CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Bo Zhao,Yao Yao,Kexin Huang,Jiaxin Li,Minjie Chen,Chao Liu,Hongjian Xu,Xinyu Zhao,Ganggang Chang
The selective hydrogenation of furfural (FFA) to furfuryl alcohol (FA) is regarded as attractive transformation to achieve the sustainable synthesis of value-added chemicals from biomass resources. However, the conventional supported catalysts are significantly restricted by their narrow pore size, ununiform dispersion and easy leaching or aggregation of catalytic sites. Herein, we designed hollow UiO-66-NH2 as the support to encapsulate Pd nanoparticles (Pd@H-UiO-66-NH2) to achieve the highly active and selective conversion of FFA to FA. Benefiting from the void-confinement effect and substrate enrichment of hollow structure, as well as the surface wrinkles, the as-prepared catalyst Pd@H-UiO-66-NH2 exhibited 96.8 % conversion of FFA with satisfactory selectivity reaching up to 92.4 % at 80 °C, 0.5 MPa H2 in isopropanol solvent within 6 h. More importantly, as-prepared Pd@H-UiO-66-NH2 catalyst exhibited excellent long-term stability, as well as good universality toward a series of hydrogenation of unsaturated hydrocarbons.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Chemistry
·
2024
·
IF 6.7
Deshuang Lu,Zhonghan Cheng,Nikom Klomkliang,Wanida Koo-amornpattana,Francis Verpoort,Somboon Chaemchuen
Organic linkers are typically controlled to create the micropore structure when synthesizing metal-organic frameworks (MOFs). However, developing a hierarchical pore structure is beneficial for improving the efficiency of MOFs in various applications. This study investigates a green strategy using a water modulator that competes with the terephthalic ligand to coordinate with zirconium clusters, thereby accessing open sites for hierarchical micro- and mesopores in UiO-66. Using a hydro-modulator induced the formation of a mesoporous structure and enhanced the hydrophilic properties of UiO-66-X due to the presence of hydroxyl groups. Also, model calculations using density functional theory (DFT) support the observed structural chemical geometry. The advantages of a hierarchical pore structure, increased hydrophilicity, and the presence of open sites in the robust structure of UiO-66-X led to a significant enhancement in both antibiotic adsorption and the catalytic activity of ring-opening epoxide reactions compared to the pristine microporous UiO-66. Therefore, utilizing water as a green modulator presents a simple and environmentally friendly approach to introducing hierarchical pore structures in MOFs. It offers a promising strategy for enhancing their performance across various applications.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Jiajun Yu,Xiao Wang,Guanhong Lu,Haijiao Xie,Xiaofeng Xie,Jing Sun
The purification of oxygenated volatile organic compounds VOCs (OVOCs), important precursors of ozone and particulate matters, has triggered intensive research interests. UiO-66 with high photocatalytic activity have shown great potential. However, the lack of active sites severely limited the trapping and degradation of OVOCs. Herein, reo-UiO-66 with increased specific surface area, hierarchical porous structure and tunable acidic/basic sites was synthesized by simply adding water as the modulator. XRD, TGA and FTIR results confirmed the formation of reo-defects, which significantly affected the surface hydrophilicity and active sites of UiO-66. The adsorption of Lewis acidic acetaldehyde was enhanced by 265 times with coordinative unsaturated Zr acting as the dominant adsorption sites. The degradation efficiency of typical OVOCs (acetaldehyde and acetone) increased from 0% and 25% to 50% and 73%, respectively. This work provided a facile method to modulate the micro-environment in MOFs for the efficient capture and catalytic purification of OVOCs.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yixin Kuang,Suxin Zhou,Cheng Mao,Xiaoying Feng,Juan Zheng,Gangfeng Ouyang
High-resolution separation of numerous isomers is highly desirable for their high-quality analysis, yet challenging, which puts forward high requirements on the precise design of stationary phase. Herein, flexible 4- tert -butylcalix[n]arenes (TBCx[n]s) with different cavities have been intelligently integrated with in-situ grown UiO-66 coatings, to investigate their separation efficiencies for alkane and substituted benzene isomers. The modifications of UiO-66 with TBCx[n]s have made up for the deficiency of UiO-66 on the separation of ethylbenzene and styrene. The effects of TBCx[n]s on the separation performance of UiO-66@TBCx[n]s have demonstrated distinct regularities, i.e., the effects of TBCx[6] are superior to those of TBCx[8], while the TBCx[4] is the least effective. The baseline separation of all analytes has been achieved by the UiO-66@TBCx[6] column with enhanced selectivity and improved separation resolution (Rs). For the six groups of isomers that are most difficult to separate, the corresponding selectivity and Rs are greater than 1.09 and 5.48, respectively, confirming the outstanding separation performance of the UiO-66@TBCx[6] column and the feasibility of integrating soft supramolecule and rigid MOF.
