ACS Catalysis
·
2020
·
IF 12.35
Junli Guo,Lingling Yang,Zhida Gao,Chenxi Zhao,Ye Mei,Yan-Yan Song
Maintaining the high activity of an enzyme is a fundamental requirement to widen the application of metal–organic frameworks (MOFs) in the biotechnology, biosensor, and biomedicine fields. However, it is still challenging to monitor and understand an MOF environment-related activity for an enzyme. Here, we developed a MOFs-in-nanochannels configuration for broadening the biocatalytic activity of an enzyme in MOFs on demand. ZIF-8 [Zn(mim)2, Hmim = 2-methylimidazolated] grown in TiO2 nanochannels is used as the platform, and cytochrome C (CytC) is used as a model enzyme encapsulated in ZIF-8. The enzymatic catalytic process converts 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) to a positively charged product (ABTS+). On the basis of current–voltage properties, the change of ion transport characteristics in nanochannels can be monitored with time. The ZIF-8 encapsulating CytC molecules not only exhibit a significantly enhanced enzymatic activity in a wide temperature region (37–80 °C) but also have remarkably long storage stability at room temperature. The results of quantum mechanical calculation indicate that the Fe–S bond of CytC is inclined to break in the environment of ZIF-8 owing to the confinement effect of the MOF structure, favorable for enzymatic catalysis. The MOFs-in-nanochannel configuration provides an innovative and label-free design for the onsite monitoring of catalytic activity of an enzyme in MOFs, which holds great potential in constructing biosensing platforms with remarkable performance and stability.
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2020
·Vol. 25
·期 6
·1312
·
IF 3.267
Kan Li,Jing-jing Li,Ni Zhao,Ying Ma,Bin Di
Serious environmental and human health problems caused by the abuse of antibiotics have attracted worldwide concern. Recently, metal–organic frameworks (MOFs) with high porosity have drawn wide attention for their effects in the adsorption and removal of pollutants from complex matrices. Herein, a high-stable metal organic framework (MOF), i.e., ((ZnCl2)3(L)2·DMF)n, whereL=1,3,5-tris((pyridin-4-ylthio)methyl)benzene), MOF1,was applied to adsorb and remove tetracycline from sewage and dairy products. The results showed that MOF1exhibited a strong performance in the adsorption of tetracycline. The effects of initial pH values, adsorbent dose, contact time and ionic strength of the adsorption performance of MOF1were investigated. The adsorption kinetics best fit the pseudo-second order model, and the adsorption isotherms matched the Langmuir adsorption model well. It was indicated that both chemical adsorption and physical adsorption play an important role in the adsorption process, and the adsorption of tetracycline was homogeneous and occurred on a monolayer on the surface of MOF1. Additionally, the stability of MOF1and the details of the adsorption mechanism were also investigated. Thus, this study provides a new candidate for the application of MOFs-based adsorbents in the removal of antibiotics from sewage and dairy products.Keywords:MOF;adsorption and removal;tetracycline
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 6
·1-9
·
IF 6.232
Chen Yang,Huang Ailan,Zhang Lu,Bie Zijun
A highly oriented crystalline metal-organic framework (MOF) nanofilm array was prepared and used for surface-assisted laser desorption ionization mass spectrometry (SALDI-MS) for determination of small molecules. The MOF nanofilm was characterized using scanning/transmission electron microscopy, X-ray diffraction, and ultraviolet-visible spectroscopy. Different small molecules (anthracene, n-eicosanoic acid, Rhodamine B) were successfully determined by this MOF nanofilm array with limits of detection (LOD) between 0.1–5 ng·mL −1 and limits of quantification (LOQ) between 1 and 10 ng·mL −1 . Compared to previously reported MOF-based SALDI-MS, this array exhibits better reproducibility (3.3–5.2%) and recovery (89–105%). The intensity of the MS peak remains the same after 25 repeated cycles. This indicates good repeatability. This MOF nanofilm-based SALDI-MS array can be used for determination of fatty acid and Rhodamine B in real samples with good recovery (83–106%).
