JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Chenghan Ji,Mujian Xu,Hang Yu,Lu Lv,Weiming Zhang
The development of heavy metal adsorbents with high selectivity has become a research hotspot due to the interference of coexisting ions (e.g., Na + , Ca 2+ ) in the actual wastewater, but the more difficult regeneration caused by high adsorption selectivity severely limits its practical applications. Herein, a carboxyl adsorbent, MIL-121, demonstrated high adsorption selectivity for heavy metals at 10,000 mg/L of Na + (removal > 99% for Cu 2+ ) as well as unexpected easy regeneration (desorption > 99%) at low H + concentration (10 −3.5 –10 −3.0 M), which is hundreds of times lower than that of ever reported selective adsorbents (> 10 −1 M H + ). X-ray photoelectron spectrometry (XPS), extended X-ray absorption fine structure (EXAFS) coupled with Density functional theory (DFT) simulation unveil that the -COOH groups in MIL-121 for heavy metals adsorption is specific inner-sphere coordination with higher binding energy (1.31 eV for Cu), and less energy required for regeneration (0.26 eV for H). Similar high selectivity and easy regeneration were also satisfied with other heavy metals (e.g., Pb 2+ , Ni 2+ ), and removal of heavy metals remained > 99% in 10 consecutive adsorption-desorption cycles. For actual copper electroplating wastewater treatment , MIL-121 could produce ~ 3600 mL clean water/g sample, outperforming 300 mL that of the benchmark commercial adsorbent D-113. This study shows the potential of MIL-121 for heavy metal wastewater treatment and provides mechanistic insight for developing adsorbents with high selective adsorption and easy regeneration.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Ziying Hu,Jing Chen,Dongxu Yan,Yan Li,Hongpeng Jia,Can-Zhong Lu
Chlorinated volatile organic compounds (CVOCs) existing widely in the industries are harmful to the environment and human’s health. It is urgent to develop highly efficient catalysts for their combustion. Herein, a series of porous MnO x/ Co 3 O 4 nanocomposites are synthesized by the pyrolysis of Mn@Co-ZIF-67 precursors, in which the Mn ions are introduced by impregnation method. XRD, Raman, ICP-OES, BET, SEM, TEM, XPS, O 2 -TPD, and H 2 -TPR have been performed to investigate the as-prepared catalysts’ physicochemical properties. The optimal catalyst MnO x /Co 3 O 4 -4h exhibits 90% and 100% chlorobenzene (CB) conversion (1000 ppm, Air, WHSV = 60,000 mL/(g h)) at 334 °C and 350 °C, respectively. And the better catalytic performance over MnO x /Co 3 O 4 -4h compared with the pure Co 3 O 4 and other MnO x /Co 3 O 4 nanocomposites mainly ascribes to its porous structures, homogeneous dispersion, optimal Mn/Co molar ratio, more lattice defects, and higher surface O Latt /O Ads ratio. Meanwhile, MnO x /Co 3 O 4 -4h displays high stability and resistance to moisture. Main intermediates have been further investigated by in situ DRIFT, and the degradation mechanism has been proposed according to the analysis of intermediates.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 16
·9702-9711
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IF 4.22
Yang Yongmei,Gao Xinna,Yang Sijun,Shen Yuhua,Xie Anjian
Abstract Fabricate surface-enhanced Raman scattering (SERS) substrate with low cost and high performance through simple method is a challenge and worthy of work. Herein, an excellent Cu 2 O SERS substrate with porous octahedron structure was synthesized by brief calcining Cu-MOFs in Ar, air and H 2 /Ar gas environment at 350 °C successively. The as-obtained octahedral Cu 2 O was utilized as SERS substrate to measure dye molecules and organic pollutants, which exhibited splendid sensitivity for the detection of methylene blue and 4-mercaptopyridine (4-MPY) with the ultralow limit of 5 × 10 –9 M and 5 × 10 –10 M, respectively. The maximum relative standard deviation for detection of 4-MPY is as low as 12.3%, which is less than limiting step in quantitative SERS (15.0%). The above excellent results are due to outstanding synergistic effect of electromagnetic enhancement of oxygen vacancy on the Cu 2 O surface and chemical enhancement of the Cu–S bonds formation. The fabricated Cu 2 O possesses superior sensitivity, selectivity and reproducibility for SERS detection of probe molecules with sulfhydryl groups and may be a prospect candidate in the practical application. Graphical Abstract
An excellent Cu 2 O SERS substrate with porous octahedron structure was synthesized by simple calcining Cu-MOFs in Ar, air and H 2 /Ar gas environment at 350 °C successively. The as-prepared Cu 2 O play significant roles in the enhancement of SERS signals for rich-thiol detection due to outstanding synergistic effect of electromagnetic enhancement of oxygen vacancy on the Cu 2 O surface and chemical enhancement of the Cu-S bonds formation. The detection limit of 4-Mercaptopyridine (4-MPY) can be as low as 5×10 –10 M. The porous octahedral Cu 2 O will have potential applications in SERS detection as the substrate.
