JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Fan Xiao,Ming Cao,Rongrong Chu,Xiaoyu Hu,Wenxiong Shi,Yingbo Chen
A new type of composite membrane was prepared through the vacuum filtration self-assembly, in which, graphene oxide (GO) was the basic material, and the horizontal insertion material is product of perylene-3, 4, 9, 10-tetracarboxylic dianhydride (PTCDA) and UiO-66-NH 2 (PTCDA-UiO-66-NH 2 ). The leading role of Π-Π conjugate, auxiliary effect of hydrogen bonding during membrane preparation have been confirmed through Fourier transform infrared spectroscopy (FTIR), UV–visible spectrophotometer, Raman spectroscopy, and X-ray diffraction (XRD). The prepared GO@PTCDA-UiO-66-NH 2 membrane had new nodular structure compared to GO membrane by scanning electron microscopy (SEM) and atomic force microscopy (AFM), which promoted the water transport. In addition, the insertion of PTCDA-UiO-66-NH 2 narrowed the actual filtration spacing between GO sheets, and PTCDA-UiO-66-NH 2 could also adsorbed dye laterally. Experiments showed that the permeance of GO@PTCDA-UiO-66-NH 2 membrane was 1.7 times of GO membrane, and the removal of methyl blue, congo red, crystal violet and disperse black 9 was close to 100%. Under extreme pH, high salt concentration and multiple recycling, its separation ability was still excellent. The GO@PTCDA-UiO-66-NH 2 membrane constituted a unique synergistic structure of vertical-screening and horizontal-adsorption, which successfully overcame the trade-off effect and obtained excellent stability of structure and performance. Therefore, GO@PTCDA-UiO-66-NH 2 membrane had great potential in practical applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Haiyuan Chi,Chengjun Li,Mei Huang,Jinquan Wan,Xiaoxia Zhou,Bing Yan
Sulfate radicals-based advanced oxidation processes are regarded as effective methods for removing organic contaminants. However, current removal technologies are often unable to achieve satisfactory results due to the low concentrations and high stability that are frequently characteristics for many types of organic contaminants. To improve the efficacy of using sulfate radicals to remove organic contaminants, we designed metal–organic frameworks (Fe(II)-MOFs) modified with enrichment and specific recognition of molecular imprinting layer (Fe(II)-MOFs@MIP). Using dibutyl phthalate (DBP) as the model target contaminant, the selectivity coefficient towards DBP was 7.28 for adsorption and 4.46 for catalytic degradation of Fe(II)-MOFs@MIP, which is excellent for most of the imprinted material. Additionally, we achieved the accurate recognition (169.25 μg × g −1 ) and efficient degradation (0.071 min −1 ) of DBP reducing levels to 100 μg × L -1 . UV–vis analysis confirmed that specific recognition of DBP was mainly through hydrogen bonding and π-π interaction, while in-situ Raman and radical quenching experiments showed that the imprinting layer could accurately adsorb and produce the spatial confinement effects on target contaminants, thereby reducing the transfer distance of free radicals. As a result, we show that Fe(II)-MOFs@MIP can achieve efficient targeted degradation of DBP, opening up a new avenue for the removal of this and other highly stable organic contaminants present at low concentrations in environmental systems.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 8
·1-10
·
IF 5.833
Liu Jia Li,Ma Yu Chan,Yang Tong,Hu Rong,Yang
Yun Hui
An ultrasensitive electrochemical sensor has been constructed for the detection of single nucleotide polymorphisms (SNPs) based on DNA-functionalized Cd-MOFs-74 as cascade signal amplification probe under enzyme-free conditions. Interestingly, the introduction of an auxiliary probe did not disturb the detection of SNP targets, but could bind more Cd-MOFs-74 signal elements to enhance the different pulse voltammetry electrochemical signal 2~3 times as compared to sensing system without auxiliary probe, which obviously improves the sensitivity of the proposed sensor. Experimental results taking p53 tumor suppressor gene as SNP model demonstrated that the proposed method can be employed to sensitively and selectively detect target p53 gene fragment with a linear response ranging from 0.01 to 30 pmol/L (detection limit of 6.3 fmol/L) under enzyme-free conditions. Utilizing this strategy, the ultrasensitive SNP electrochemical sensor is a promising tool for the determination of SNPs in biomedicine.
