JOURNAL OF CATALYSIS
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2024
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IF 6.5
Cheng Liu,Huiling Chen,Qi Chen,Jinhong Bi,Jimmy C. Yu,Ling Wu
A series of Al 3+ -doped UiO-66(Ce) MOFs (U(Ce x Al 1−x )) was developed to reveal the roles of metal doping on active site formation and substrate activation in photocatalytic selective transformation of amines to imines. Al 3+ doping induced crystal structure distortion to form coordinately unsaturated metal (Al, Ce) sites as Lewis acid sites to chemisorb and activate benzylamine (BA). In situ FTIR revealed that the Al site with stronger acid strength facilitated BA activation. The activation degree of N–H bonds in BA was evaluated by changes of calculated force constant. The intermediate products were confirmed through time-dependent in situ FTIR. The Al 3+ -doped sample U(Ce 0.90 Al 0.10 ), the optimal catalyst, showed a significantly increased BA conversion (97.6 %) than that (47.5 %) of undoped sample, which was attributed to enough active sites and the optimal charge mobility. Finally, the present study proposes a synergistic photocatalytic mechanism associated with molecular activation to demonstrate selective oxidation pathways at the molecular level.
研究领域:
材料科学
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化学工程
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催化化学
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产品关联
DOI
高影响因子
RARE METALS
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2024
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IF 9.6
Liu Cheng,Shi Ying-Zhang,Chen Qi,Ye Bing-Hua,Bi Jin-Hong,Yu Jimmy C.,Wu Ling
Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce 3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H–N···Ce and the C–S···Ce interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O 2 activation and reduction occur at coordinatively unsaturated Ce 3+ sites to form ·O 2 – . This is accelerated by the Ce 3+ /Ce 4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level. Graphical abstract
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
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2024
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IF 3.9
Jingwei Yuan,Wanyin Xu,Yirong Wang,Shao Wang,Ronghui Hao,Yubing Dong,Qianqian Li,Yufeng Zhao
Metal-organic frameworks (MOFs), characterized with highly ordered porous structures and relatively high surface area, exhibit significant application potential in the field of electrochemistry catalysis. In this study, we successfully prepared UiO-66(Ce) particles with uniform nanocube morphology and the size distribution ranging from 90 to 156 nm. Both morphology and size can be precisely tuned by directly adjusting detailed synthesis parameters, including solvent concentration and reaction time. Moreover, the crystal growth mechanism of UiO-66(Ce) was comprehensively investigated through the microstructure characterization. Such uniform particles demonstrated a desirable electrocatalytic performance with hydrogen evolution reaction (HER) overpotential of 118.6 mV (at 10 mA cm −2 ) in alkaline electrolyte (1 M KOH). This study not only introduces a novel approach for the morphological manipulation of UiO-66(Ce), but also presents new material candidates for the advancement of high-performance electrochemical energy conversion systems.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Surfaces and Interfaces
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2025
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IF 6.3
Fen Yang,Shuai Zhao,Biaobiao Ge,Jie Huang,Qianmin Dong,Qiang Chen,Shangzhong Jin,Pei Liang
We demonstrate a method for the detection of Ziram in water by using the adsorption properties of UiO-66(Ce) metal-organic framework (MOF) combined with the surface-enhanced Raman scattering (SERS) substrate of precious metal nanoparticles. The traditional UiO-66 is based on Zr as the metal center. After replacing the Zr metal center with Ce, the synthesized UiO-66(Ce) has short aging, high efficiency, low energy consumption, and energy saving. Furthermore, by adding P123, UiO-66 is modified to have a structure similar to the durian shell spine, which can provide more composite sites for metal nanoparticles. Thus, more SERS hot spots are generated. The combination of AuNPs with UiO-66(Ce) has been confirmed by XRD, XPS, and other characterization and analysis techniques. The Raman probe molecule R6G was used as an evaluation tool to evaluate the performance of this SERS substrate. The results showed that the relative standard deviation (RSD) of the substrate was as low as 8.96 % at a concentration of 10 –6 M of the R6G solution, and the substrate demonstrated high stability. Finally, the substrate was applied for the detection of ziram in lake water, achieving a detection concentration of 10 –8 M, an enhancement factor of 2.57 × 10 5 , and a detection limit as low as 5.21 × 10 –9 M, demonstrating excellent sensitivity and enabling efficient trace pollutant detection in complex water environments.
