ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 11
·2211845
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IF 19
Chuan Fan,Yong Luo,Meng Tian,Mengyun Zhou,Lirong Wang,Tailin Xu,Xueji Zhang
“Green Synthesis” has been broadly applied in drug synthesis and nanomaterial preparation. The integration of automated micro-synthesis and high-throughput screening systems is a key way to achieve the goal of green manufacturing. Here, a one-click green synthesis platform is designed that integrates droplets arrays-based micro-synthesis for Raman enhancement performance high-throughput screening of MNPs@Cu-MOF (AuNPs@, AgNPs@, PtNPs@Cu-MOF) under room temperature and normal pressure. The fully integrated ultrasound units can achieve rapid multi-component mixing in the droplet array systems, and significantly accelerate materials growth as well as enhance encapsulation of noble metal nanoparticles into Cu-MOF structures. Based on such integrated systems, structures with high Raman enhancement performance can be high-throughput evaluation and easily screened out. The results indicated that the AgNPs@Cu-MOF exhibited the best Raman enhancement performance, which is ≈8 times higher than pure AgNPs. Such a green and integrated platform provides a way for automated multi-type composites fabrication, which can be expanded to multiple fields in the future via combined robotic platforms and artificial intelligence technology.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Rong Guo,Xinghui Hou,Caixin Shi,Wenpu Zhang,Ying Zhou
Metal organic frameworks (MOFs) with unique interior structure play a significant role in the field of gas-sensing. In this research, Co 3 O 4 - x hierarchical porous structure is successfully prepared by the solvothermal method and subsequent heat treatment using MOF as a sacrificial template. The effect of cobalt sources with different proportions of cobalt nitrate and cobalt chloride on the morphology, structure and gas-sensing of as-prepared Co 3 O 4 - x ( x = 0, 1, 2, 3) samples is characterized and investigated in details by various techniques of XRD , Raman, SEM, TEM, BET and XPS . The findings demonstrate that the typical Co 3 O 4 -2 sensor exhibits a significantly higher response (27.6) than Co 3 O 4 -0 (6.1) to 50 ppm acetone at 140 °C. Furthermore, Co 3 O 4 -2 sensor exhibits fairly low detection limit of 0.1 ppm, superior selectivity, repeatability, and long-term stability. The optimized acetone-sensing capability of the as-obtained Co 3 O 4 - x samples may be ascribed to the hierarchical porous structure composed of the adhered nanoparticles due to the slow dissolution of CoCl 2 ·6H 2 O, which is beneficial to increasing electron transport channels, thus improving gas sensitivity. The work provides a new idea for the preparation of respiratory monitoring materials for diabetic patients.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Luwei Wang,Chenliu Tang,Pengfei Huang,Xiang Hu,Zhirong Sun
The widespread detection and potential adverse effects of antibiotics in the aquatic environment call for effective treatment technology. Electro-Fenton is a promising strategy, but the preparation of efficient and stable cathodes is still challenging. In this study, a novel metal-organic framework (MOF)-derived N-doped cathode Fe/Cu-C400Ar was synthesized successfully for the degradation of ceftazidime (CAZ) in heterogeneous electro-Fenton (hetero-EF) system. The doping of copper could enhance electrocatalysis with a high electrochemical surface active area and low resistance. Fe/Cu-C400Ar cathode achieved CAZ removal efficiency of 99.5 ± 0.4% within 120 min, and it exhibited excellent stability after six recycle runs. Quenching experiments and electron paramagnetic resonance (EPR) tests proved that the primary species was hydroxyl radical during the CAZ degradation. In addition, the degradation pathway of CAZ was proposed including the cleavage of the pyridine ring and the shedding of the thiazole ring. Moreover, the prediction of intermediates toxicity by Ecological Structure Activity Relationships (ECOSAR) software indicated the environmentally friendly features of the CAZ degradation process. This study provided a promising cathode for the electrocatalytic degradation of antibiotic wastewater in hetero-EF system.
