RSC Advances
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2018
·Vol. 8
·期 18
·10009-10016
·
IF 2.936
Zichen Xu,Guoying Zhao,Latif Ullah,Meng Wang,Aoyun Wang,Yanqiang Zhang,Suojiang Zhang
A facile strategy for the synthesis of acidic ionic liquid based UiO-67 type MOFs was developed in this study. Brønsted acids (H2SO4, CF3SO3H and hifpOSO3H (hexafluoroisopropyl sulfuric acid)) were introduced into UiO-67–bpy (bpy = 2,2′-bipyridine-5,5′-dicarboxylic acid) frameworks by reacting with bipyridyl nitrogen to introduce the properties of an acidic ionic liquid into the frameworks. The prepared catalysts, denoted as UiO-67–HSO4, UiO-67–CF3SO3 and UiO-67–hifpOSO3, were characterized by XRD, SEM, FT-IR, EA, TGA and N2 adsorption–desorption studies. The relatively high surface area was still maintained and acidic active groups were uniformly dispersed in the frameworks. The catalytic performance of UiO-67–HSO4, UiO-67–CF3SO3 and UiO-67–hifpOSO3 was evaluated by the esterification of acetic acid with isooctyl alcohol. The prepared catalysts showed good catalytic activities in the esterification, of which UiO-67–CF3SO3 gave the maximum isooctyl alcohol conversion of 98.6% under optimized conditions. The catalyst could be reused five times without a significant decrease in the conversion of isooctyl alcohol, and almost no active species were leached, indicating the excellent stability and reusability of the catalyst. Our study provides one effective way to synthesize heterogeneous acidic ionic liquid catalysts consisting of isolated, well defined acidic groups that will probably attract interest in acid catalyst chemistry.
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Nano Today
·
2024
·
IF 13.2
Qizhi Liang,Qianxi Zhou,Hai Shi,Shuai Wu,Jiahua Yang,Tianyu Zeng,Jing Zhao,Yongmei Yin,Genxi Li
The controllable assembly of metal-organic frameworks (MOFs) nanomaterials is an effective means to enhance their application capabilities. In this paper, a novel method is reported to control MOFs assembly by using a DNA framework material, a tetrahedral DNA nanostructure (TDN) labeled with phosphate groups at the vertex. In particular, various well-defined superstructures can be tailored by regulating the number of phosphate groups that coordinate with catalytic Zr-MOFs to create polymeric MOFs superstructures (Poly(MOFs)), exhibiting excellent catalytic activities and molecular recognition ability as well as greatly amplified signal readout. Furthermore, based on the DNA framework-controlled Poly(MOFs), a colorimetric biosensor with excellent analytical performance is fabricated for improving the diagnosis of human epidermal growth factor receptor 2 (HER2)-positive breast cancer. It is demonstrated that the quantification of HER2 protein can be achieved at molecular level with the limit of detection (LOD) of 12 pg L -1 and cellular level with the LOD of 10 cells. More importantly, the detection of HER2 in the serum of breast cancer patients have been achieved, thus HER2-positive and triple-negative breast cancer patients can be well distinguished. Considering the substitutability of the target, this study shows great potential in biomedical research as well as clinical applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Xueping Yan,Peng Jing,Zitian Zhuang,Jianing Zhang,Haiming Chen,Tifeng Xia,Ke Jiang