研究领域:
环境科学
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分析化学
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产品关联
DOI
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Rongrong Yu,Jingjing Wang,Xinyu Zhi,Danyi Yang,Yongqi Zhao,Guifeng Chen,Chengchun Tang,Yi Fang
With growing concerns about antibiotic contamination in water environments, developing efficient photocatalysts for tetracycline (TC) degradation has become imperative. In this study, a novel nanoflower-like BiOI/UiO-66(Ce/Fe) S-scheme heterojunction photocatalyst was developed for efficient TC degradation under visible light. Experimental evaluations revealed that the optimized 0.05-Bi/U(Ce/Fe) sample achieved 99.5 % TC degradation efficiency, maintaining 88.8 % of its initial activity after four consecutive cycles. The superior photocatalytic activity arises from three synergistic mechanisms: Fe 3+ doping modulates the band structure to broaden visible-light absorption, while the synergistic effect of Ce 4+ /Ce 3+ and Fe 3+ /Fe 2+ redox pairs optimizes charge transport. The internal electric field at the BiOI/UiO-66(Ce/Fe) heterojunction enhances charge separation while maximizing the redox capacity of the photocatalyst. Radical capture experiments and LC-MS analysis confirmed ·O 2 − and ·OH as the dominant reactive radicals, with proposed possible degradation pathways. Thus, a new synergistic strategy for designing efficient photocatalysts is proposed in this work.
研究领域:
环境催化
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材料化学
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光化学
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水污染治理
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纳米材料
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环境功能材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Xun Liu,Yufei Shu,Mengxia Wang,Weiwen Chen,Aling Wan,Zhongying Wang
Efficient and selective removal of fluoride from water remains a critical challenge in environmental remediation. In this work, we report a thermally modulated strategy to enhance the electrosorption performance of cerium-based metal–organic frameworks (UiO-66(Ce)) for fluoride removal. Rather than complete carbonization, controlled partial carbonization at 400 °C was found to be optimal, inducing the in situ formation of well-dispersed CeO2 nanoparticles and the development of interconnected mesoporous channels. The evolution of the pore structure with different thermal treatment temperatures was comprehensively characterized by N2 adsorption–desorption analysis and high-resolution transmission electron microscopy (HRTEM). This approach effectively balances electrical conductivity and active site availability, leveraging a nanoconfinement effect that restricts CeO2 aggregation, preserves active sites, and facilitates efficient ion transport. The optimized UiO-66(Ce)-400 °C material exhibits a high electrosorption capacity of 73.7 mg·g–1, rapid kinetics, and strong fluoride selectivity in the presence of competing anions. Finite element simulations and electrochemical analyses confirm that the synergy between enhanced mesoporosity, conductivity, and active site accessibility drives superior performance. Furthermore, the electrode demonstrates excellent regeneration and stability over five cycles. This study presents a versatile and scalable approach for engineering MOF-derived materials, offering valuable insights into the design of next-generation electrosorption systems for water treatment.