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FOOD CHEMISTRY
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2022
·
IF 9.231
Hui Shu,Tingrun Lai,Zhichao Yang,Xuechun Xiao,Xiumin Chen,Yude Wang
High sensitivity and ultra-trace detection of imidacloprid are important and challenging in the field of food. In this study, we prepared a Fe-rich FeCoNi-MOF in-situ modified nickel foam working electrode by one-step hydrothermal method, and achieved a highly sensitive detection of the imidacloprid. The characterization techniques confirmed that Fe-rich FeCoNi-MOF had excellent crystallinity, tighter structure, and exposed rich active sites. The detection results showed that Fe-rich FeCoNi-MOF electrochemical sensor had a minimum detection limit of 0.04 pmol/L (100 times lower than that of the bioelectrochemical sensors), a wide response range (1 pmol/L–120 μmol/L), and high sensitivity (124 μA pmol/L -1 cm −2 ). These advantages of the electrochemical sensor were revealed theoretically by the valence change of active metal and the first principle calculation. Lastly, the Fe-rich FeCoNi-MOF electrochemical sensor was applied to detect imidacloprid in apple, fresh tea leaves, tomato, cucumber, and had an excellent recovery of 98–102.8 %.
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高影响因子
JOURNAL OF ELECTRONIC MATERIALS
·
2022
·Vol. 52
·期 1
·1-9
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IF 2.047
Wang Liang,Jiang Shiqi,Li Xiaoyue,Huang Jiajie,Li Yaxuan,Gao Jingyi,Wang Yuting,Yang Yefeng
Cobalt disulfide (CoS 2 ) has attracted much attention as anodes of sodium-ion batteries (SIBs) due to its high theoretical capacity. Nevertheless, the serious volume variation and polysulfide dissolution issues during cycling usually lead to poor electrochemical performance, greatly limiting its application. Here, by employing a CuCo-based metal organic framework (MOF) and bacterial cellulose (BC) as precursor and template, we have fabricated heterostructured CoS 2 /CuCo 2 S 4 particles anchoring on an N-doped carbon framework (denoted as CuCo-S/NC) through ion adsorption and exchange reaction with a subsequent thermal annealing process. The generation of a CoS 2 /CuCo 2 S 4 heterostructure which can boost the charge transfer rate in the hybrid composite has been investigated, while the introduction of an N-doped carbon framework derived from the BC could not only enhance the electrical conductivity but also improve the structural integrity by mitigating the mechanical stress and inhibiting the aggregation of active materials. Benefitting from the designed composition and structure, the optimal CuCo-S/NC electrode exhibits a high capacity of 889 mAh g −1 at 0.2 A g −1 and an outstanding rate capability of 394 mAh g −1 at 10 A g −1 . The results achieved in this work indicate the great potential of this bimetallic MOF-derived template method for the rational design and fabrication of novel hybrid composite anodes for high-performance SIBs.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2022
·Vol. 195
·期 2
·1216-1230
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IF 3.094
Cheng Qiaojuan,Chi Xinyu,Liang Yingchao,Li Wanxin,Sun Jiaxin,Tao Jin,Wang Zhi
Metal–organic frameworks (MOFs) can be used as the immobilization carriers to protect the physicochemical properties of enzymes and improve their catalytic performance. Herein, we report an in situ co-precipitation method to immobilize lipase from Candida sp. 99–125 in Cu-BTC MOF (BTC = 1, 3, 5-benzene tricarboxylic acid, H 3 BTC). Characterizations of the immobilized lipase (lipase@Cu-BTC) have confirmed the entrapment of lipase molecules in Cu-BTC MOF. The immobilized lipase has been successfully applied for resolving N- hydroxymethyl vince lactam ( N -HMVL) and its catalytic activity is five times that of native enzyme. More importantly, we found that Cu-BTC MOF can afford powerful protection for enzyme in nearly dry organic solvent and endow the immobilized lipase with excellent reusability and storage stability. Our present study may widen the application of immobilized enzyme with MOF as the immobilized carrier. Graphical Abstract
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Xiaolu Tian,Yikun Yi,Zhendi Wu,Guangyu Cheng,Shentuo Zheng,Binren Fang,Tao Wang,Dmitry G. Shchukin,Feng Hai,Jingyu Guo,Mingtao Li
Although the low t Li + and fluid nature of ionic liquid electrolytes can lead to weakened rate capability and higher leakage risks, these challenges can be tackled by incorporating ILs into solid hosts with controlled properties. Herein, we designed a heterogeneous metal organic framework (MOF)/polymerized ionic network (PIN) core-shell composite as a porous host for IL N,N-diethyl-N-(2-methoxyethyl)-N-methylammonium bis(trifluoromethylsulphonyl)imide (DEME-TFSI). The PIN shell with abundant ionic structures exhibit nice compatibility with ILs to achieve high loading, while the MOF core has narrow nanopores to confine large anions in ILs and enhance Li + selectivity. The as-synthesized conductive solid electrolyte (HKUST@PIN-IL-Li) showed high IL loading, high ionic conductivity over 4 × 10 −4 S cm −1 at 25 °C and increased Li + transfer number (0.367) in comparison to hollow H-PIN-IL-Li and bare IL-Li electrolyte. Overall, our research demonstrates for the first time a novel MOF@PIN core-shell structure as a solid framework for IL with high battery performance.