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Dandan Guo,Diya Zheng,Ding Zhou,Changlun Tong,Shaohua Huang
Lysine (Lys) is an essential nutrient that plays a crucial role in the growth and development of living organisms. Chiral analysis of Lys holds significant importance for ensuring the safety of food, pharmaceuticals, and health products. In this work, an achiral Zr-based metal organic frameworks (MOFs), UiO-66-NH 2 , was proposed as a fluorescent probe to achieve rapid response to l -lysine (L-Lys) in solution. Additionally, Zr 4+ in the skeleton of UiO-66-NH 2 framework exhibited different binding capacities towards Lys enantiomers, leading to distinct fluorescence responses for L-Lys and d -lysine (D-Lys). Leveraging these properties, the UiO-66-NH 2 probe enabled accurate determination of L-Lys concentrations in solution, as well as the enantiomeric excess (ee) values of Lys solutions. Notably, in the detection of Lys enantiomers, the achiral UiO-66-NH 2 acted as both a chiral selector and a fluorescent indicator, greatly improving the efficiency and stability of the detection system. The probable mechanism was further elucidated by pH titration experiments and density functional theory calculations. Additionally, the general applicability of this mechanism was validated by similar amino MOFs. The application of the UiO-66-NH 2 fluorescent probe in analysis of infant formula milk powders and liquid milk samples confirmed the reliability of the method. Moreover, the construction of fluorescence test paper by immobilizing UiO-66-NH 2 onto filler papers enabled the rapid identification of Lys enantiomers. Compared to previous fluorescent analyses of chiral amino acids assisted by additional metal ions, this study presented a novel approach and methodology that offers high efficiency, stability, reproducibility and reusability for the identification and detection of Lys enantiomers, highlighting the potential of the UiO-66-NH 2 fluorescent probe in advancing analytical techniques.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Zhihua Wang,Mingda Han,Yiqiao Wang,Ning Wang,Yilin Yang,Bingru Shao,Qiannan Miao,Zhan Shi,Fei Yan,Shouhua Feng
B-cell lymphoma (BCL) is a hematological malignancy with high heterogeneity and represents an aggressive proliferation of mature B-cells. Despite the initial success of traditional treatments for BCL in clinical trials, a majority of patients eventually develop resistance to therapy and have poor clinical outcomes. Epigenetic dysregulation is a major contributor to the pathogenesis of BCL, and therapies targeting epigenetic pathways is a promising alternative strategy for treating BCL. Herein, we developed a metal–organic framework (MOF)-based nano-sonosensitizer for ultrasound-driven cascade immunotherapy against BCL. The nano-sonosensitizer was synthesized by encapsulating copper complex of the m6A-mRNA demethylase inhibitor into UiO-66-NH2, which possesses a Z-scheme heterostructure and allows efficient electron–hole pair separation for generating reactive oxygen species (ROS) under ultrasound activation. These CuR@UiO66 sonosensitizers were functionalized with mPEG-PO3 and anti-CD19 antibody, and the resulting CRUPPA19 particles could specifically accumulate in the BCL tissue and also target lymphoma cells that infiltrated into the bone marrow. Once internalized, CRUPPA19 could induce intracellular ROS production and apoptosis under ultrasound irradiation. Subsequently, ultrasonic stimulation triggered autophagy-mediated release of Cu and Rhein from CRUPPA19, thereby increasing protein lipoylation and global mRNA methylation, which led to