研究领域:
环境修复
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材料科学
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电化学
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纳米技术
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水处理技术
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Rushuo Li,Tao Ban,Danfeng Zhao,Fajie Hu,Jing Lin,Xiubing Huang,Zhiping Tao,Ge Wang
Defect engineering improves the catalytic performance of metal-organic frameworks (MOFs) loaded metal nanoparticles (MNPs@MOFs), but there is still a challenge in defining the structure-activity relationships. Herein, the content of linker-missing defects in UiO-66(Ce) was systematically regulated via formic acid as the modulators, and defective UiO-66(Ce) loaded Ni nanoparticles (NPs) were constructed for dicyclopentadiene (DCPD) hydrogenation. The fine regulation of defect engineering and reduction conditions affected the structure properties of UiO-66(Ce) and the electronic metal-support interaction between MOFs and Ni NPs, thereby optimizing the microenvironment and electronic state of Ni NPs. The optimized U(Ce)-40eq with suitable defects, small size and structure stability effectively promoted the production of highly dispersed abundant electron-deficient Ni 0 active sites, enhancing the adsorption and activation of H 2 and C=C bonds, especially accelerating the rate-determining step. Therefore, U(Ce)-40eq loaded 5 wt% Ni NPs achieved DCPD saturated hydrogenation to tetrahydrodicyclopentadiene (70 °C, 2 MPa, 90 min), superior to most high-loading Ni-based catalysts. This work reveals the synergistic mechanism of MOFs defect engineering and electronic structure of Ni NPs, providing effective guidance for the precise preparation of highly efficient and stable MNPs@MOFs heterogeneous catalysts.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Rushuo Li,Linmeng Wang,Peiyun Zhou,Jing Lin,Zhiyuan Liu,Juan Chen,Danfeng Zhao,Xiubing Huang,Zhiping Tao,Ge Wang
Developing catalysts for dicyclopentadiene (DCPD) hydrogenation to tetrahydrodicyclopentadiene (THDCPD) at low temperature is crucial and challenging for the green and energy-saving production of high energy density aviation fuel. Herein, hierarchically porous UiO-66(Ce) encapsulate Ru nanoclusters (NCs) was successfully customized by soft template method and in-situ reduction. The mesoporous UiO-66(Ce) promoted the high dispersion of Ru NCs, and the transfer of substrate molecules. By controlling the synthesis conditions, the electronic state, abundance, and microenvironment of Ru NCs were precisely regulated. Theory calculation and experimental results revealed that metallic Ru as the main active sites greatly promoted the adsorption and activation of substrate molecules. Therefore, mesoporous UiO-66(Ce) encapsulated Ru NCs showed remarkable catalytic DCPD hydrogenation performance with DCPD conversion of 100% and THDCPD selectivity of ~100% (60 °C, only 35 min). This study has brought new inspiration and guidance to the rational design of function materials for various catalytic applications.
研究领域:
催化材料
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能源化学
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纳米科技
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Yanqing Ran,Rui Dai,Xiaoshuo Zhang,Faqiong Zhao,Baizhao Zeng
Epithelial cell adhesion molecule (EpCAM) is a transmembrane glycoprotein and its detection is important for diagnosis and therapeutic prognostic assessment of many cancers. Herein, a highly sensitive electrochemiluminescence (ECL) sensor was developed for its detection. In the ECL sensor, dimercaptosuccinic acid-capped core/shell structured CdTe/CdS quantum dot (QD) was loaded on metal-organic framework material UiO-66(Ce) as electrochemical luminophore; Ti 3 C 2 /Ag composite was introduced for immobilizing EpCAM aptamer. Due to the well immobilization of QD and catalysis of UiO-66(Ce), the obtained luminophore CdTe/CdS QDs@UiO-66(Ce) displayed a strong and stable ECL signal. Furthermore, the Ti 3 C 2 /Ag could act as a co-reactant accelerator to boost the ECL signal. Thus, the resulted sensor had quite strong initial ECL signal for signal-off detection. Further experiment showed that it exhibited good linear response to EpCAM over the concentration range of 1 pg mL −1 − 10 ng mL −1 in pH 7.4 Tris buffer, with a detection limit low to 0.66 pg mL −1 . Additionally, the ECL sensor also presented high selectivity and satisfying reproducibility; its practicability was demonstrated by the successful determination of EpCAM in serum samples.