As an alternative to chemotherapy, emerging gas therapy is considered a “green” treatment due to its minimal side effects. However, even typical gas molecules like nitric oxide (NO) face challenges such as a very short half-life (1.5–6 min), poor targeting, and limited therapeutic effects. This study employs a one-pot method to simultaneously encapsulate the NO donor L-arginine (L-Arg) and the H 2 O 2 precursor Vitamin K3 (VK3) into the pores of zeolitic imidazolate framework-8 (ZIF-8), achieving their co-delivery to tumor sites to address these issues. Furthermore, ZIF-8 is functionalized with hyaluronic acid (HA) to impart active targeting properties to tumor tissues. In the acidic tumor microenvironment, pH-sensitive ZIF-8 degrades, releasing VK3 and L-Arg. Under the action of the NAD(P)H quinone oxidoreductase-1 (NQO1) enzyme, VK3 generates H 2 O 2 , increasing oxidative stress levels in the tumor microenvironment, and reacts with L-Arg to produce NO, thereby achieving tumor oxidative stress-based gas therapy. Both in vitro and in vivo experiments showed good tumor treatment effects, with a tumor inhibition rate of up to 90.5 % and minimal impact on normal tissues and organs. This approach demonstrates efficient loading, controlled release, and significant anti-tumor performance, offering new insights into gas and reactive oxygen species (ROS) synergistic therapy.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Weining Liu,Hairong Li,Dandan Huang,Xi Tan,Mingyang Zhao,Qionglin Cheng,Ming Yi,Qi Ding,Yaqian Ren,Guohan Liu
Triethylamine (TEA) poses severe safety hazards to industrial production and human health. To accurately detect TEA concentrations and rapidly warn of leakage, a simple reflux condensation method was deployed to successfully incorporate Zn 2+ in situ into Mo-MOFs precursor in a green, safe, and time-efficient synthesis condition. Subsequently, through calcination, MoO 3 /ZnMoO 4 -X (MMZ-X) were prepared, which exhibited an increased number of defects and enriched porosity, facilitating the access and interaction of TEA with adsorption sites. Simultaneously, rationally built in situ MoO 3 /ZnMoO 4 heterostructures accelerated carrier migration and induced a drastic resistive change. MMZ-2 demonstrated outstanding TEA sensing performance, exhibiting extremely high sensitivity ( R = 572.3, 100 ppm), along with superior selectivity, repeatability and stability, rapid response and recovery times, and a low detection limit. Moreover, the key intrinsic parameters of the heterostructure on the atomic scale were determined by density functional theory (DFT) calculations, providing a detailed elucidation of the sensing enhancement mechanism of the MoO 3 /ZnMoO 4 heterostructure. The simple and efficient synthesis method and the related mechanistic analysis pave a new path for designing high-performance TEA gas sensors with practical applications.
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Materials
·
2017
·Vol. 10
·期 8
·879
·
IF 2.654
Tao Chen,Cong Zhang,Yuemei Qin,Haiguan Yang,Peng Zhang,Fanggui Ye
A cationic porous framework with mobile anions (MIL-101(Cr)-Cl) was easily and successfully synthesized by utilizing the stronger affinity of F−to Al3+than Cr3+in the charge-balanced framework of MIL-101(Cr). The structure, morphology and porosity of MIL-101(Cr)-Cl were characterized. The obtained new materials retain the high surface area, good thermostability, and structure topology of MIL-101(Cr). With the mobile Cl−anion, MIL-101(Cr)-Cl can be used as an ion-exchange material for anionic organic pollutions. In this work, 2,4-dichlorophenoxyacetic acid (2,4-D) was used as a model to test the absorption performance of this new material. This new material exhibited improved adsorbability compared to that of the original metal-organic frameworks (MOFs). At the same time, this material also shows high anti-interference performance with changing solution pH.Keywords:adsorption;2,4-dichlorophenoxyacetic acid;ion exchange;metal-organic frameworks
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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.