cuproptosis and the transcriptional repression PDL1, respectively. These cascades synergistically induced immunogenic cell death in the tumors and promoted activation of CD8+ T cells, eventually leading to an antilymphoma immune response. CRUPPA19-mediated sono-immunotherapy not only eliminated the primary and metastatic lymphomas but also cleared lymphoma cells from the bone marrow. This study provided an insight into a MOF-based nanoepigenetic therapy platform with ultrasound-triggered cascade amplification for enhanced antihematological tumor immunity.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-18
·
IF 2.4
Xu Lingling,Pan Xiaomei,Gao Lijing,Wei Ruiping,Li Jihang,Wen Xiu,Li Yuanzhuang,Xiao Guomin
UiO–66–NH 2 (Ti/Zr) modified by Ti metal oxide (TiO 2 ) was used to catalyze the hydrolysis of cellulose to prepare 5-HMF. Under the optimal reaction conditions of H 2 O(NaCl)/THF(1/4 mL), 190 °C, 2 h and 50 mg UNT-3(Ti/Zr) (TiO 2 and UiO–66–NH 2 with mass of 1.5 and 0.1 g, respectively), the yield of 5-hydroxymethylfurfural reached 59.88%. UiO–66–NH 2 (Ti/Zr) nanocomposites with different mass ratios were successfully prepared by simple solvent evaporation method. SEM and TEM have shown that the modified UiO–66–NH 2 (Ti/Zr) are wrapped into sphere by TiO 2 densely attached to the surface of UiO–66–NH 2 , which provides favorable conditions for the uniform dispersion of TiO 2 and coordination of the Lewis acidic site of UiO–66–NH 2 . NH 3 –TPD results confirmed the existence of super-strong, strong, middle and weak acid sites in UiO–66–NH 2 (Ti/Zr), and Py-FTIR confirmed the existence of Brønsted and Lewis acids. After four cycles, the yield of 5-HMF and FUR decreased slightly from 59.88 to 51.89% and 9.11 to 7.66%, respectively, and the yield of 5-HMF could still remain above 50%. The results showed that the modified composite treatment of TiO 2 with rich Lewis acid/base and UiO–66–NH 2 could provide a certain idea for the extensive application of biomass research in the future. Graphic
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xiaoyan Han,Shan Wang,Tingting Cui,Yumin Yang,Haixiang Li,Haiwen Zhang,Huanhuan Zhou,Xiaoxia Li
Aristolochic acid I (AA-I), a known nephrotoxin and carcinogen, is commonly found in certain medicinal plants, posing significant safety concerns. In this work, defect-engineered, molecularly imprinted UiO-66-NH2 was synthesized via a one-pot hydrothermal method using indomethacin (IND) as a green alternative template. The resulting imprinted metal–organic framework effectively mitigates matrix interference, enabling highly selective recognition and the efficient adsorption of AA-I. Structural characterization confirmed that the imprinting process and template removal did not compromise the framework integrity of UiO-66-NH2. Spectroscopic analysis revealed that AA-I recognition was governed by Zr coordination, electrostatic interactions, and spatially confined recognition sites within the porous framework. Density functional theory calculations further elucidated the interaction mechanisms involved in the adsorption process. The imprinted UiO-66-NH2 exhibited a maximum adsorption capacity of 42.74 mg/g and an imprinting factor of 2.48. In real sample analysis, the material achieved recovery rates of 96.7–103.5% and excellent selectivity in Clematis armandii extracts. The adsorption efficiency remained above 80% after five adsorption–desorption cycles, indicating good structural stability and reusability. This work offers a promising and sustainable strategy for improving herbal medicine safety through the rational design of ecofriendly MOF-based adsorbents.
