Chemistry-An Asian Journal
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2021
·Vol. 16
·期 21
·3413-3418
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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.
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Analytical Methods
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2021
·Vol. 13
·期 48
·5851-5858
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IF 2.896
Yan Guan,Xiao-Lan Zhao,Qiu-Xia Li,Long Huang,Jian-Mei Yang,Tong Yang,Yun-Hui Yang,Rong Hu
In this paper, a novel colorimetric strategy based on iodide ion (I−) and Cu-MOF catalysis was developed for simple, low-cost, and naked-eye detection of Fe3+. Both I− and MOFs display catalytic activity toward peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB). Adsorption and embedding of I− in Cu-MOF generates Cu-MOF/I with a three-dimensional porous structure that exhibits higher specific surface area, providing more active sites to facilitate interaction with TMB, resulting in enhanced catalytic efficiency. Reports have shown that Fe3+ can oxidize TMB in the absence of H2O2. We found that as Fe3+ concentration increases, the color of the system gradually deepens and the UV absorption peak gradually increases, thus providing a colorimetric sensor for quantitative Fe3+ detection. The detection limit (LOD) obtained in the presence of I− is 200 nM; however, in the absence of I−, the LOD is approx. 10 μM. Thus, the sensing system is ideal for signal amplified analysis of Fe3+. In the presence of various interfering metal ions, the developed sensing system displays excellent selectivity. Additionally, the practical application to Fe3+ detection in real samples is explored.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 45
·21350-21358
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IF 3.591
Zhen-Zhen Ma,Yao Ma,Bing Liu,Ling Xu,Huan Jiao
Two cobalt metal–organic frameworks (Co-MOFs), [Ch]2[Co3(BDC)3Cl2] (1) and [Ch]2[Co3(BDC)4]·2DMU (2) (Ch+ = choline cation; H2BDC = terephthalic acid; DMU = 1,3-dimethylurea), were prepared through ionothermal reactions with deep eutectic solvents (DESs) of ChCl and DMU as the reaction media. The 1/GCE electrode with better current response was selected as the electrocatalyst. The detection performance of the 1/GCE electrode towards glucose is excellent with a wide linear range of 10–1200 μmol L−1, a detection limit of 3.2 μmol L−1 (S/N = 3), and a rapid response less than 3 s in 0.01 mol L−1 NaOH. 1 also exhibits high anti-interference with the existence of D-Man, D-Fru, DL-AA, and BA, long-term stability of 15 days and reproducibility for glucose detection. 1 was utilized to detect glucose in human serum and orange juice. The found glucose concentrations are very close to the added glucose concentrations in the selected situations with low RSD and high recoveries. This demonstrates that as a non-enzymatic glucose sensor, 1/GCE can detect glucose with high accuracy and reliability in different environments.
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ACS Applied Materials & Interfaces
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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.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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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.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Lin Yue,Yunmeng Cao,Yonghui Han,Zaixing Li,Xiao Luo,Yanfang Liu
The magnetic metal-organic framework composite Fe 3 O 4 @Sn-MOF with core-shell structure was successfully prepared by hydrothermal synthesis. It was characterized by XRD , TEM , BET, DRS , FT-IR, XPS and VSM. The photocatalytic performance of the composite was evaluated by degradation of Acid Red 3R (AR3R) dye under simulated light source. Under the conditions that the additive amount of the catalyst was 6.7 g/L, the initial concentration of AR3R was 50 mg/L and the initial pH of AR3R was 3.0, Fe 3 O 4 @Sn-MOF revealed the optimized photocatalytic activity with 100% degradation efficiency of AR3R at 30 min. The excellent photocatalytic ability was mainly ascribed to the effective charge separation, strong photo-response and rich active sites. Besides, using Fe 3 O 4 as the magnetic nucleus was conducive to improve the recovery rate of the catalyst. The EPR and free radical analysis indicate that •O 2 − and •OH played important roles in the photocatalytic reaction. Meanwhile, a possible degradation process and mechanism were proposed by the full band scanning of AR3R, 3D-EEM fluorescence analysis and electrochemical measurement.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 33
·6646-6657
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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.
