Biofabrication
·
2025
·Vol. 17
·期 3
·035012
·
IF 8
Mengyuan Li,Jiaming Ge,Jingwen Yao,Yuanhao Zhang,Lin Ma,Zheng Li,Xiangli Han,Ming Liu,Fei Tian,Jing Zhao
Oral squamous cell carcinoma (OSCC) is the most common malignant tumor in the head and neck. Due to low bioavailability and passive targetability of anticancer drugs show great limitations in cancer therapy, the treatment of OSCC faces major challenges. Folic acid (FA) targeting can deliver anticancer drugs efficiently into the tumor environment, further enhance the anti-cancer efficacy. Herein, the nanoplatform based on UiO-66 that encapsulated with an effective FA targeting ligands and the pH-responsive polyethylene glycol (PEG) layer for the targeted delivery of berberine (Ber) is constructed for fighting against OSCC. The FA modification and controlled pH-responsiveness enable the targeted delivery of UiO-66/PEG-FA, which promotes the release of Ber and increases the cumulative intracellular Ber concentration, which both promote consumption of glutathione (GSH) and induced generation of reactive oxygen species (ROS), further stimulate the secretion of inflammatory factors (TNF-α and IL-1β). A comprehensive evaluation of in vitro and in vivo experiments show that UiO-66@Ber/PEG-FA promote autophagy and apoptosis of tumor cells by regulating the expression of Beclin-1, ATG13, BAX and Bcl-2, and effectively inhibit tumor growth. Overall, UiO-66@Ber/PEG-FA exhibit superior pH-responsiveness and targeted therapeutic efficiencies in vitro and vivo, it can serve as an approach for OSCC therapy.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ying Gao,Qinqin Chen,Xinhao Shen,Shuang Yao,Zhiwen Jiang,Sanjian Ma,Hailiang Yang,Juanhong Li,Zixia Lin,Xin Liu
Both the sluggish kinetics of Fe(II) regeneration and usage restriction of H2O2 have severely hindered the scientific progress of the Fenton reaction toward practical applications. Herein, a reduction strategy of activated hydrogen, which was used to simultaneously generate H2O2 and accelerate the regeneration of ferrous in a Fenton-like reaction based on the reduction of activated hydrogen derived from H2, was proposed. Two types of composite catalysts, namely, Pd/UiO-66(Zr)-2OH and Pd@UiO-66(Zr)-2OH, were successfully prepared by loading nano-Pd particles onto the outer and inner pores of UiO-66(Zr)-2OH in different loading modes, respectively. They were used to enhance the reduction of activated hydrogen. The characterization results based on the analysis of scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy revealed that the materials were successfully prepared. By using a trace amount of ferrous iron and without adding H2O2, trimethoprim (C0 = 20 mg·L–1), as a target pollutant, could be nearly 100% degraded within 180 min in the reaction system composed of these two materials. The cycle of iron and the self-generation of H2O2 were verified by the detection of ferrous H2O2 in the system. Density functional theory calculation results further confirmed that the pore-filled Pd0 NPs, as the main catalytic site for Pd@UiO-66(Zr)-2OH, could produce H2O2 under the combined action of hydrogen and oxygen. The Pd@UiO-66(Zr)-2OH system had excellent stability after multiple applications (at least 6 cycles), all of which resulted in 100% removal of trimethoprim. The degradation efficiency of the Pd/UiO-66(Zr)-2OH system for TMP gradually decreased from 97 to 80% after six cycles. The results of electron paramagnetic resonance combined with classical radical burst experiments revealed the degradation pathways in the reaction system with hydroxyl radicals and singlet oxygen as the main reactive oxygen particles.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Ying Gao,Ruibin Yang,Qinqin Chen,Xinhao Shen,Dapeng Li,Juanhong Li,Feng Liu,Jianhua Wu,Sanjian Ma,Guoliang Dai,Dongmei Wang,Lei Xie,Zixia Lin,Xin Liu
