MOLECULES
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2023
·Vol. 28
·期 15
·5930
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IF 4.6
Xuan Wang,Wei Liang,Changqing Lin,Tie Zhang,Jing Zhang,Nan Sheng,Zhaoning Song,Jie Jiang,Bing Sun,Wei Xu
Propane catalytic oxidation is an important industrial chemical process. However, poor activity is frequently observed for stable C–H bonds, especially for non-noble catalysts in low temperature. Herein, we reported a controlled synthesis of catalyst Co3O4@CeO2–IE via inverse loading and proposed a strategy of oxygen vacancy for its high catalytic oxidation activity, achieving better performance than traditional supported catalyst Co3O4/CeO2–IM, i.e., the T50(temperature at 50% propane conversion) of 217 °C vs. 235 °C and T90(temperature at 90% propane conversion) of 268 °C vs. 348 °C at the propane space velocity of 60,000 mL g−1h−1. Further investigations indicate that there are more enriched oxygen vacancies in Co3O4@CeO2–IE due to the unique preparation method. This work provides an element doping strategy to effectively boost the propane catalytic oxidation performance as well as a bright outlook for efficient environmental catalysts.Keywords:propane catalytic oxidation;inverse loading;oxygen vacancy
研究领域:
化学工程
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催化科学
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PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
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2026
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IF 4.8
Xiaoli Liu,Jianbei Zhang,Yan Cheng,Jiangning Shi,Jianjun Li,Yongjun Liu
Co 3 O 4 /CeO 2 catalyst with rich oxygen vacancies was fabricated. • Co 3 O 4 /CeO 2 catalyst achieves 100% NO x conversion within 225 −400 °C under oxygen-enriched conditions. • The heterostructure interface induces a strong Ce(4 f)–O(2p)–Co(3d) orbital coupling and triggers electron redistribution. • The heterostructure and oxygen vacancies ensured the pathway less affected by O 2 . The development of efficient and low-cost catalysts for the selective catalytic reduction of NO by CO (CO-SCR) under aerobic conditions remains a critical challenge. Heterostructure catalysts, particularly those engineered at the interface between rare earth and transition metal oxides, represent a promising frontier for the CO-SCR reaction. However, a deep understanding of their catalytic mechanism and active sites remains limited. In this work, the Co 3 O 4 /CeO 2 heterostructure catalyst with dispersed Co 3 O 4 nanoparticles on CeO 2 is designed and synthesized via a two-step precipitation method, serving as a model system. The optimized catalyst exhibits superior performance with 100% NO conversion across a wide temperature window (225–400 °C) and robust thermal stability, outperforming pure CeO 2 . Advanced spectral characterization and density functional theory calculations reveal that the heterostructure interface induces a strong Ce(4 f)-O(2p)-Co(3d) orbital coupling, which triggers electron redistribution. This unique interface environment optimizes the adsorption and activation of NO molecules and lowers the N-O bond cleavage energy, thereby enabling the high catalytic performance. This work offers a facile synthesis strategy for designing high-performance heterostructure catalysts and provides fundamental insight into the interface-driven mechanism for CO-SCR applications. Download: Download high-res image (215KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Ying Yang,Hua Li,Yilong Hou,Ce Wang,Kangyi Zhang,Zhihao Man,Jiangwei Shang,Xiuwen Cheng
Antibiotics that permeate aquatic environments present significant risks to both ecosystems and human health. In this study, we employed the techniques of room temperature aqueous solution precipitation to fabricate ZIF-67 derivatives, and established a Co 3 O 4 /CeO 2 /O 3 /PMS (Co-Ce/OP) system. Furthermore, a 10 mg/L Levofloxacin (LEF) solution could reach rapid degradation (97.2%) and effective mineralization (40.4%) under specific conditions. Subsequent investigations identified the primary active substances, intermediates, and reaction mechanism in the Co-Ce/OP system. Evidence from Electron Paramagnetic Resonance (EPR) and quenching experiments indicates that SO 4 · - , OH·, O 2 · - and 1 O 2 contribute to the degradation process. Applying High Performance Liquid Chromatography-Mass Spectrometry (HPLC-MS), we discovered that the principal degradation mechanisms for LEF encompass the cleavage and subsequent loss of the piperazine, quinolone, and morpholine rings, in addition to decarboxylation and defluorination reactions. Besides, we studied the acute toxicity, bioconcentration factor, developmental toxicity, and mutagenicity of LEF and its intermediate products. Our findings reveal a notable reduction in the toxicity of the intermediate products relative to LEF. Later experiment demonstrates that the degradation rate of LEF sustains above 90% after five cycles of reactions, indicative that the catalyst has excellent recyclability and stability. Furthermore, this study employed experiments across four different natural water matrices, demonstrating the system's considerable potential for effective application within authentic aquatic settings.