Graphical Abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Zhenlin Ma,Rong Zheng,Yu Liu,Yulong Ying,Weidong Shi
Recently, carbon nanotubes (CNT)-based interconnected architectures exhibit promising prospects in supercapacitors due to their flexibility and high electrical conductivity. Herein, a three-dimensional (3D) interconnected network structure combined with conductive carbon nanotubes interpenetrating MOFs-derived Co-Ni-S composite spheres (Co-Ni-S/CNTs) was synthesized. Such 3D interconnected architecture significantly leads to a favorable electronic structure, fast charge-transfer capacity, and more pseudocapacitive. The Co-Ni-S/CNTs-based hybrid electrode exhibits an extraordinary specific capacitance of 540.6C g −1 at 1 A g −1 and competitive rate performance (capacity retention rate of 69.9% when the current density increases to 10 times). Subsequently, a hybrid supercapacitor is assembled using Co-Ni-S/CNTs as the positive electrode and commercial activated carbon as negative electrode. The device delivers a high energy density of 63.5 W h kg −1 at 800 W kg −1 and keeps 83.0% initial capacitance retention after 10,000 cycles. The encouraging performances demonstrate the significant contribution of the 3D interconnected architecture for the future energy storage.
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ACS ES&T Engineering
·
2021
·
IF 0
Xuedong Du,Wenyang Fu,Pei Su,Linlan Su,Qizhan Zhang,Jingju Cai,Minghua Zhou
A Fe0/Cu0-based bimetallic submicro-particle core with porous carbon (PC) shell hybrid rods, i.e., core–shell structured FeCu@PC-800/6, was successfully fabricated from the mixture of MIL-88B(Fe) and Cu-BDC through pyrolysis at 800 °C for 6 h and employed as novel heterogeneous electro-Fenton (Hetero-EF) catalysts to remove sulfamethazine (SMT). A trace dose catalyst (25.0 mg L–1) could achieve efficient catalytic activity (turnover frequency (TOFd), 3.92 L g–1 min–1) due to the synergy of catalytic reactivity among iron, copper, and PC, possessing the pseudo-first-order rate for SMT removal that was 3.27-foldsand 4.08-fold of the Fe@PC-800/6/Hetero-EF and Cu@PC-800/6/Hetero-EF process, respectively. According to experiments and density functional theory (DFT) calculations, Hetero-EF reactions enhanced by internal-microelectrolysis (IME) were proposed, in which Cu0 promoted the electrons transfer of Fe0 to PC while the introduced Cu+ could promote the decomposition of H2O2 and the cycle of Fe3+/Fe2+. A possible mechanism and SMT degradation pathway were suggested for this Hetero-EF process, confirming that the surface-bound hydroxyl radical played a major role. This FeCu@PC-800/6 catalyst was cost-effective and could be reused after thermal treatment in H2, demonstrating super efficiency for organic contaminants degradation by EF process.
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ULTRASONICS SONOCHEMISTRY
·
2020
·
IF 6.513
Nannan Geng,Wei Chen,Hang Xu,Mingmei Ding,Tao Lin,Qiangshun Wu,Lei Zhang
In this work, as a new strategy, ultrasound/H 2 O 2 /MOF system was firstly applied by environmental-benign Fe-MOFs (MIL-53, MIL-88B and MIL-101) for tetracycline hydrochloride removal. The synthetic Fe-MOFs were characterized by XRD, FTIR, SEM, XPS, N 2 sorption-desorption isotherms and CO-FTIR. MIL-88B demonstrated the best catalytic performance because of its highest amount of Lewis acid sites. Influencing factors, contrast experiment, and corresponding dynamics were carried out to obtain the best experimental conditions and reaction system. Under optimal conditions ([Tetracycline hydrochloride] = 10 mg/L, [MIL-88B] = 0.3 g/L, [H 2 O 2 ] = 44 mM, [ultrasound power] = 60 W, and pH = 5.0), the-first-order kinetic rate constant k was calculated to be 0.226 min −1 , higher than the simple combination of the ultrasound system (0.004) and MIL-88B/H 2 O 2 system (0.163), indicating the importance of synergistic effect between ultrasound and Fenton reaction. EPR test and quenching experiment proved that ·OH is mainly responsible for tetracycline hydrochloride removal. The major reaction path is the adsorption and decomposition of H 2 O 2 by coordinative unsaturated iron sites on Fe-MOF, but it is not the only path. The direct decomposition of H 2 O 2 and the cavitation effect caused by ultrasound also contribute to the generation of OH.