The large-scale production of iron sludge and the safety issues of H2O2 usage are two limitations in the promotion and application of the Fenton reaction. To further solve the problems, an active hydrogen reduction strategy was proposed. Herein, the reducing property of active hydrogen was utilized to simultaneously generate H2O2 in situ and accelerate the regeneration of ferric in the reaction process. The composite metal–organic frameworks (MOFs) Pd@UiO-66(Zr) and Pd@UiO-66(Zr)-2OH, which were stable under acidic conditions, were synthesized for hydrogen activation. Under the condition of only trace amounts of ferrous and hydrogen added, both catalysts showed excellent performance in the degradation experiments of trimethoprim. The kobs of the Pd@UiO(Zr)-66-mediated system is 0.0487 min–1, which is 1.67 times that of Pd@UiO-66(Zr)-2OH. In the pollutant degradation reaction system constructed by these two materials, both of the hydroxyl radicals and singlet oxygen play a dominant role. The Bader charge analysis showed that the charge transfer from Pd to the MOF host was higher on Pd@UiO-66(Zr) than Pd@UiO-66(Zr)-2OH, which could be a key factor in distinguishing the catalytic activity of the catalysts. In addition, both catalysts showed excellent stability over six cycles. Nearly 100% degradation of trimethoprim could be achieved. This study provides some reference for the control of emerging pollutants by UiO-66(Zr) series materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.7
Haileyesus Hatano Haitosa,Osman Ahmed Zelekew,Pu Chen,Daniel Manaye Kabtamu,Weimao Yan,Hong Wang,Yi-nan Wu
Fluoroquinolone antibiotics like ciprofloxacin (CIP) pose environmental risks when released into water. Herein, a visible-light-active Fe-doped NH 2 -UiO-66(Zr)@AgI Z -scheme heterostructure was prepared via an ion exchange precipitation method. By varying AgI content, reduced particle size and enhanced charge separation for efficient photodegradation was achieved. The optimum composition (Fe-UNH@AgI-20) exhibited a 95.2 % degradation efficiency toward CIP after 60 min of visible-light irradiation. It also showed high removal efficiencies for tetracycline, lomefloxacin, and Rhodamine B. Reaction kinetics followed pseudo-first-order behavior, with rate constants significantly higher than those of pristine NH 2 -UiO-66(Zr) and AgI. The catalyst maintained 85.1 % activity after cycles, indicating good stability. Scavenger tests and electron paramagnetic resonance (EPR) analyses identified holes (h + ), superoxide radical (•O 2 − ), and hydroxyl radical (•OH) as key reactive species. Fe doping enhanced visible-light absorption and created defect sites, while AgI introduction promoted charge separation and suppressed AgI photocorrosion. Under irradiation, a small fraction of Ag + was reduced to metallic Ag, forming an electron bridge that switched the initial type-II heterojunction to a Z -scheme configuration. This Z-scheme mechanism efficiently separated carriers, facilitated generation of ROS, and enabled thorough mineralization of CIP; toxicity predictions showed most products were less mutagenic than CIP, confirming reduced ecological risk. The findings demonstrate that the Fe-doped NH 2 -UiO-66(Zr)@AgI heterostructure is a promising photocatalyst for antibiotic-contaminated wastewater remediation.
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高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2013
·Vol. 19
·期 42
·14279-14285
·
IF 5.831
Dengrong Sun,Yanghe Fu,Wenjun Liu,Lin Ye,Dengke Wang,Lin Yang,Xianzhi Fu,Zhaohui Li
Graphical Higher CO 2 photoreduction activity than previously studied metal–organic framework (MOF) NH 2 -MIL-125(Ti) in the presence of triethanolamine (TEOA) as the sacrificial agent under visible light is exhibited by the amino-functionalized MOF NH 2 -Uio-66(Zr). The photoinduced electron transfer from 2-aminoterephthalate linkers to Zr oxo clusters was revealed for the first time by photoluminescence studies, and the generated Zr III was detected by ESR analysis (see figure). Metal–organic framework (MOF) NH 2 -Uio-66(Zr) exhibits photocatalytic activity for CO 2 reduction in the presence of triethanolamine as sacrificial agent under visible-light irradiation. Photoinduced electron transfer from the excited 2-aminoterephthalate (ATA) to Zr oxo clusters in NH 2 -Uio-66(Zr) was for the first time revealed by photoluminescence studies. Generation of Zr III and its involvement in photocatalytic CO 2 reduction was confirmed by ESR analysis. Moreover, NH 2 -Uio-66(Zr) with mixed ATA and 2,5-diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO 2 reduction due to its enhanced light adsorption and increased adsorption of CO 2 . This study provides a better understanding of photocatalytic CO 2 reduction over MOF-based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO 2 reduction.