Schematic representation of the principle of crystalline MOFs nanofilm-based SALDI-MS array
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2020
·
IF 3.557
Qingsi Li,Hongshuang Guo,Jing Yang,Weiqiang Zhao,Yingnan Zhu,Xiaojie Sui,Tong Xu,Jiamin Zhang,Lei Zhang
A metal–organic framework (MOF)-based antibiofouling hemoadsorbent (PCB-MIL101) was developed through a facile encapsulation of MIL-101(Cr) in zwitterionic poly carboxybetaine (PCB) hydrogel. PCB-MIL101 possessed strong mechanical strength and superior hemocompatibility, ensuring its safety in hemoperfusion applications. In addition, it showed efficient and effective adsorption toward bilirubin (BR), and its maximum adsorption capacity was ∼583 mg g–1. Moreover, due to the protection of antibiofouling PCB hydrogel, PCB-MIL101 showed ability to resist protein adsorption, thus working effectively to remove BR molecules from their binding albumin in biological solutions. The finding in this study provides a novel insight into developing MOF-based hemoadsorbents for the improvement of hemoperfusion therapies.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CONTROLLED RELEASE
·
2020
·
IF 7.727
Cheng Zhang,Sheng Hong,Miao-Deng Liu,Wu-Yang Yu,Ming-Kang Zhang,Lu Zhang,Xuan Zeng,Xian-Zheng Zhang
Glucose-responsive insulin delivery system mimicking the function of pancreatic β-cells to maintain blood glucose homeostasis would effectively alleviate diabetes. Here, a new glucose-responsive delivery ( [email protected] &GOx) for self-regulated insulin release was constructed by encapsulating insulin and glucose oxidase (GOx) into pH-sensitive zeolitic imidazole framework-8 (ZIF-8) nanocrystals . After entering the cavities of ZIF-8, glucose can be oxidized into gluconic acid by GOx , causing a decrease in local pH. Then, ZIF-8 nanocrystals would be degraded under the acidic microenvironment that in turn triggers the release of insulin in a glucose responsive fashion. In vitro studies indicated that the biological activity of insulin could be protected by the rigid structure of ZIF-8 and the release of insulin could be modulated in response to glucose concentrations. In vivo experiments demonstrated that a single subcutaneous injection of the [email protected] &GOx would facilitate the stabilization of blood glucose level of normoglycemic state for up to 72 h in type 1 diabetes (T1D). The multifunctional insulin delivery system shows a new proof-of-concept for T1D treatment by using ZIF-8 nanocrystals loaded with insulin and enzyme.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 21
·3413-3418
·
IF 4.568
Yuxiao Li,Ting Wang,Dahuan Liu
Graphical In this work, we report the fabrication of ultrathin and defect-free Zr-BTB membranes constructed by the assembly of monolayer MOF nanosheets with tunable gas separation performance. H 2 /CO 2 selectivity of the membranes can be enhanced by increasing the membrane thickness or by introducing the thermal disturbance during the membrane fabrication process. Two-dimensional (2D) metal-organic frameworks (MOF) nanosheets have emerged as novel membrane materials for gas separation. However, the development of ultrathin MOF membranes with tunable separation performances is still a challenge. Herein, we developed a facile GO-assisted restacking method to fabricate defect-free membranes with monolayer Zr-BTB nanosheets. Obtained ultrathin membranes ranging from 130 nm to 320 nm show tunable separation performances and exceed the 2008 Robeson upper bound by changing the amount of nanolayers in vertical stacking direction. Furthermore, a heating filtration method was used to change the restacking process of nanosheets in the horizontal direction. As a result, H 2 /CO 2 selectivity can be enhanced by two times with the same membrane thickness (130 nm) and H 2 permeance is almost maintained to be 7.0×10 −7 mol m −2 s −1 pa −1 . This method may provide a possible way to efficiently tune the gas separation performances of MOF membranes.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 33
·6646-6657
·
IF 6.331
Xue Cai,Yuewu Zhao,Li Wang,Mingchao Hu,Zeen Wu,Lifen Liu,Weipei Zhu,Renjun Pei