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BIOCHEMICAL ENGINEERING JOURNAL
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2022
·
IF 4.446
Jiacong Wu,Yi Wang,Juan Han,Lei Wang,Chunmei Li,Yanli Mao,Yun Wang
In this work, a mesoporous Zr-based MOF (MP-UIO-66) was first synthesized by biomineralization method using dextran as template and the resultant particles were applied in the immobilization of cellulase . Compared with conventional UIO-66, MP-UIO-66 has more mesoporous channels (4.6 nm) that allow cellulase (3.4 * 12.4 nm) to be entrapped into the channels, improving loading capacity and stability of immobilized enzyme . Specifically, the results showed that MP-UIO-66 had an excellent loading capacity (265 mg g −1 ) for cellulase, and the residual enzyme activity of PVP-cellulase@MP-UIO-66 (PCMU) was still about 83% after 6 cycles. Moreover, the suitable pore structure exposes the active center of cellulase to the external environment, which facilitates the mass transfer of the substrate. Based on Michaelis-Menten constant analysis, the substrate affinity (13.355 mg mL −1 ) and catalytic efficiency (1.311 mL mg −1 min −1 ) of PCMU were better than those of free cellulase (14.525 mg mL −1 , 0.732 mL mg −1 min −1 ).
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 3
·1-11
·
IF 6.408
Qiang Yu,Yang Weixia,Zhang Xiaoshuo,Luo Xueli,Tang Wenzhi,Yue Tianli,Li Zhonghong
A nanocomposite was prepared by loading UiO-67 nanoparticles onto porous carbon materials derived from Ce-MOF (Ce-PC) for fluorescence detection of glyphosate. The probe (UiO-67/Ce-PC) exhibits fluorescence emission at 414 nm as the response signal under excitation at 310 nm. The fluorescence enhancement mode of UiO-67 reduces the background interference, and the introduction of Ce-PC provide hierarchical nanostructure and large specific surface area that can increase the contact availability and improve the pre-enrichment effect, ensuring UiO-67/Ce-PC with superior sensitivity. The abundant metal hydroxyl group (M–O-H) of UiO-67/Ce-PC could recognize phosphoryl groups (-PO 3 H 2 ) of glyphosate through ligand exchange, which synergizes with H-bonding interaction and electrostatic attraction to exhibit specificity toward glyphosate. The competitive coordination effects weaken the ligand-to-metal charge transfer (LMCT) and consequently induce the fluorescence recovery. The calibration plot of the fluorescence enhancement response of UiO-67/Ce-PC towards glyphosate was recorded in the range 0.02–30 μg mL −1 with a low limit of detection (LOD) of 0.0062 μg mL −1 , which is superior to the pure UiO-67. In addition, the sensor exhibited high selectivity and satisfactory accuracy and precision with recoveries of 92.1–105.6% and RSDs below 3.4%. This work not only presents a feasible sensor for sensitive and selective determination of glyphosate from cereal samples, but also provides a promising strategy for the design of MOF-based nanocomposites to achieve trace detection of various pollutants. Graphical abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Minghui Xiang,Zhen Lu,Siyang Li,Hui Li,Chen Wang,Jin Zhang,Lide Jin,Chunyang Li
In recent years, new heterogeneous catalysts derived from metal organic frameworks (MOFs) have been widely used in advanced oxidation processes (AOPs). In this work, zeolite imidazole framework-67 (ZIF-67) and sulfide nanozero-valent iron (S-Fe) were used as precursors to prepare S-Fe/Co bimetallic nanoparticles embedded in graphitized carbon (S-Fe/Co@GC) and used to activate peroxymonosulfate (PMS) to degrade tetrabromobisphenol A (TBBPA). Morphological and structural characterization indicated that S-Fe/Co@GC compared to pre-carbonization, the pore size of the material became larger, formed a graphite carbon skeleton with excellent electrical conductivity. In a 0.2 g/L S-Fe/Co@GC and 0.6 mM PMS system, 96.1% of TBBPA (20 mg/L) was degraded within 30 min, and the