalysts were analyzed using hydrophobicity evaluation, TEM, BET, FTIR, and other characterization methods. The SO3H-APG catalysts exhibited good hydrophobicity and dispensability. Sulfonation grafting improved their excellent hydrocarbon conversion activity. According to the GC–MS results, the addition of the SO3H-APG catalysts shifted the co-liquefaction products of microalgae and oil shale towards lower carbon numbers, with the majority of the products concentrated between C5 and C12, and a content of 84.9% in the range of C5–C11, while the content of products in the range of C12–C20 was only 15.1%. In the co-pyrolysis experiments, the addition of the catalysts promoted the thermal decomposition reaction. The synergistic effect between oil shale and microalgae facilitated the production of more hydrocarbon compounds with a higher H/C atomic ratio. The development of this type of catalyst provides an economically favorable approach for the co-conversion of algae and oil shale. The oil shale pyrolysis kinetic diagram shows that adding the APG clay-based catalyst significantly reduces the time for achieving the same conversion rate, especially below 300 °C, where the in situ catalytic effect is most pronounced.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shuilian Cheng,Zhan Cen,Chengyang Tang,Li Xu,Zuofang Yao,Xiaosong Zhou,Qingyou Liu,Shengsen Zhang
Sulfamethoxazole (SMX), as a typical and widely-used antibiotic, its residue in the water environment poses a serious threat to human health and ecological balance. Herein, an environmentally friendly and cost-effective melamine sponge (MS) was utilized as a carrier for the preparation of three-dimensional (3D) porous cobalt and nitrogen co-doped carbon catalysts (Co-N/C) via an impregnation-pyrolysis method. This approach successfully yielded an easily recoverable Co-N/C@MS catalyst. By utilizing this catalyst to activate peroxymonosulfate (PMS), efficient degradation and purification of wastewater containing SMX were achieved. The experimental results showed that the Co-N/C@MS/PMS system achieved 98.39 % degradation efficiency, attributed to the sponge substrate's high pore structure allowing uniform catalyst dispersion. After four cycles, the system remained stable, addressing traditional powder catalysts' recovery and loss issues. Mechanistic studies revealed that C O, pyrrolic N, and Co 2 + are the primary active sites in Co-N/C@MS for PMS activation. Both radical (primarily SO 4 ·- ) and non-radical (mainly 1 O 2 ) pathways contribute to SMX degradation, with the latter pathways playing a dominant role. The optimal design and performance evaluation conducted in this study offer a novel perspective on the application of recyclable flake catalyst materials for persulfate purification of organic wastewater.
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