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JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Siyu Zhou,Xiaoquan Feng,Junyong Zhu,Qiangqiang Song,Guang Yang,Yatao Zhang,Bart Van der Bruggen
Although membrane separations have evinced an enormous potential in the treatment of dye wastewater, the ubiquitous membrane fouling leads to a dramatic decline of separation efficacy and life span, impeding the progress of membrane-based applications. The copper-triazolate MOFs (CuTz-1) exhibit robust thermal and chemical stability with a unique feature of degrading organic molecules under the visible light, rendering them highly promising for construction of self-cleaning membrane. This study presents the utilization of photocatalytic MOFs (CuTz-1) for construction of the CuTz-1/graphene oxide (CuTz-1/GO) composite membranes via filtration-assisted assembly followed by chemical crosslinking. The presence of CuTz-1 among the GO nanosheets promotes an enhancement of the GO interlayer distance, thereby promoting a higher water flux without compromising the dye rejections. The best-performing CuTz-1/GO membranes exhibits the high water permeance of 40.2 L m −2 h −1 bar −1 and superior dye rejections (Congo red: 99.4%, direct red: 98.2%, methyl blue: 94.9%), low salt rejections (e.g., NaCl: 0.3% and Na 2 SO 4 : 19.6%), as well as long-term nanofiltration stability. Furthermore, after visible light irradiation, the treated membrane was nearly recovered to have the original separation efficacy due to effective photocatalytic removal of the attached dyes from the membrane surface. The CuTz-1/GO membrane also exhibits an ultra-high bacteriostasis rate of 100%, probably to be ascribed to the combined antimicrobial effect of CuTz-1 and GO. This work is expected to give a useful guideline for developing loose nanofiltration membranes with favorable photocatalytic and antimicrobial properties, offering an appropriate solution of using self-cleaning membranes for the treatment of dye wastewater.
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JOURNAL OF CHEMICAL SCIENCES
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2020
·Vol. 132
·期 1
·1-10
·
IF 1.406
Huang Kai,Yu Sibing,Li Xiaoxin,Cai Zhenyu
Abstract A series of novel bimetallic organic framework materials (Cu x -Co y -MOF) have been successfully prepared by a simple one-pot synthetic method, and their characters were evaluated via means of various techniques. The tested data showed a series of Cu x -Co y -MOFs displayed good crystallinity and the doping of Co in original Cu-based framework would not change the morphology of the MOF catalysts. The catalytic activity of prepared materials was tested in the catalytic oxidation of styrene in the presence of TBHP. The effects of reaction time, reaction temperature and other reaction conditions on catalytic performance were systematically studied. The results revealed that the introduction of Co can improve the selectivity to form epoxides and reduce the yield of benzaldehyde without affecting the conversion rate of catalytic oxidation reaction of styrene. Excitingly, the Cu 0.25 -Co 0.75 -MOF showed better catalytic performance than Cu-MOF and Co-MOF under the optimal reaction conditions, the conversion rate of styrene reached 97.81%, and styrene oxide selectivity reached 83.04%, which indicated a significant synergistic effect of the Cu/Co bimetallic MOF. Furthermore, the Cu 0.25 -Co 0.75 -MOF catalyst exhibited good reusability that could be reused at least four times without significant inactivation. Graphic abstract A series of novel bimetallic organic framework materials (Cu x -Co y -MOF) have been successfully prepared via a simple one-pot synthetic method, and they exhibited high activity and selectivity as catalyst towards for oxidation of styrene.
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Nano-Micro Letters
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2020
·Vol. 12
·期 1
·1-16
·
IF 12.264
Deng Baiwen,Xiang Zhen,Xiong Juan,Liu Zhicheng,Yu Lunzhou,Lu Wei
Sandwich-like laminated Fe&TiO 2 @C nanocomposites were successfully prepared from the MXene–MOFs hybrids.
A broad effective bandwidth of 6.5 GHz at a thickness of only 1.6 mm was achieved.