研究领域:
环境科学
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材料科学
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毒理学
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Guangtao Wang,Yue Hou,Sha Yu,Yuan Dang,Xiaoqin Sun
Herein, the bimetallic oxides Co 3 O 4 -CeO 2 with abundant oxygen vacancy (V O ) were successfully prepared and applied to activate peroxymonosulfate (PMS) for degradation of ceftiofur sodium (CEF). By optimizing the molar ratio of Co and Ce, nanosheet structures were obtained, which had large surface area and rich oxygen vacancies. The degradation efficiency of CEF can reach 94.3 % and the corresponding TOC removal is as high as 50.3 % after 40 min under the optimum conditions with 10 mA −1 cm −2 current density, pH 3, 5 mM PMS and 25 ℃. 1 O 2 is the main reactive species and its formation is related with V O in the process of degradation CEF. In details, the abundant V O on the catalyst surface can not only accelerate electron transfer to promote the conversion of PMS → ·SO 5 -· → 1 O 2 but also act as electron transport channels to facilitate Co 3+ /Co 2+ redox cycle. This study is of far-reaching significance for oxygen vacancy-activated PMS to promote the efficient degradation of refractory organic pollutants.
研究领域:
环境科学
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材料科学
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高影响因子
TALANTA
·
2023
·
IF 6.1
Chaonan Jiao,Ying Zhu,Tongkai Ji,Xingwei Cai,Jing Wang
For yolk-shell structured nanoreactors , multiple active components can be precisely positioned on core and/or shell that can afford more exposed accessible active sites, and the internal voids can guarantee sufficient contact of reactants and catalysts. In this work, a unique yolk–shell structured nanoreactor [email protected] 3 O 4 /CeO 2 @mSiO 2 was fabricated and applied as nanozyme for biosensing. The [email protected] 3 O 4 /CeO 2 @mSiO 2 exhibited superior peroxidase-like activity with a lower Michaelis constant ( K m ) and a higher affinity to H 2 O 2 . The enhanced peroxidase-like activity was attributed to the unique structure and the synergistic effects between the multiple active components. Colorimetric essays were developed based on [email protected] 3 O 4 /CeO 2 @mSiO 2 for the ultra-sensitive sensing of glucose in the range of 3.9 nM–1.03 mM with the limit of detection as low as 3.2 nM. In the detection of glucose-6-phosphate dehydrogenase (G6PD), the cooperation between G6PD and [email protected] 3 O 4 /CeO 2 @mSiO 2 triggered the redox cycling between NAD + and NADH, thereby achieving the amplification of the signal and enhancing the sensitivity of the assay. The assay showed superior performance as compared to other methods with linear response of 5.0 × 10 −3 –15 mU mL −1 and lower detection limit of 3.6 × 10 −3 mU mL −1 . The fabricated novel multi-enzyme catalytical cascade reaction system allowed rapid and sensitive biodetection, demonstrating its potential in biosensors and biomedical applications.
研究领域:
纳米技术
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生物化学
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分析化学
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生物医学工程
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Shuang Wei,Sheng Zhong,Chao Bao,Linbo Huang,Kexin Li,Ruirui Wang,Bin He,Ruirui Zhang,Ruixia Liu
The selective electrocatalytic oxidation of glycerol to high-value C2–C3 chemicals offers a promising approach to glycerol overproduction, while it struggles with precise C–C cleavage and limited selectivity from multiple pathways. Regulating the adsorption capacity of glycerol oxidation intermediates and the degree of C–C bond cleavage through the interfacial electronic structure of electrocatalysts is crucial for controlling C2–C3 selectivity. Herein, a self-supported p-n heterojunction catalyst (Co3O4/CeO2) is developed for the efficient electrocatalytic oxidation of glycerol to C2 chemicals, achieving a glycolic acid selectivity of 42%, with a yield of 19.6 μmol cm–2 h–1. The built-in electric field enables rapid interfacial charge transfer from CeO2 to Co3O4, which leads to the upshifted d-band center of active Co3O4. Electrochemical characterization and theoretical calculations demonstrate that the heterojunction promotes the adsorption of hydroxyl species and glycerol, thereby enhancing the activity of the glycerol oxidation reaction (GOR). Concurrently, the optimized electron cloud distribution of Co3O4 active sites strengthens the adsorption of oxygen-containing intermediates while weakening the adsorption of glycolic acid and suppresses the further cleavage of C–C bonds, thus increasing glycolic acid selectivity. This study clarifies the redox kinetic adsorption regulation mechanism of the Co3O4/CeO2 heterojunction catalyst and provides a highly promising electrocatalyst design strategy for the production of high-value-added C2 products via glycerol oxidation.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2025