Photodynamic/photothermal therapy (PDT/PTT) has become a research focus of cancer treatment due to the non-invasiveness, spatio-temporal controllability, and effectiveness of repeated treatment. Here, Au@MOF core–shell hybrids were designed and constructed by the layer-by-layer method, and the thickness of the MOF shell can be adjusted by controlling the coordination reaction between the layers. Au nanorod cores mainly produce the PTT effect due to their strong absorbance at 650 nm. The porphyrin ligand in the MOF shell can convert O2 into 1O2 under light conditions, resulting in a high PDT effect. Moreover, the metal node Fe3O(OAc)6(H2O)3+ cluster of the MOF can catalyze the decomposition of H2O2 into O2 to overcome the hypoxic environment of tumors, which further improves the effect of PDT. The combination of the porphyrin ligand in the MOF structure and Au nanorods has promoted the synergistic effects of PDT/PTT. As expected, the results confirmed that Au@MOF hybrids showed no obvious biotoxicity in both cells and animal experiments, and exhibited good biocompatibility. With the synergistic effects of PDT/PTT, cancer cells could be effectively killed and tumor growth could be inhibited. In addition, the modification of folic acid on the surface of Au@MOF can further enrich the hybrids at the tumor site and enhance the inhibitory effect on tumors. These studies have proved that PDT and PTT can be effectively combined and have greater advantages in enhancing the treatment of tumors.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Changfei Liu,Yaoyao Liu,Zhonghua Xiang,Dahuan Liu,Qingyuan Yang
The synthesis of highly efficient and stable CdS composites without noble metals has become a hotspot in the photocatalytic field. Although NiS is an ideal candidate, it remains a challenge to optimize the combination of NiS and CdS to improve the photocatalytic activity for hydrogen evolution. Herein, we have successfully synthesized a CdS@NiS photocatalyst using bimetallic metal–organic frameworks (MOFs) as the precursor. The formation of bimetallic Cd/Ni-MOFs can lead to well-contacted heterogeneous interfaces between CdS and NiS at the nanoscale, efficiently promoting the separation of photogenerated carriers and boosting electron interface transfer. The obtained results demonstrated that CdS@NiS exhibits a high photocatalytic hydrogen evolution rate of 42.7 mmol·g–1·h–1, and the corresponding apparent quantum yield reaches 13.23% at 450 nm, superior to those obtained using the traditional simple physical mixing methods. This work provides a promising strategy for the design of new photocatalysts for hydrogen evolution.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zhong Wei Jiang,Ting Ting Zhao,Chun Mei Li,Yuan Fang Li,Cheng Zhi Huang
A reliable and sensitive detection approach for SARS-CoV 2 is essential for timely infection diagnosis and transmission prevention. Here, a two-dimensional (2D) metal–organic framework (MOF)-based photoelectrochemical (PEC) aptasensor with high sensitivity and stability for SARS-CoV 2 spike glycoprotein (S protein) detection was developed. The PEC aptasensor was constructed by a plasmon-enhanced photoactive material (namely, Au NPs/Yb-TCPP) with a specific DNA aptamer against S protein. The Au NPs/Yb-TCPP fabricated by in situ growth of Au NPs on the surface of 2D Yb-TCPP nanosheets showed a high electron–hole (e–h) separation efficiency due to the enhancement effect of plasmon, resulting in excellent photoelectric performance. The modified DNA aptamer on the surface of Au NPs/Yb-TCPP can bind with S protein with high selectivity, thus decreasing the photocurrent of the system due to the high steric hindrance and low conductivity of the S protein. The established PEC aptasensor demonstrated a highly sensitive detection for S protein with a linear response range of 0.5–8 μg/mL with a detection limit of 72 ng/mL. This work presented a promising way for the detection of SARS-CoV 2, which may conduce to the impetus of clinic diagnostics.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 38
·17782-17790
·
IF 6.97
Xiaoyu Wang,Wenshi Xu,Jin'ge Gu,Xiaoying Yan,Yi Chen,Mengyu Guo,Guoqiang Zhou,Shengrui Tong,Maofa Ge,Ying Liu,Chunying Chen