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Reaction Kinetics Mechanisms and Catalysis
·
2026
·
IF 2.1
Wang Jiahao,Liu Feng,Xie Lei,Yang Hailiang,Ma Sanjian,Lin Zixia,Liu Xin,Wang Suqin
Refractory wastewater treatment via Fenton reactions is hindered by iron sludge. Herein, fluorinated UiO-66(Zr)-F4 was employed as a hydrogen-storage carrier to confine Pd⁰ catalytic centers, and an [H]-mediated (H 2 -precursored) Fenton-like system was constructed for carbamazepine degradation under ambient conditions. With 25 μM Fe 2 + and 60 mL min⁻ 1 H 2 flow, 53% carbamazepine removal was achieved in 1 h via ⋅OH/ 1 O 2 oxidation, and > 59% efficiency was retained over six 3-h cycles. However, [H]-driven hydrogen spillover reduced C-F bonds, causing a 92.3% drop in specific surface area that compromised long-term stability. It was concluded that fluorination is suboptimal; modulating the carrier’s hydrophobicity via electron-donating groups (instead of fluorination) is critical for stable Zr-MOF-based catalysts in [H]-assisted advanced oxidation, offering alternative perspectives for process optimization. Graphical abstract
The alternative text for this image may have been generated using AI.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2026
·Vol. 40
·期 4
·e70546
·
IF 4.3
Hangyu Zhang,Shuang Yao,Zhiwen Jiang,Lei Xie,Zixia Lin,Guoliang Dai,Juanhong Li,Xin Liu,Feng Liu
In Fenton-like reactions, the catalysts generally have an inherent drawback: Their active centers are prone to being lost from the catalyst supports, leading to a continuous decline in catalytic efficiency and causing secondary pollution. To address this issue, two catalysts, including Fe 3 O 4 @UiO-66(Zr) and Fe 3 O 4 @UiO-66(Zr)-COOH, were prepared in this study by confining Fe 3 O 4 active centers within the pores of UiO-66(Zr) and grafting -COOH groups to enhance metal coordination interactions. The Fe 3 O 4 @UiO-66(Zr)-COOH achieved 99% removal efficiency of carbamazepine within 5 min under the conditions of pH = 3.0, 40 mM H 2 O 2 , 20 mg·L −1 carbamazepine, and 2 g·L −1 catalyst. This efficiency far exceeded that of Fe 3 O 4 @UiO-66(Zr) (61.5%) and was 3.96 times higher than that of the Fenton-like system. The rapid degradation of CBZ was realized through stabilized active centers and enhanced metal coordination. In this work, the iron-based material was found to enhance the coordination between Fe and Zr. As confirmed by quenching experiments, electron spin resonance, electrochemical tests, and density functional theory calculations, ·OH and 1 O 2 were identified as the dominant active species. The -COOH, acting as electron bridges, enhanced electrical conductivity and reduced electron transfer barriers, thereby facilitating faster charge transfer processes. In addition, it was demonstrated by six cycles of experiments that Fe 3 O 4 @UiO-66(Zr)-COOH possessed excellent stability. It was also shown by the characterization of the catalyst after the cycles that both the performance and morphology of the composite material could be maintained unchanged.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 41
·19432-19438
·
IF 3.591
Fangyuan He,Heyi Zhang,Xiaonan Li,Jie Yang,Wenqing Ma,Hong Zhang
