JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Yalin Yu,Zhihao Dong,Ling Tan,Nannan He,Rong Tang,Fang Jiang,Huan Chen
Diminishing the size of metal nanostructures can significantly improve the performance of catalysts. However, the self-aggregation of small particles is still an insurmountable obstacle, resulting in the unfavorable stability and recyclability. Herein, we designed and fabricated the Pd-CeO 2-x -NC catalyst though an accurate deposition strategy to downsize the Pd particle to sub-nanometer level and enhance its running stability. The CeO 2-x nanoclusters were firstly dispersed on the nitrogen-doped carbon nanosheets. Further, the active Pd sub-nanoclusters were accurately scattered on the surface of CeO 2-x ascribing to the strong metal-support interaction (SMSI) between Pd and CeO 2-x , which was beneficial to promote the catalytic activity. Subsequently, the high oxidation state Pd n + species were formed due to the electron transfer from Pd to CeO 2-x caused by the SMSI effect. Strikingly, the HER performance of Pd-CeO 2-x -NC was surprisingly correlated with the ratio of Pd n + , suggesting Pd n + acted as the dominant active species. Besides, the SMSI effect stabilized the valence state of active Pd n + species and prevented the sub-nanometer Pd clusters from aggregation, which played a vital role for the enhanced stability of the hybrid catalyst. This synthetic process described here is contributed to prepare various nanostructured catalysts with satisfactory stability through the direct targeting strategy.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2026
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IF 7.8
Zhiqian Lin,Huaiqing An,Liyuan Qian,Yun Wang,Haibin Lin,Xiaofei Wang,Guojun Zou,Jinlong Zhu,Songbai Han
Propane dehydrogenation (PDH) is a key process for propylene production, but conventional catalysts are often constrained by high cost, environmental impact, and limited stability under harsh reaction conditions. Fe-based catalysts offer a cost-effective and sustainable alternative due to their intrinsic ability to activate C–H bonds in alkanes. However, precise control over the oxidation state and coordination environment of Fe species to balance PDH activity and stability remains challenging. Herein, we develop a molten-salt-assisted synthesis strategy integrated with CeO2–x-mediated interfacial engineering to finely tune the structural and electronic properties of Fe species supported on Al2O3. The molten salt medium enables uniform dispersion and controlled crystallization of Fe3O4, effectively mitigating its over-reduction during high-temperature H2 treatment. The subsequent incorporation of CeO2–x modulates the local electronic structure of Fe3O4, inducing a controlled partial reduction to metallic Fe0 and forming a well-defined Fe0–Fe3O4 dual-interface architecture. This interfacial electronic reconstruction enriches the electron density of low-valent Fe sites, facilitating efficient charge transfer during propane activation and promoting rapid propylene desorption. As a result, the optimized catalyst demonstrates accelerated PDH kinetics, high propylene selectivity, and enhanced resistance to coking. This work establishes a scalable route for constructing dual-interface active sites, providing a general design principle for low-cost, high-performance PDH catalysts.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Dan Guo,Yao Lu,Yongzhe Ruan,Yifan Zhao,Yujun Zhao,Shengping Wang,Xinbin Ma
Dry reforming of methane is a promising process to convert two greenhouse gases into syngas. Calcinated nickel silicate nanotubes (C-NSNT) as well as CeO 2-x interface-confined and nickel silicate nanotubes (NSNT)-derived Ni catalysts, which are marked as λCeO 2-x -NSNT (λ = 0.5, 1, 1.5 and 2.25), is prepared and evaluated in dry reforming of methane. Compared with C-NSNT, the λCeO 2-x -NSNT samples exhibit improved catalytic performance in dry reforming of methane, which is closely related to Ni-CeSiO 2-x interface along with extrinsic defects from the interfacial reaction between CeO 2 and NSNT during the reduction process. Extrinsic defects can generate oxygen vacancies that can be accompanied by Ce 3+ species. The enhancement of catalytic activity is ascribed to confined effects of extrinsic defects at contact interface of Ni-CeSiO 2-x and electronic effects of CeO 2-x . Furthermore, Ni-CeSiO 2-x interface with rich extrinsic defects can promote the adsorption and activation of CO 2 as electron donor on reduced λCeO 2-x -NSNT catalysts, which is fast dissociated into CO* and O*. Meanwhile, oxygen vacancies can transfer adsorbed O* species to Ni active sites to promote the carbon gasification reaction, which is responsible for the enhancement of catalytic stability in methane dry reforming for λCeO 2-x -NSNT catalysts. 