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CHEMICAL PHYSICS
·
2021
·
IF 2.348
Xingchang Tang,Yongwei Luo,Zhijian Zhang,Wanwu Ding,Dexue Liu,Jingchuan Wang,Li Guo,Ming Wen
The high surface areas and tunable properties of Zr-based MOFs make them as attractive materials for gas capture, storage, and separation. In this work, UiO-66, one kinds of Zr-based MOFs, functionalized by single or binary –NO 2 and –NH 2 groups are synthesized. Water adsorption ability and hydrophilicity of UiO-66 and functionalized UiO-66-X were investigated. It is found that surface area of UiO-66 is decreased after introducing functional groups, while hydrophilicity of UiO-66 increased after functionalized with –NO 2 and –NH 2 . Therefore, after balance the effects of surface area and hydrophilicity, UiO-66-NH 2 shows the best water adsorption propriety.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 6
·1699-1707
·
IF 5.721
Yu-Ping Xu,Zhi-Qiao Wang,Hong-Zi Tan,Kai-Qiang Jing,Zhong-Ning Xu,Guo-Cong Guo
CO esterification to dimethyl carbonate (DMC) is an attractive route, although the catalyst is the main problem restricting the industrialization of this route. Supported palladium catalysts have been often used for this route. However, the effect of the support is not always clear. In this work, we firstly introduced three metal–organic frameworks (MOFs) materials as catalyst supports, namely UiO-66, MIL-101 and MOF-5, and studied the effect of Lewis acid sites in the MOFs supports on the catalytic activity and selectivity for CO esterification to DMC. Interestingly, the Pd(II)/UiO-66 catalyst exhibits superior catalytic performance to the other catalysts, with 87.9% CO conversion and 98.5% DMC selectivity due to the abundant Lewis acid sites in UiO-66. It was proven that UiO-66 with more defects would have a large number of Lewis acid sites, and the catalytic performance was positively correlated with the number of Lewis acid sites in MOFs supports, which can be demonstrated by characterization by NH3-TPD, pyridine-IR, XPS and in situ DRIRS. The current work not only revealed the relationship between the Lewis acidity of the support and catalytic performance, but also promotes the development of practical catalysts for CO esterification to DMC.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 2
·1-9
·
IF 6.232
Hu Peng,Zhu Xiaoming,Luo Xiaohui,Hu Xiaofeng,Ji Liudi
The authors describe a novel electrochemical determination method for bisphenol A (BPA) based on the electrosynthesised Cu-BTC (H 3 BTC: trimesic acid) films. Using H 3 BTC as the ligand, Cu(NO 3 ) 2 as the precursor of copper ions, and triethylamine hydrochloride (Et 3 NHCl) as the probase source, Cu-BTC films were directly deposited on glassy carbon electrode (GCE) surface via cathodic electrochemical reduction under −1.30 V. Considering the electrocatalytic activity of metal center Cu 2+ , Cu-BTC films were applied to construct the electrochemical determination platform for BPA. Chronocoulometry and electrochemical impedance spectroscopy were used to study the signal enhancement mechanism. The determination conditions were optimized. As a result, a sensitive electrochemical method was constructed for BPA. The peak currents, best measured at voltage of 0.496 V vs. SCE (KCl saturated calomel reference electrode), increase linearly in the range from 5.0 to 2000 nM. The value of determination limit is 0.72 nM. The proposed method was successfully applied to determine BPA in spiked urine, spiked waste water samples and plastic products. The results were in good agreement with those obtained for the same samples by high-performance liquid chromatography (HPLC).
