CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Jie Yin,Wendi Fu,Jinrui Zhang,Xinyu Liu,Xinmiao Zhang,Chao Wang,Jing He,Wei Jiang,Hongping Li,Huaming Li
Porous ionic liquids are a novel category media that possesses the catalytic activity of porous solids and the extraction property of ionic liquids. Herein, a new type of porous ionic liquids (denoted as UiO-66-T3PILs) was fabricated by employing UiO-66(Zr) as the pore generator and the ionic liquid ([P 6,6,6,14 ][NTF 2 ]) as the size-excluded solvent for extraction coupled catalytic oxidative desulfurization (ECODS) using hydrogen peroxide (H 2 O 2 , 30 wt%) as an oxidant. Furthermore, several significant reaction parameters such as UiO-66 loading in porous ionic liquids, reaction temperatures, molar ratio of H 2 O 2 /DBT and sulfide species as well as recyclability were investigated in detail. As UiO-66-T3PILs exhibited higher efficiency (95.3%) than the summarized efficiency of UiO-66 and [P 6,6,6,14 ][NTF 2 ], there did exist a synergistic effect between the UiO-66(Zr) moiety and the ionic liquid moiety in UiO-66-T3PILs. With the assistance of density functional theory calculations, a possible mechanism was proposed that aromatic sulfur compounds in the oil phase were first extracted into ionic liquids moiety phase via C-H···π interactions and then rapidly oxidized by OH radicals in the presence of the UiO-66 moiety. This work will pave the way for the rational design of novel porous ionic liquids towards catalysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Wenwen Li,Chuncai Zhou,Chen Li,Wenrui Zhu,Jiaqian Shi,Guijian Liu
To alleviate the supply–demand contradiction of gallium metal (Ga), this study reports a method of preparing 2-CNT/UiO-66-NH 2 composite materials by combining carbon nanotubes (CNTs) with UiO-66 series metal–organic frameworks (MOFs) to improve the recovery and utilization efficiency of Ga in solution. The adsorbent material is used for selective adsorption and recovery of Ga in aqueous solutions. The physical properties of the composite adsorbent, such as morphology, structure, and elemental composition, were explored by analyzing the surface characteristics of the samples. The impacts of variables like the amount of adsorbent used, time, solution concentration, pH value, and coexisting ions on adsorption efficiency were explored during the experiment. The results indicate that ion exchange and chelation play a major role in the adsorption of Ga by 2-CNT/UiO-66-NH 2 , and Ga ions can be separated and recovered from the mixed solution through selective adsorption. At 313 K and pH = 8, the greatest amount of adsorption is 925.44 mg/g, and the rate at which it is absorbed can reach 99% when the adsorption time is only 1 h. The hybrid absorbent generally has a high adsorption efficiency and good selective adsorption performance for Ga, providing more efficient and economical technical assistance for the future recovery and exploitation of Ga supplies.