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高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Guocheng Zhu,Yongning Bian,Andrew S. Hursthouse,Shengnan Xu,Nana Xiong,Peng Wan
Dissolved organic matter (DOM) is not only a vector for the migration of aquatic environmental pollutants, but is also key to the control of water pollution . Economic and effective DOM removal through coagulation is essential in water treatment processes. This work investigated the role of carboxylated magnetic metal organic frameworks (MMOFs) nanoparticles in polymeric iron-based coagulation for the removal of aquatic DOM using a MMOFs-doped polyferric iron-based coagulant (MMOF-PIC). Analytical methodologies and tools used in this research included scanning electron microscopy (SEM), zeta potential , molecular weight cut off (MWCO), vibrating sample magnetometer (VSM) measurement, excitation emission matrix spectroscopy (EEMs), and X-ray photoelectron spectroscopy (XPS). The results showed that MMOF-PIC had the potential to change the structure of the polyferric iron-based coagulant (PIC) and charge, as determined by a porous surface morphology, a higher medium polymeric species distribution, and a more positive zeta potential. The MMOFs consequently enhanced PIC action on the removal of UV254 exposed DOM species with molecular weight <30 kDa, including aromatic C C based compounds, org-N as primary amines and amide/peptide bound species, water containing microbial metabolites and protein-like materials. The coagulation of DOM was enhanced by improving charge neutralization, adsorption-bridging and sweep-flocculation in the presence of MMOFs nanoparticles. This was due to hydrogen bonds , π-π bonds and covalent bonds resulting from actions of nanoparticles and pollutants. These results indicate that magnetic MOF nanoparticles can improve PIC coagulation for DOM, enhancing future removal of target pollutants.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
·
IF 3.807
Cuizhu Ye,Xingguang Chen,Junjun Xu,Huiting Xi,Tiantian Wu,Danwen Deng,Jinsheng Zhang,Ganhui Huang
Supported by metal-organic frameworks (MOFs), a new molecular imprinted electrochemical sensor (MIES) taking nano-structure Co 2+ @Fe 3 O 4 as the support point of receptor was developed for highly sensitive detection of GA in this paper. Gold electrode was modified with Co 2+ @Fe 3 O 4 , then Co 2+ @Fe 3 O 4 /Au was soaked and compounded to Fe 3 O 4 @ZIF-67/Au. MIPs film was obtained by potentiostatic polymerization with polypyrrole as monomer and GA as template. SEM, EDS, FTIR, XRD, DPV and EIS characterizations indicate the success of the preparation of the modified electrode . By optimization, the Δ i response of MIP/Fe 3 O 4 @ZIF-67/Au was strengthened from 25.38 μA to 30.84 μA. The MIP/Fe 3 O 4 @ZIF-67/Au sensor showed a superior sensitivity with a lower LOD of 0.297pM (S/N = 3) and a wider linear range of 6–600pM for GA detection, which profits from the combination of high surface area of Co 2+ @Fe 3 O 4 and high porosity of MOFs. Because of the specificity of molecular imprinted polymers (MIPs), our sensor showed advanced selectivity and not affected by similar structure interfering substances. In addition, the stability, reproducibility and real-sample detection were also satisfactory with the recovery rates between 89.5% and 118.4% and the RSD were lower than 5.5%. This sensitive and simple method can be further used to prepare polypyrrole-based MIES suported by MOFs-Co 2+ @Fe 3 O 4 for highly sensitive detection of other small and weight molecules.
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高影响因子
Small
·
2020
·Vol. 16
·期 23
·2000553
·
IF 11.459
Wen-Chao Hu,Muhammad Rizwan Younis,Yue Zhou,Chen Wang,Xing-Hua Xia
As one of the common reactive oxygen species, H 2 O 2 has been widely used for combating pathogenic bacterial infections. However, the high dosage of H 2 O 2 can induce undesired damages to normal tissues and delay wound healing. In this regard, peroxidase-like nanomaterials serve as promising nanozymes, thanks to their positive promotion toward the antibacterial performance of H 2 O 2 , while avoiding the toxicity caused by the high concentrations of H 2 O 2 . In this work, ultrasmall Au nanoparticles (UsAuNPs) are grown on ultrathin 2D metal–organic frameworks (MOFs) via in situ reduction. The formed UsAuNPs/MOFs hybrid features both the advantages of UsAuNPs and ultrathin 2D MOFs, displaying a remarkable peroxidase-like activity toward H 2 O 2 decomposition into toxic hydroxyl radicals (·OH). Results show that the as-prepared UsAuNPs/MOFs nanozyme exhibits excellent antibacterial properties against both Gram-negative ( Escherichia coli ) and Gram-positive ( Staphylococcus aureus ) bacteria with the assistance of a low dosage of H 2 O 2 . Animal experiments indicate that this hybrid material can effectively facilitate wound healing with good biocompatibility. This study reveals the promising potential of a hybrid nanozyme for antibacterial therapy and holds great promise for future clinical applications.