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Jiaqi Niu,Jinhui Liu,Ping Guo,Min Du,Wanqing Wu,Ziyang Zhang,Ye Ning,Dedi Zhou,Haidong Cao
As a common contaminating bacterium, Escherichia coli (E. coli) has caused severe harm in various fields such as food, healthcare, and the environment. Traditional detection methods for Escherichia coli, owing to factors like high cost and low efficiency, are unable to meet the detection requirements at the present stage. Therefore, the development of a simple, rapid, and highly efficient detection method for Escherichia coli represents an urgent issue that needs to be addressed promptly. This study focused on the development of a highly selective molecularly imprinted electrochemical sensor for E. coli. Molecularly imprinted polymers (MIPs) were prepared by electropolymerization on the surface of glassy carbon electrode using o-phenylenediamine as the functional monomer, aminated metal-organic frameworks (MOFs) and carbon nanotubes (CNTs) as the composites, and bovine serum albumin (BSA) was added into the polymer film to attenuate the non-imprinting effect. The linear range of the sensor was 10-10 7 CFU/mL and the detection limit was 5.2 CFU/mL. Good recovery rates were shown in real samples of drinking water, milk and orange juice. In addition, the good binding ability of the E. coli template molecule to the functional monomer o-phenylenediamine was verified by molecular docking and molecular dynamics (MD) simulations. This study was able to detect E. coli in 20 min, which provides a more open idea for the application of rapid detection of E. coli on-site, as well as the construction of molecularly imprinted electrochemical sensors and the analysis of the binding mechanism between template molecules and functional monomers.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Chengyu Sun,Yihao Ji,Wenyan Huang,Fuli Deng,Yi Zhang
The recovery of rare earth elements from mineral wastes is extremely critical for the soaring global demand due to their unique roles and resource scarcity. In this work, the defective phosphoric acid functionalized UiO-66-COOH (UiO-66-COOH-OP-ST2) was prepared via the successive phosphoric acid functionalization and defect modulation procedures towards UiO-66-COOH. The adsorption results disclosed that maximal adsorption capacities of UiO-66-COOH-OP-ST2 and phosphoric acid functionalized UiO-66-COOH (UiO-66-COOH-OP) were found to be 132.76 and 83.11 mg/g at pH = 6, respectively. Adsorption kinetics curves and isotherms revealed that the adsorption process was consistent with pseudo second order kinetic model and Langmuir isothermal model. Furthermore, UiO-66-COOH-OP-ST2 can maintain 91.74 % of initial adsorption capacity after five consecutive adsorption–desorption cycles, and exhibit no significant changes in the XRD patterns, demonstrating an excellent recycling stability. In addition, the adsorption mechanism elucidated that the elevated adsorption performance was mainly attributed to the electrostatic attraction and complex interaction between the O sites and Yb(III) based on EDS and XPS analysis. This work efficiently improved adsorption performance of metal organic frameworks after simultaneously grafting functional groups and creating defective sites without affecting their stabilities.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Wenli Zhang,Yijie Zhou,Zhenzhen Wu,Cheng Pan,Qunpeng Cheng,Guozhi Fan
A porous sulfonic acid-functionalized zirconium-based metal–organic framework possessing both Lewis acid and Brønsted acid sites (UiO-66-SO 3 H) was synthesized and tested for the selective conversion of furfural (FUR) to isopropyl levulinate (IPL) through one-pot cascade reaction. UiO-66-SO 3 H exhibited excellent catalytic performance, and the conversion of FUR as well as the yield and selectivity of IPL reached 96.4 %, 86.0 %, and 89.2 %, respectively. UiO-66-SO 3 H could be simply recovered and reused, but the catalytic performance was significantly decreased. The FUR conversion and IPL yield dropped to 73.8 % and 65.1 %, respectively, after 1 cycle, and the reason for the decrease in the catalyst activity were also investigated. It was found that the decrease was mainly caused by the loss of some −SO 3 H groups, and the cyclic performance of UiO-66-SO 3 H could be restored by supplementing a small amount of BDC-SO 3 Na. A plausible mechanism for the selective synthesis of IPL from FUR was proposed, wherein both Lewis acid and Brønsted acid sites played important roles. This work provides guidance for the selective conversion of FUR into IPL, and the high-valued utilization of biomass and its derivatives.
✓ 已验证
产品关联
DOI
高影响因子
Chemosensors
·
2025
·Vol. 13
·期 9
·340
·
IF 3.7
Hongmei Gao,Yourong Zhao,Yuhong Xie,Yiying Wang,Jie Che,Daojiang Gao,Zhanglei Ning
In this study, a novel carbon quantum dots-functionalized UiO-66 composite was successfully prepared via the post-synthetic modification method and further developed into a ratiometric fluorescent probe for detecting uric acid. The composite demonstrates excellent structural and luminescent stability under challenging environmental conditions. As a ratiometric fluorescent probe, its recognition principle relies on the ratio of response signals from two different fluorescent emission centers in the composite. In the presence of uric acid, the fluorescence emission intensity at 430 nm from CDs did not change significantly. However, the fluorescence intensity at 545 nm from Tb3+ions decreased remarkably. This material was evaluated for its capacity to sense urinary components and was shown to specifically recognize uric acid over a wide concentration range (0~5 × 10−3M). Moreover, it exhibited strong resistance to interference and high sensitivity in uric acid detection. The detection limit (LOD) was determined to be 0.102 μM through quantitative analysis. The sensing mechanism was validated through spectral overlap and fluorescence lifetime analysis, which can be attributed to the fluorescence resonance energy transfer (FRET) process. This ratiometric fluorescent probe provides an efficient and reliable strategy for detecting the biomarker uric acid.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）