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Small
·
2024
·
IF 13
Xiaowen Wang,Hong Zhang,Ping-Ping He,Xiaoxue Du,Yuxin Shen,Wensheng Cai,Weiwei Guo
With sequence-programmable biological functions and excellent biocompatibility, synthetic functional DNA holds great promise for various biological applications. However, it remains a challenge to simultaneously retain their biological functions while protecting these fragile oligonucleotides from the degradation by nucleases abundant in biological circumstances. Herein, a smart delivery system for functional DNA payloads is developed based on proton-mediated dynamic nestling of cytosine-rich DNA moieties within the precisely size-matched nanochannels of highly crystalline metal–organic frameworks (MOFs): At neutral pH, cytosine-rich DNA strands exhibit a flexible single-stranded state and can be accommodated by MOFs nanochannels with a size of ca. 2.0 nm; while at acidic conditions, the protonation of cytosine-rich strands weakens their interaction with the nanochannels, and the tendency to form four-stranded structures drives these DNA strands out of the nanochannels. Results confirm the successful protection of DNA payloads from enzymatic hydrolysis by the MOFs nanochannels, and the delicate coupling of the endocytosis processes and the proton-responsive Cytosine-rich DNA/MOFs systems realized the efficient intracellular delivery of DNA payloads. Furthermore, with a complementary sequence to the telomere overhangs, direct imaging of telomeres and the nucleus is successfully achieved with the proton-mediated DNA/MOFs system.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Yao Ning,Yuqi Yang,Dongming Shan,Shuxing Mei,Yibai Yan,Linjie Ding,Ying Zhang
Ethylene oligomerization plays an important role in industrial production. However, when taking the traditional non-metallocene catalysts and MOF catalysts for ethylene oligomerization, they typically require methylaluminoxane (MAO), aluminum alkyl, and other cocatalysts, which is neither environmentally friendly nor helpful in reducing production costs. Here, three sulfonic acid-modified MOFs (SA/MIL-101(Cr), UiO-66-NS and MIL-101(Cr)-NS) were prepared and used as catalysts for ethylene oligomerization at room temperature without using any cocatalysts. All of them exhibited excellent catalytic performances (e.g., 10SA/MIL-101(Cr), 21 953 g molCr−1 h−1, with C8 selectivity greater than 70.32%), and their oligomerization activity increased by almost tenfold compared to unmodified MOFs. The presence of Lewis acid (L acid) and Brønsted acid (B acid) sites in modified MOFs is the key to improved performances. In particular, the presence of B acid weakens the role of metal clusters and ligands in MOFs, making it easier for metal centers to bind to ethylene molecules for further oligomerization. This work first demonstrates that bifunctional MOF catalysts can catalyze ethylene tetramerization under mild conditions without cocatalysts.
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ANALYTICA CHIMICA ACTA
·
2025
·
IF 6
Feng Zhang,Sen Zhang,Xing Liu,Wei Gao,Jun Luo,Yi-fan Pan,Wei-Juan Zheng,Xin Hu,Hong-zhen Lian
Background Glycoproteins are critical in various biological processes and attract lots of attention of researchers. It still remains a challenge to detect glycopeptides by mass spectrometry because of their low abundance with heterogeneity and lability, as well as signal suppression by non-glycopeptides. The boronate affinity-based enrichment is an effective solution for detecting cis -diols-containing compounds including glycopeptides in complex matrices. However, there has not been any report about absolute quantitation of boron in the absorbent materials for glycopeptides, which obstructed the tailored design of boronate affinity materials and deeper understanding of interaction mechanisms. Results This work presents the development of a boronic acid-functionalized magnetic zirconium metal-organic framework (mMOF–AAPBA) with actual boron content for specific capture of glycopeptides. The synthesized nanocomposite could enrich glycopeptides by magnetic solid-phase extraction (MSPE) via the synergistic effect of hydrophilic interaction and boronate affinity. After full characterization including quantitative analysis of boron by laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS), mMOF–AAPBA was applied as MSPE absorbent to capture glycopeptides. Under the optimized conditions, it could enrich 28 glycopeptides both from horseradish peroxidase and immunoglobulin digests, with a limit of detection of 1 fmol μL −1 coupled with matrix-assisted laser desorption/ionization time of flight mass spectrometry. The boronate affinity absorbent also possessed great ability of anti-interference and good reusability. Furthermore, it possessed high performance in enriching glycopeptides in real samples including human saliva and traditional Chinese medicine injections. Significance In the preparation of the boron-containing nanocomposites, there is a special interest that an accurate protocol was established to assay boron based on LA-ICP-MS assisted by home-made matrix reference substances for the first time. These findings highlight the quantitative boron-containing mMOF–AAPBA as a robust affinity material for glycopeptide enrichment in real biological samples, offering potential applications in glycoproteomics and other cis -diols compound related researches.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Zhikun Zhang,Ying Shi,Zhengjie Li,Jilong Han,Zhiyan Chen,Fangfang Ma,Yanchao Qi,Yumin Liu
MicroRNA-21 (miR-21) has shown great promise as a biomarker for early cancer diagnosis. However, its trace-level abundance in clinical samples complicates point-of-care detection. Herein, we developed a new DNA-modified bimetallic dual-ligand MOF-based electrochemical sensor for highly sensitive and rapid detection of miR-21. The MOF was synthesized using 2,2′-bipyridine-5,5′-dicarboxylic acid (DPDC) and meso‑2,3-dimercaptosuccinic acid (DMSA) as organic linkers, with Ni²⁺/Co²⁺ serving as metal centers. Subsequently, the capture DNA (cDNA) was designed and modified MOF with high porosity and large surface area, significantly enhancing molecular interactions between the cDNA and target miR-21 to boost sensitivity. The developed biosensor exhibits a linear detection range of 10 fM to 100 nM, with a low detection limit of 10 fM and excellent specificity. This method effectively detects miR-21 in blood samples, showcasing strong clinical potential and providing a reliable platform for precision biosensing.