degradation yielded a total organic carbon (TOC) removal of 56.2% in 60 min. This excellent catalytic activity was attributed to the synergistic effect of graphitic carbon, sulfide nanozero-valent iron and metallic cobalt. Radical quenching experiments and electron paramagnetic resonance (EPR) technology indicated that reactive oxygen species (ROS) included HO • , SO 4 •− , O 2 •− and 1 O 2 , among which O 2 •− plays a leading role in the degradation of TBBPA. Based on the LC-MS analysis of the degradation intermediates, the degradation pathway of TBBPA in the S-Fe/Co@GC/PMS system was proposed. In addition, S-Fe/Co@GC showed a low ion leaching rate, and the regenerated S-Fe/Co@GC still had high catalytic performance. This work will extend the development of MOFs encapsulate functional nanoparticle materials for environmental remediation.
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CATALYSIS LETTERS
·
2022
·Vol. 152
·期 11
·3437-3446
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IF 2.936
Yue Yihang,Li Yong,Wang Tingting,Wang Shifeng,Han Lin,Du Chun
A Pd/CeO 2 -M with high methanol oxidation performance was prepared from metal–organic framework (MOF). The reaction results indicate that the Pd/CeO 2 -M could achieve 100% methanol oxidation at 200 °C over the traditional Pd/CeO 2 -C at 350 °C. The high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and Raman show that the Pd was uniformly distributed over the CeO 2 that was rich in oxygen vacancies. The methanol temperature program surface reaction (MeOH-TPSR) demonstrates that the Pd/CeO 2 -M could effectively decompose methanol at a lower temperature with the assistance of oxygen vacancies compared with Pd/CeO 2 -C. Methanol oxidation was conducted with in-situ Raman, CO diffuse reflectance infrared Fourier transformed spectroscopy (CO-DRIFTS) and in-situ DRIFTS to elucidate the reaction mechanism and establish the structure–activity relationship. The oxygen vacancies have participated in the assistance of methanol oxidation, which was revealed via in-situ Raman. The CO-DRIFTS indicates that the chemisorbed CO was more in linear form, which demonstrates that the Pd particles were over CeO 2 -M with a smaller size. The in-situ DRIFTS experiments show the methanol could be further effectively oxidized to bidentate formate over Pd/CeO 2 -M with the assistance of oxygen vacancies. The Pd/CeO 2 -M catalysis and its enhancement mechanism studies provided a potential strategy in the VOC removal catalysis development. Graphical Abstract
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 22
·10682-10689
·
IF 3.925
Miaomiao Han,Mengzhen Ren,Zhaohui Li,Lingbo Qu,Lanlan Yu
Nanozymes with the advantages of excellent enzyme-mimicking activity, low cost and high stability have displayed great application potential in diverse fields as replacements for natural enzymes. In this study, a new nanozyme based on an ultrathin two-dimensional metal–organic framework nanomaterial D-ZIF-67 was prepared and characterized. D-ZIF-67 exhibited remarkable oxidase-like activity, which was attributed to the large specific surface area of the two-dimensional sheet structure, as well as its numerous exposed active sites compared with crystal MOFs. In the catalytic process of D-ZIF-67, the hydroxyl radical and superoxide anion played an essential role and facilitated the oxidation of the substrate 3,3′,5,5′-tetramethylbenzidine (TMB) by oxygen. The reducing agent glutathione (GSH) inhibited the catalytic activity of D-ZIF-67 besides reducing the oxidized oxTMB, based on which a simple, sensitive and accurate colorimetric method was developed to determine GSH, with the detection limit of 229.2 nM. This work mainly proposes a new two-dimensional metal–organic framework with high oxidase-like activity and provides a simple and practical platform for visual GSH detection by naked eyes.
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