研究领域:
分析化学
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生物化学
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癌症研究
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2024
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IF 9.5
Li Rushuo,Ban Tao,Zhao Danfeng,Lin Jing,Liu Zhiyuan,Wang Linmeng,Huang Xiubing,Tao Zhiping,Wang Ge
Olefin hydrogenation under mild condition is crucial and challenging for industrial applications. Herein, defective UiO-66(Ce) was constructed by using cyanuric acid as the molecular etching “scissors” and further to synthesize heterogeneous catalyst with highly dispersed RuNi nanoparticles (Ru 1 Ni 1.5 @UiO-66(Ce)-12 h). The construction of Ce-O-Ru/Ni heterogeneous interfaces and Ni–Ru bonds provide electron transfer channels from Ce-oxo clusters and Ni species to Ru species. Furthermore, the microenvironment and electronic structure of Ru 0 active sites were synergistically regulated by adjusting the content of metal-organic frameworks (MOFs) defects and Ni promoter, thereby enhancing the adsorption and activation ability of H–H and C=C bonds. Therefore, Ru 1 Ni 1.5 @UiO-66(Ce)-12 h achieved dicyclopentadiene saturated hydrogenation (100% conversion) to tetrahydrodicyclopentadiene (∼ 100% selectivity) under mild condition (35 °C, 1 MPa) with only 25 min. Meanwhile, the sample exhibited excellent structural stability after 6 cycles test. This study provides a promising strategy for the rational design of remarkable noble metal-based catalysts for practical applications.
研究领域:
催化
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化学工程
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材料科学
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纳米技术
✓ 已验证
DOI
高影响因子
Molecular Catalysis
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2022
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IF 5.089
Zhengjie Li,Chen Ma,Miao Qi,Yunlong Li,Yanchao Qu,Ying Zhang,Lilong Zhou,Jimmy Yun
Nano CeO 2 (CeMOF) maintaining the primary micromorphology and pore structure of MOFs was successfully synthesized by controlled pyrolysis of UiO-66(Ce) in air. CeMOFs showed excellent activity for catalytic combustion of VOCs, including toluene, benzene and xylene. The results showed that the T 10% , T 50% and T 90% of toluene over CeMOF were 185, 198 and 206 ℃ (GHSV = 22500 h −1 , toluene concentration = 1000 ppm), respectively, which are the lowest among ever reported ceria catalysts. According to various characterization results, the high catalytic activity of CeMOF can be ascribed to its neat pore structure and high percentage of Ce with low chemical valence. The latter leads to massive surface oxygen species and oxygen vacancies which provides abundant oxidative sites for VOCs. The low-temperature reducibility and multiple weakly acidic sites also enhanced the catalytic activity. In addition, CeMOF shows good ability to resist H 2 O and thermal stability. The in-situ DRIFTs study of CeMOF shows toluene is degraded by continuous stages through quick conversion of toluene to benzaldehyde and adsorbed benzoate, and forms CO 2 and H 2 O at last.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Haiping Zhao,Ziyi Zhang,Yong Han,Weixia Yang,Wenzhi Tang,Tianli Yue,Zhonghong Li
A nanocomposite (UiO-66/Ce-MnO 2 ) was fabricated by combining UiO-66 with cerium-doped manganese dioxide (Ce-MnO 2 ) for colorimetric detecting vitamin C (Vc). Compared with traditional artificial enzymes, the as-synthesized UiO-66/Ce-MnO 2 were simple to prepare and did not require the participation of other active substances. The doping of cerium increased the oxygen vacancies and the UiO-66 as a carrier improved the dispersibility. The formation of superoxide anion (O 2 − ) and the inside Ce 4+ /Ce 3+ and Mn 4+ /Mn 3+ redox couples of UiO-66/Ce-MnO 2 endowed UiO-66/Ce-MnO 2 with a high catalytic capability, which could catalytically oxidize 3, 3′, 5, 5′-tetramethylbenzidine (TMB) into oxidation state TMB (oxTMB) without H 2 O 2 , accompanying with color change and a prominent peak at 652 nm in UV–vis spectra. Based on the inhibitory effects of Vc on catalytic oxidation of TMB, detection of Vc can be achieved, exhibiting a linear relationship in the concentration of 1.13–17.01 μmol L −1 with a low detection limit of 65.82 nmol L −1 . This system can also be detected by smartphone, the linear detection range is 12.47–22.67 μmol L −1 . Vc contents in fruits and vegetables detected by the sensor were in good agreement with the 2, 4-Dinitrophenylhydrazine colorimetry method ( P > 0.05), indicating a reliable sensor for Vc detection.
研究领域:
生物化学
·
食品科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）