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ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Wen-Chao Hu,Jie Pang,Sudip Biswas,Kang Wang,Chen Wang,Xing-Hua Xia
Bacterial infection is one of the major causes of human death worldwide. To prevent bacterial infectious diseases from spreading, it is of critical importance to develop convenient, ultrasensitive, and cost-efficient methods for bacteria detection. Here, an electrochemical detector of a functional two-dimensional (2D) metal–organic framework (MOF) nanozyme was developed for the sensitive detection of pathogenic Staphylococcus aureus. A dual recognition strategy consisting of vancomycin and anti-S. aureus antibody was proposed to specifically anchor S. aureus. The 2D MOFs with excellent peroxidase-like activity can efficiently catalyze o-phenylenediamine to 2,2-diaminoazobenzene, which is an ideal electrochemical signal readout for monitoring the bacteria concentration. Under optimal conditions, the present bioassay provides a wide detection range of 10–7.5 × 107 colony-forming units CFU/mL with a detection limit of 6 CFU/mL, which is better than most of the previous reports. In addition, the established electrochemical sensor can selectively and accurately identify S. aureus in the presence of other bacteria. The present work provides a new pathway for sensitive and selective detection of S. aureus and presents a promising potential in the realm of clinical diagnosis.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2021
·Vol. 45
·期 9
·13040-13054
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IF 5.164
Peng Su,Hai Liu,Qingxiang Ma,Zhiliang Jin
Summary The photocatalytic hydrogen evolution reaction is one of the important ways to convert solar energy into renewable hydrogen. In this work, the Co 9 S 8 hollow polyhedron was formed after sulfidation and calcination with the metal-organic framework ZIF-67. The hollow polyhedron Co 9 S 8 provides abundant support sites for Mn 0.05 Cd 0.95 S and effectively reduces the agglomeration degree of Mn 0.05 Cd 0.95 S. The Co 9 S 8 hollow polyhedron as the reaction site has a large specific surface area and a mesoporous structure, which is beneficial to the progress of the photocatalytic reaction. A series of tests showed that the introduction of Co 9 S 8 hollow polyhedron significantly improved the light-trapping ability and exposed more reaction sites. Co 9 S 8 hollow polyhedrons are used as electron capture sites, which can effectively collect electrons and induce the interface charge transfer of Mn 0.05 Cd 0.95 S to Co 9 S 8 . Because the Co 9 S 8 -Mn 0.05 Cd 0.95 S composite catalyst had a strong light-trapping ability, abundant reaction sites and Co 9 S 8 -Mn 0.05 Cd 0.95 S heterojunction accelerate the separation and transfer of charges. Therefore, the hydrogen evolution rate of the 10%Co 9 S 8 -Mn 0.05 Cd 0.95 S composite catalyst was relatively high, which was 13.369 mmol g −1 h −1 . In addition, the 10%Co 9 S 8 -Mn 0.05 Cd 0.95 S composite catalyst still has good hydrogen evolution stability after four cycles. This research may supply a new idea for the preparation of high-efficiency photocatalysts with hollow structures. Novelty Statement The Co 9 S 8 hollow polyhedron provides abundant support sites for M 0.05 C 0.95 S particles, which effectively reduces the degree of agglomeration. The Co 9 S 8 -M 0.05 C 0.95 S heterojunction catalyst not only accelerates the migration and transfer of electrons, but also provides abundant reaction sites. Therefore, the Co 9 S 8 -M 0.05 C 0.95 S composite catalyst has good catalytic activity.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Donghong Duan,Jiarong Feng,Shibin Liu,Yunfang Wang,Xianxian Zhou