In this study, for the first time, we selected a size-matched polyoxometalate α-Mo8O26, and successfully prepared Mo8-UiO-66(Zr) as a catalyst with double active sites for extractive and catalytic oxidative desulfurization systems (ECODS). UiO-66(Zr) can encapsulate Mo8O26 in the cage and avoid its leaching, while the sulfur compounds can also enter the cage to approach the sites. As a result, in the presence of H2O2 as an oxidant, the catalyst exhibited extraordinary oxidative desulfurization performance towards benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT). It only takes 10 min for the desulfurization efficiency to reach 100%. The catalyst can be reused for at least 4 times without significant loss in the desulfurization activity. Also, the possible reaction mechanisms of the catalytic oxidation process have also been proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Peng Hu,Xiaopeng Liang,Muhammad Yaseen,Xiaodan Sun,Zhangfa Tong,Zhongxing Zhao,Zhenxia Zhao
A novel mechano-chemical strategy using dopamine to modify UiO-66(Zr) by N-coordination was proposed to enhance its competitive adsorption for acetaldehyde, chlorobenzene/H 2 O, both thermodynamically and kinetically. The newly synthesized material was characterized by SEM, EDX, XPS, PXRD, FT-IR, TGA/DTG and BET techniques. Results showed that N was successfully grafted into UiO-66(Zr) frameworks through coordination interaction with Zr-O clusters resulting in M-UiO-66(Zr-N 3.0 ). The obtained M-UiO-66(Zr-N 3.0 ) exhibited a significant increase in adsorption of chlorobenzene (4.94 mmol/g) and acetaldehyde (9.42 mmol/g) compared to parent UiO-66(Zr) and UiO-66(Zr)-NH 2 . The H 2 O adsorption uptake of M-UiO-66(Zr-N 3.0 ) decreased by 20% that of UiO-66(Zr) and 47% of UiO-66(Zr)-NH 2 indicating higher hydrophobicity of the modified material. Kinetic performance indicated that diffusivity of chlorobenzene on M-UiO-66(Zr-N 3.0 ) was about 7.8 and 40 times higher than that of the parent UiO-66(Zr) and UiO-66(Zr)-NH 2 respectively and 15.4 times higher than that of H 2 O on itself. Based on the results, the current N-modification strategy can be deemed as an efficient way to improve MOFs competitive adsorption towards VOCs under humid conditions and it might play active role in industries involving adsorbent applications.
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MICROCHEMICAL JOURNAL
·
2018
·
IF 2.746
Guihua Gao,Yanyan Xing,Tingting Liu,Jian Wang,Xiaohong Hou
Four water stable metal-organic frameworks (MOFs), MIL-101(Cr), MIL-100(Fe), MIL-53(Al), and UiO-66(Zr), were used as adsorbents for concentration of four androgens and progestogens from water. The adsorption abilities of target analytes on the four MOFs were investigated by experimental and molecular simulation strategies, and UiO-66(Zr) was ultimately selected as the sorbent to develop a porous membrane protected micro-solid-phase extraction (μ-SPE) method for simultaneous extraction androgens and progestogens in environmental water samples followed by LC-MS/MS detection. Several variables affecting the extraction efficiency were systematically investigated, including pH, salt concentration, extraction time, kind of desorption solvent, and desorption time. Under the optimized conditions, excellent linearity was obtained in the range of 20.32–2032 ng/L for T, 10.24–1024 ng/L for P, 7.624–762.4 ng/L for TP , and 8.376–837.6 ng/L for MPA . Limits of detection (LODs) and limits of quantification (LOQs) were 10 ng/L and 20 ng/L for T, 4.0 ng/L and 10 ng/L for P, 2.0 ng/L and 7.0 ng/L for TP, and 3.0 ng/L and 8.0 ng/L for MPA, respectively. The recoveries were ranged from 80.5% to 102.4%. Furthermore, the μ-SPE device could be used for at least 10 extractions (RSD < 10.0%). Meanwhile, comparison was made with solid-phase extraction, and the developed method was demonstrated to be a convenient and eco-friendly pretreatment method for water samples.
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