Air pollution is harmful to the functioning of the lungs, heart, and brain even at low concentrations of particle matter (PM) and toxic gases. Purification methods and materials have made tremendous progress to improve the purity of air to adhere to national quality standards. Metal–organic frameworks (MOFs) have an excellent gas adsorption capacity due to their high specific surface area and porous structure, but the intrinsic fragility of MOF crystals limits their application. In this study, we selected appropriate organic ligands to prepare MOF-surface-grown fibrous membranes using an electrospinning technique, which have an excellent ability to adsorb PM and capture toxic gases selectively. The efficiency of the MOF-surface-grown fibrous membranes to remove PM reached 99.99%, even for fine PM. More importantly, under low partial pressure and complex gas composition conditions, the fibrous membrane was able to selectively adsorb SO2. The concentration of SO2 dropped from 7300 ppb to 40 ppb. Interestingly, the MOF-surface-grown fibrous membrane had a higher purification capacity toward O3 than toward SO2. The concentration of O3 rapidly dropped from 3000 ppb to 7 ppb, which was far below national air quality standards (81 ppb). The MOF-surface-grown fibrous membrane was able to adsorb toxic atmospheric gases selectively, while not being influenced by the presence of other gases, such as CO2 and O2. MOF-based fibrous membranes prepared using a simple and inexpensive electrospinning technique have wide potential for practical use in the field of environmental protection and air purification.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Di Tian,Na Song,Mengxiao Zhong,Xiaofeng Lu,Ce Wang
The rational design of metal–organic framework (MOF)-based materials with a huge specific surface area, high redox activity, and favorable conductivity is currently a hot subject for their potential usage in supercapacitor electrodes. Herein, novel bimetallic MOFs with a flowerlike nanosheet structure grown on the electrospun nanofibers (PPNF@M-Ni MOF, M = Co, Zn, Cu, Fe) have been prepared by controlling the incorporation of various types of metal ions, which display superior electrochemical performance. For example, PPNF@Co–Ni MOF possesses a large specific capacitance of 1096.2 F g–1 (specific capacity of 548.1 C g–1) at 1 A g–1 and excellent rate performance. In addition, an asymmetric solid-state device composed of PPNF@Co–Ni MOF (positive materials) and KOH-activated carbon nanofibers embedded with reduced graphene oxide (negative materials) reaches a maximum energy density of 93.6 Wh kg–1 at the power density of 1600.0 W kg–1 and long cycling life. This work may greatly advance the research toward the design of supported MOF-based electrode materials for a promising prospect in energy conversion and storage.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTENGCOMM
·
2019
·Vol. 21
·期 41
·6186-6195
·
IF 3.382
Qian-Qian Liu,Ke-Fen Yue,Xian-Jun Weng,Yao-Yu Wang
A novel two-dimensional Cd-based metal–organic framework, {[Cd(Hcpnc)(DMF)]·DMF·2H2O}n (Cd-MOF) has been synthesized successfully under solvothermal conditions by utilizing a multifunctional N,O-building block ligand, 2-(2,5-dicarboxylphenyl)nicotinic acid (H3cpnc), which is a new and virtually unexplored multifunctional pyridine-tricarboxylic building block. The product was isolated as a stable crystalline solid and was fully characterized by IR spectroscopy, elemental analyses, thermogravimetry and differential scanning calorimetry, powder X-ray diffraction, single-crystal X-ray diffraction analyses, and X-ray photoelectron spectroscopy. The solid-state luminescence properties of the Cd-MOF were studied at ambient temperature. The compound shows high selectivity and sensitivity for Cu2+ ions and nitrobenzene by the luminescence quenching behavior with excellent repeatability. Additionally, the Cd-MOF exhibits an excellent specific capacitance of 321 F g−1 at 0.5 A g−1 and it still retains 95.2% of the original capacitance after 1000 cycles. Therefore, the Cd-MOF as a kind of bifunctional material will have broad application prospects in luminescence detection and supercapacitors.
✓ 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）