Given the scarcity and high cost of metal Pt, the search for cheap and readily available non-precious metal catalysts remains the key to solving hydrogen evolution reactions (HER) today. Transition-metal phosphides (TMPs) have been widely studied in recent years due to their excellent catalytic activity. In this work, we using Co-based metal-organic framework (MOF) as the precursor, prepared two kinds of cobalt phosphide (CoP/C) by direct phosphating and indirect phosphating methods, which showed good electrochemical performance of HER. The Di-CoP/C showed lower overpotential of 136 mV at 10 mA cm −2 in the acid electrolyte, and the slope of Tafel was 49.3 mV dec −1 . At the same time, the catalyst showed excellent stability.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Manlin Li,Weiqiu Huang,Bo Tang,Qianxi Fang,Xiang Ling,Aihua Lv
Four different kinds of metal–organic framework (MOF) materials Zn-BTC, Cu-BTC, Cr-BTC, and Fe-BTC are incorporated into alginate, forming various hydrogels for n-hexane vapor adsorption. The cross-link networks between center cations of MOFs and alginate are verified by comparing the Fourier transform infrared characteristic peaks of the MOF/alginates with that of bare alginate. Interestingly, the MOF/alginate composites cross-linked by trivalent cations (Cr3+ and Fe3+) contain micropores while those cross-linked by divalent cations (Zn2+ and Cu2+) do not. The specific surface parameters of the as-prepared hydrogels are affected by the concentration of the alginate. In addition, the Fe-BTC/alginate performs the best n-hexane vapor adsorption capacity among the four kinds of composites. This study would be helpful for a better understanding of the effect of ionic cross-linking on the alginate hydrogel surface area parameters and provide basic knowledge and reference for expanding the applications of the MOF/alginate hydrogels.
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RSC Advances
·
2020
·Vol. 10
·期 60
·36862-36872
·
IF 3.119
Mengru Cai,Liuying Qin,Longtai You,Yu Yao,Huimin Wu,Zhiqin Zhang,Lu Zhang,Xingbin Yin,Jian Ni
Metal organic frameworks (MOFs) are widely used in drug carrier research due to their tunability. The properties of MOFs can be adjusted through incorporation of mono-substituents to obtain pharmaceutical carriers with excellent properties. In this study, different functional groups of –NH2, –CH3, –Br, –OH and –CH2CH are connected to MOF-5 to analyse the effect of mono-substituent incorporation on drug delivery properties. The resulting MOFs have similar structures, except for Br–MOF. The pore size of this series of MOFs ranges from 1.04 nm to 1.10 nm. Using oridonin (ORI) as a model drug, introduction of the functional groups appears to have a significant effect on the drug delivery performance of the MOFs. The IRMOFs can be ranked according to drug-loading capacity: MOF-5 > HO–MOF-5 > H3C–MOF-5 = Br–MOF-5 > H2N–MOF-5 > CH2CH–MOF-5. The ORI release from ORI @IRMOFs is explored at two different pH values: 7.4 and 5.5, and the ORI@IRMOFs are ranked according to the cumulative release percentage of ORI: ORI@MOF-5 > ORI@Br–MOF-5 > ORI@H3C–MOF-5 > ORI@H2N–MOF-5 > CH2CH–MOF-5 > ORI@ HO–MOF-5. In particular, the release behaviour of ORI@MOFs is described through a new model. The different drug delivery performance of MOFs may be due to the complex interactions between MOFs and ORI. In addition, the introduction of single substituents does not change the biocompatibility of MOFs. MTT in vitro experiments prove that this series of MOFs has low cytotoxicity. This study shows that the incorporation of single substituents can effectively adjust the drug delivery behaviour of MOFs, which is conducive to realization of personalized drug delivery modes. The introduction of active groups can also facilitate post-synthesis modification to achieve coupling of targeting groups. MOFs incorporated with single substituents perform favorably in terms of use as biomedical drug delivery alternative carriers in effective drug payload and flexible drug release.
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