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CARBOHYDRATE POLYMERS
·
2025
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IF 12.5
Yilan An,Shiping Cheng,Qiaoling Ding,Dongbo Guan,Yi Hu,Yanli Dou
Flexible sensors are essential for human-machine interfaces and bioinspired intelligent robotics, yet achieving a balance between mechanical robustness and high sensitivity at lower temperatures remains a challenge. Herein, a multifunctional hydrogel sensor (PG 2 /Ag-MOFs-XG) was fabricated through physical crosslinking of polyvinyl alcohol (PVA) and xanthan gum (XG) in glycerol (Gly) and deionized water mixture via freeze-thaw circulation and NaCl crosslinking. The in situ growth of Ag-MOFs on XG molecular chains is facilitated by the electrostatic interactions between the hydroxyl groups and the carboxyl groups of XG and Ag + , restricting molecular chain movement, thereby enhancing comprehensive properties. The PG 2 /Ag-MOFs-XG hydrogel exhibits outstanding mechanical properties across a broad temperature range, with a 101 % increase in tensile strength (from 0.583 MPa to 1.17 MPa) at 25 °C and a 112 % increase (from 0.352 MPa to 0.746 MPa) at −18 °C, compared to the pure PVA hydrogel. Additionally, it demonstrates exceptional sensitivity to stretching (GF = 3.65) and compression (S = 3.38 × 10 −2 kPa −1 ). Furthermore, the hydrogel functions as a flexible sensor for monitoring human motion, assessing industrial robot performance, and detecting the tightness of robotic components. This work offers valuable insights into the development of portable, highly sensitive, and flexible sensors for intelligent robotics.
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NANOTECHNOLOGY
·
2024
·Vol. 35
·期 42
·425702
·
IF 2.9
Rui Li,Huilin Hu,Furong Xiong,Xiang Xue,Minqi Wu,Xuan Zuo,Wang Zhang,Xiangliang Pan
Efficient metal–organic frameworks (MOFs) photocatalytic bactericidal catalysts are urgently needed in water purification. Herein, a Fe-MOF (MIL-88B-NH2(V1Fe5) with promoted electron transport was achieved by vanadium (V) ions doping and V/Fe ratio optimization, showing excellent photocatalytic bactericidal activity against E. coli under visible light irradiation (99.92%). The efficient antibacterial mechanism, V as a Ti-like mediator boosting electronic transmission in MIL-88B-NH2(V1Fe5), was revealed by its band structure, transient photocurrent, electrochemical impedance spectroscopy, and scavenger quenching experiments. The enhancement of photocatalytic bactericidal performance of Fe-MOFs by V–ion-doping was confirmed by two other Fe-MOFs, MIL-53-NH2(V1Fe5) and MIL-101-NH2(V1Fe5), with the same metal ions and ligands, both of which have higher performance than the corresponding undoped MOFs. Among them, MIL-88B-NH2(V1Fe5) exhibits the highest photocatalytic bactericidal activity due to its suitable metal clusters ([M(μ3-O)] cluster) and topological structure (three-dimensional rhomboid network structure). This work demonstrated the amplification effect of V ion doping on electron transport in Fe-MOFs photocatalysts.
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