Schematics for the construction of electrochemical determination for bisphenol A.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Qi Yang,Dan Chen,Libing Chu,Jianlong Wang
In present work, we studied a novel Fe/C nanomaterial fabricated using Fe-based metal organic frameworks (MOFs) as precursors through thermal pyrolysis to catalyze gamma irradiation-induced degradation of antibiotics, cephalosporin C (CEP-C) and sulfamethazine (SMT) in aqueous solution. The MOFs-derived Fe/C nanomaterials (DMOFs) had the regular octahedrons structure of MOFs and contained element C, Fe and O, while Fe° with a fraction of Fe 3 O 4 and Fe 2 O 3 were identified. Results showed that DMOFs addition could accelerate the generation of OH during gamma irradiation, while the intermediates of bonds cleavages of antibiotic molecules and OH addition were identified. DMOFs were more effective to improve the decomposition of antibiotic having the higher adsorption capacity like SMT. The degradation rate of CEP-C and SMT increased by 1.3 times and 1.8 times, and TOC reduction at 1.0 kGy reached 42 % and 51 %, respectively by gamma/DMOFs treatment, while only 20.2 % (CEP-C) and 4.5 % (SMT) of TOC reduction were obtained by γ-irradiation alone. The crystal structure, functional groups and magnetism of DMOFs changed slightly after gamma irradiation, which made it possible to be reused. DMOFs were promising to enhance the degradation of antibiotics during gamma irradiation.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Qi Zhang,Tao Wei,Jiahao Lu,Cheng Sun,Yanyan Zhou,Mengting Wang,Ye Liu,Beibei Xiao,Xiangyun Qiu,Shoudong Xu
All solid-state lithium-ion batteries (ASSLBs) are thought to benefit from using solid composite electrolytes (SCEs) to increase their energy density and safety. In this study, we firstly introduce the PVB additives to SCEs and prepared a SCE composed of a mixture of nanostructured MOFs (UiO-67), PVDF-HFP, PVB, and LiTFSI. Electrochemical characterizations of the SCEs (EIS, LSV, CV and battery test) were also conducted. The SCE UBP-2 (PVB:PVDF-HFP = 1:10) shows a high lithium-ion transference number (t Li + =0.72) and good ionic conductivity (3.27×10 −4 S cm −1 at 60 °C). A symmetric Li cell with SCE UBP-2 can be continuously cycled at 0.1 mA cm −2 for more than 2500 h without experiencing a short circuit. The full cell (LiFePO 4 /UBP-2/Li) also maintained a high reversible discharge capacity of 154.9 mAh g −1 at 0.1C after 200 cycles at 60 °C. At 3C, a capacity of around 100 mAh g −1 was also achieved. This work might help to enhance the development of the forthcoming all solid-state batteries.
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DESALINATION
·
2023
·
IF 9.9
Jingjing Zhen,Faguang Ma,Rongxin Lin,Ming Yan,Yilin Wu
We present the design and fabrication of high-performance molecularly imprinted membranes (MIMs) using a UiO-66@PDA framework with densely imprinted sites for the targeted adsorption of artemisinin (ATSN). UiO-66@PDA was synthesized by modifying polydopamine with metal-organic frame (MOF) that contain Zr(IV) ions. The unique UiO-66@PDA structure exhibits an excellent specific surface area and strong binding abilities towards ATSN due to the abundant phenolic , quinone , and amino functional groups. The addition of SiO 2 nanoparticles further enhanced the stability of the hybrid membrane during the adsorption process, and the preparation of inorganic-organic hybrid membranes (k-SUPCP-IMs) involves the use of a click chemistry-based imprinted polymer that takes advantage of the heterogeneous structure of the material. This process highlights the importance of different building blocks and functional reactions in controlling the morphology and porosity of porous organic polymers . The results showed satisfactory rebinding ability (40.07 mg g −1 ) and superselective ( β ATMT/ATSN = 7.87, β DDTM/ATSN = 8.26, β ATST/ATSN = 6.40). It was noteworthy that the unique electrostatic interaction between SiO 2 and the imprinted molecules provides optimal conditions for the formation of high-affinity binding sites , thereinto, the creation of additional active sites played a critical role in improving the sensitivity of MIMs.
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