1.5CeO 2-x -NSNT sample with more extrinsic defects has particular higher catalytic stability due to the improvement of anti-coking.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Guoqiang Zhang,Xiya Zhao,Xiushuai Guan,Xiaokun Wang,Xiaoyang Wang,Xiaochao Zhang
The light-driven conversion of CO 2 to dimethyl carbonate (DMC) represents a promising green and sustainable pathway for achieving dual-carbon goals. However, the inherent difficulty in activating CO 2 molecules results in low DMC yields when synthesizing DMC from CO 2 and methanol (CH 3 OH) under light-driven conditions. In this study, the activation of CO 2 and CH 3 OH is enhanced by modulating the number of hydroxyl groups and the concentration of oxygen vacancies on the surface of spindle-like CeO 2-x through the introduction of cetyltrimethylammonium bromide (CTAB). Photothermal catalytic experiments show that the optimal CTAB-modified CeO 2-x achieves excellent DMC yield of 5.26 mmol·g −1 under mild conditions (0.1 MPa, 120℃). The X-ray photoelectron spectroscopy and CO 2 temperature-programmed desorption results demonstrate that CTAB modification increases the number of hydroxyl groups and oxygen vacancies on the CeO 2-x surface, which improves the effective activation of CO 2 to form the reactive intermediates such as *HCO 3 – and *CO 2 . Notably, the increased hydroxyl groups promote the dissociation of CH 3 OH into *CH 3 O. Meanwhile, isotopic labeling and in situ infrared characterization confirm the light-driven reaction pathway of CO 2 and CH 3 OH, involving the oxidation of CH 3 OH to *CH 2 OH via photogenerated holes, followed by rapid coupling with *CO 2 to generate the reactive intermediate (CH 3 OCOO*). These findings provide new insights into the rational design and construction of CeO 2 -based catalysts to achieve high yields of DMC under mild conditions.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Pengxin Song,Renlu Han,Yun Gao,Zhen Guo,Xiangjun Wei,Na Li,Jiancheng Yu,Keqi Tang
Energy is the basis of survival for all organisms, and proliferative tumuor cells rely primarily on glycolysis to obtain energy to meet high bioenergetic demands. Glycolysis inhibition has emerged as a key target for cancer therapeutic applications. However, the therapeutic efficiency of glycolysis suppression is restrained by the mutual compensation of multiple energy-generating pathways and biological barriers in the complex tumuor microenvironment (TME). In this study, we developed polydopamine (PDA)-coated porous CeO 2-x nanorods with metformin (MET) and glucose oxidase (GOx) co-loading and bovine serum albumin (BSA) encapsulation (denoted as CPGMB) for dual-pathway glycolysis inhibition-boosted bioenergetic therapy with photothermal/chemodynamic therapy (PTT/CDT). MET and GOx are released due to the weakly acidic TME and the photothermal effect to suppress glycolysis via hexokinase 2 (HK2) inhibition and glucose deprivation pathways, respectively. Interestingly, H 2 O 2 produced by GOx-catalysed glucose oxidation was converted into O 2 by Ce 4+ , resulting in closed-loop glucose depletion, further potentiating glycolysis restraint via hypoxia relief. Meanwhile, H 2 O 2 could also be transformed into •OH by Ce 3+ for CDT. Furthermore, the photothermal effect of CPGMB ablated the cancer cells and amplified •OH production. In vitro and in vivo experiments confirmed the anti-tumour efficacy and biosafety of CPGMB. This study presents a novel strategy for a synergistic bioenergetic antitumour therapy.
研究领域:
癌症治疗
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纳米医学
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生物化学
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诊疗学
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DOI
高影响因子
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