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IF 11.3
Hao Liu,Siqing Cheng,Jianjun Chen,Xiaoping Chen,Shangchao Xiong,Fang Huang,Houfeng Liu,Junhua Li,Chuanzhi Sun
Mitigating industrial nitrous oxide (N2O) emissions is critical for climate action, yet developing efficient low-temperature N2O decomposition catalysts under O2-containing conditions remains challenging. The weak oxygen–support interaction leads to unsatisfactory N2O decomposition performance in the supported Co3O4/CeO2 catalyst. This study aims to enhance the electronic oxide–support interaction in the Co3O4/CeO2 catalyst through Zn doping, thereby improving its catalytic performance for N2O decomposition under O2-rich conditions. The results demonstrate that, in the presence of 5% O2, the activation energy of the catalyst sharply decreases from 117.5 to 60.4 kJ·mol–1 after Zn doping (Co2.4Zn0.6O4/CeO2). Additionally, the doped catalyst exhibits strong durability to the O2 + H2O + NOx impurity gas components. Advanced spectral characterization and density functional theory calculations reveal that Zn doping modulates the geometry and electronic structure of active cobalt sites, optimizing the adsorption and activation capabilities of N2O molecules. This study elucidates the mechanism of N2O decomposition over the catalysts and establishes a clear structure–activity relationship between the atomic-scale configuration of active sites and their performance. These findings provide critical insights for designing efficient supported oxide catalysts through targeted doping strategies and offer new perspectives for developing highly efficient and low-energy N2O decomposition catalysts.
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 23
·7161-7170
·
IF 6.177
Kaiyuan Hu,Jia Li,Yang Han,Dickon H. L. Ng,Ningning Xing,Yangsai Lyu
Micromotors have great potential in environmental monitoring and treatment. Herein, ZIF-67 derived Co3O4–CeO2 micromotors with a porous nanocage structure were synthesized by the ingenious combination of template scarification and calcination methods. Co3O4 inherited the typical porous structure of the ZIF-67 precursor and its skeleton offered a substrate for uniform in situ growth of CeO2 nanoparticles. The ZIF-67 derived Co3O4–CeO2 revealed a unique nanocage structure with a broken corner, resulting in the autonomous movement in the presence of H2O2. Based on the combination of peroxide-like activity, self-propelled motion and photo-Fenton like performance, a strategy to selectively and sensitively detect and quickly remove hydroquinone (HQ) from water was established. Taken together, this novel Co3O4–CeO2 nanocage-based micromotor could be effectively harnessed for water treatment.
研究领域:
环境科学
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材料科学
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分析化学
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2024
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IF 5.5
Yaqi Yang,Jiejun Li,Yilin Wang,Zhifang Liu,Yixi Xie,Pengcheng Zhao,Xiayi Hu,Junjie Fei
Multicomponent heterogeneous structures of yolk@shell nanospheres embedded in MOF-derived porous carbon are potentially excellent electrocatalytic materials. In this work, the multicomponent yolk@shell nanospheres (Au@Co 3 O 4 @CeO 2 ) were synthesized through an autocatalytic redox reaction. The synergistic and interfacial effects between Co 3 O 4 and CeO 2 can expose more active sites and enhance the catalytic activity. Then, the electrical conductivity of Au@Co 3 O 4 @CeO 2 was improved using N-doped carbon nanomaterials (NPC), which was derived from ZIF-8 by high-temperature pyrolysis. The synergistic catalytic effect between ZIF-8 derived NPC and Au@Co 3 O 4 @CeO 2 resulted in the highest electrochemical response current to caffeic acid in this composite. Under optimal conditions, the prepared modified electrode showed a LOD (limit of detection) of 5.7 × 10 −10 M for CA and a linear range of 1.0 × 10 −9 to 3.0 × 10 −6 M. Meanwhile, it showed remarkable selectivity for CA in the anti-interference experiments and can be applied to the detection in food samples (strawberry and red wine). This work has developed a novel sensing material for sensitive detection of CA, broadening the application of multi-component shell-core structured metal oxidation.
研究领域:
材料科学
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电化学
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食品科学
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纳米技术
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分析化学
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高影响因子
危险品化学品经营许可证（带存储）