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高影响因子
Science Bulletin
·
2020
·
IF 9.511
Weiwei Zhao,Tiantian Chen,Weikang Wang,Beibei Jin,Jiali Peng,Shuaihang Bi,Mengyue Jiang,Shujuan Liu,Qiang Zhao,Wei Huang
The flexible transparent supercapacitors have been considered as one of the key energy-storage components to power the smart portable electronic devices. However, it is still a challenge to explore flexible transparent capacitive electrodes with high rate capability. Herein, conductive Ni 3 (HITP) 2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) thin films are adopted as capacitive electrodes in flexible transparent supercapacitors. The Ni 3 (HITP) 2 electrode possesses the excellent optoelectronic property with optical transmittance ( T ) of 78.4% and sheet resistance ( R s ) of 51.3 Ω sq –1 , remarkable areal capacitance ( C A ) of 1.63 mF cm −2 and highest scan rate up to 5000 mV s −1 . The asymmetric Ni 3 (HITP) 2 //PEDOT:PSS supercapacitor ( T = 61%) yields a high C A of 1.06 mF cm −2 at 3 μA cm −2 , which maintains 77.4% as the current density increases by 50 folds. The remarkable rate capability is ascribed to the collaborative advantages of low diffusion resistance and high ion accessibility, resulting from the intrinsic conductivity, short oriented pores and large specific areas of Ni 3 (HITP) 2 films.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Guohuan Huang,Danxia Xu,Zhimei Qin,Qun Liang,Chuanhui Xu,Baofeng Lin
Nanoscale metal-organic frameworks (nanoMOFs) are promising materials for many applications. However, for actual applications, it is a big challenge to change the brittle MOFs into flexible materials suitable for universal, large-scale fabrication. Herein, we develop a facile, universal, controllable, large-scale strategy to fabricate the tightly-bonded and flexible nanoMOFs-based composites by flexibly controlling the nucleation and growth of nanoMOFs. Based on this universal strategy, a series of tightly-bonded and flexible nanoMOFs@carboxymethylated filter paper (nanoMOFs@CMFP) are successfully prepared under mild conditions. Specifically, the retention of ZIF-67 on the ZIF-67@CMFP is still up to 93.87% after the mechanical deformation and abrasion (200 cycles), which confirms the flexibility and ultra-stability of nanoMOFs@CMFP. Moreover, besides the universal applicability, this method also can be used for large-scale synthesis of flexible nanoMOFs@CMFP. Furthermore, the excellent performance of low toxicity, antibacterial and wound healing confirms that the flexible composites have practical application value. Therefore, this study is expected to solve the problem of the flexible use of nanoMOFs in the practical application.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 8
·087502
·
IF 3.721
Ya Li,Lina Hou,Zhiling Liu,Wenbo Lu,Man Zhao,He Xiao,Tianjun Hu,Zhanfeng Zheng,Jianfeng Jia,Haishun Wu
Mucin 1 protein (MUC1) is a well-known tumor marker overexpressed in a variety of human malignancies, and thus its highly selective and sensitive detection is significantly desired for clinical diagnostics. Herein, a sensitive electrochemical MUC1 sensing platform has been fabricated based on copper-based metal-organic frameworks (Cu-MOFs) decorated with gold-platinum alloy nanoparticles (AuPt NPs). Besides serving as a redox probe to avoid introducing extra redox media, the electroactive Cu-MOFs function as catalysts in the hydrogen peroxide reduction, resulting in electrochemical signal amplification. Meanwhile, AuPt NPs loaded on the Cu-MOFs mimic horseradish peroxidase to promote the reduction of hydrogen peroxide, giving rise to the secondary-amplified electrochemical signal. Moreover, the target MUC1 triggered catalytic hairpin assembly (CHA) further improves the sensitivity of the developed biosensor via the target recycling amplification. The constructed sensing platform displayed a desirable dynamic range between 10 fM and 10 nM in the MUC1 detection, with a sufficiently low limit-of-detection (3.33 fM). The current strategy of utilizing hybrid nanocomposite consisting of MOFs and alloy NPs and enzyme-free CHA provides a promising platform for the detection of biomarkers in the clinical diagnosis with high selectivity and sensitivity.
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