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Catalysts
·
2023
·Vol. 13
·期 7
·1073
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IF 3.9
Kaiwen Yuan,Bo Gong,Chundong Peng,Yanmei Feng,Yingmo Hu,Kai Chen,Daimei Chen,Derek Hao
Cr(VI) is a common heavy metal pollutants present in the aquatic environment, which possess toxic and carcinogenic properties. In this study, a solvothermal reaction was used to prepare porphyrin (TCPP)-modified UiO-66-NH2(UNT). The UNT integrated adsorption and photocatalytics in the application for dealing with Cr(VI). The photocatalytic reduction activities of UNT for Cr(VI) were investigated under visible light illumination. We found that the TCPP doping amount of 15 mg UNT (15-UNT) had a 10 times higher reduction rate of Cr(VI) than pristine UiO-66-NH2. The optimal 15-UNT photocatalyst demonstrated the highest photocatalytic activity, and Cr(VI) was completely removed within 80 min. In addition, the introduction of porphyrin not only enhanced the absorption of light but also enabled the transport of photogenerated electrons from porphyrin to UiO-66-NH2, which promoted the separation of charge carriers. Furthermore, the effects of factors such as porphyrin content, pH and light source on the photocatalytic reduction performances of UNT were also explored. Overall, this work presented a possible relationship between the crystal structures and the performance of UNT.Keywords:photocatalytic reduction;porphyrin;UiO-66-NH2;hexavalent chromium
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RESEARCH ON CHEMICAL INTERMEDIATES
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2023
·Vol. 49
·期 10
·4257-4274
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IF 3.3
Cao Wenbo,Ren Haitao,Cai Chaochen,Li Dashuai,Li Tingting,Lou Chingwen,Lin Jiahorng
Photocatalysis is a promising technology for wastewater treatment. It is a key problem to develop photocatalytic materials that can efficiently remove tetracycline (TC) under weak light intensity. This article synthesized the UiO-66-NH 2 /Bi 2.15 WO 6 heterojunction using a solvothermal method, and its specific surface area increases by 2.1 times relative to Bi 2.15 WO 6 , endowing good adsorption capacity for TC. Compared with Bi 2.15 WO 6 , the heterojunction effectively improves the separation of electrons and holes and enhances the photocatalytic performance. Under weak light intensity (4 mW cm −2 ), the removal percentage of 50 mg L −1 TC can reach 78.0%, attributing to a synergistic effect between adsorption and photocatalysis. The free radical capture experiment showed that TC was photodegradation mainly under the action of hole (h + ) and superoxide radical (·O 2 − ). Finally, through LC/MS analysis, it is inferred that TC is degraded into H 2 O and CO 2 after a series of reactions such as deamination, dehydroxylation, amide bond breaking and ring opening. This study provides insights for the synthesis of more powerful photocatalysts for TC removal.
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Journal of Inorganic and Organometallic Polymers and Materials
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2022
·Vol. 33
·期 2
·328-336
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IF 3.518
Gao Feifei,Wu Feiyang,Zhang Xianyang,Jiang Bowen,Li Qizhong
In this paper, zirconium-based MOF (Zr-MOFs) materials, namely UIO-66, UIO-66-NH 2 , GMA-UIO-66 and NB-UIO-66, were selected as fillers to enhance the mechanical properties of polydicyclopentadiene (PDCPD) nanocomposites, and Zr-MOFs/PDCPD nanocomposites were prepared by in situ polymerization. The functional groups and morphology of Zr-MOFs were characterized by Fourier transform infrared (FT-IR), X-ray diffraction (XRD) and field emission scanning electron microscopy (SEM). The mechanical properties of Zr-MOFs/PDCPD composites were studied by tensile toughness, notched impact strength and bending strength test. Furthermore, the optimum Zr-MOFs loading was determined. The results show that when the mass fraction of NB-UIO-66 is 0.4%, the composites’ tensile toughness, flexural strength, impact strength and heat distortion temperature (HDT) are simultaneously increased by 47.3%, 37.5%, 119.4%, and 59.2% respectively, compared with the pure PDCPD, which synergistically enhances the mechanical properties. Graphical Abstract
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Qingyuan Song,Xueling Shan,Liyin Bu,Anna Dai,Ding Jiang,Wenchang Wang,Hiroshi Shiigi,Zhidong Chen
A highly efficient electrochemiluminescence resonance energy transfer (ECL-RET) aptasensor was constructed for ultrasensitive detection of diethylstilbestrol (DES). The composite composed of silver orthophosphate and zirconium-based metal–organic frameworks (Ag 3 PO 4 -UiO-66) was prepared as a sensing platform for aptasensor incubation. Ag 3 PO 4 , a novel ECL donor, whose emission could be obviously enhanced through loading on UiO-66. Particularly, the composite of Ag 3 PO 4 -UiO-66 could minimize the aggregation of Ag 3 PO 4 , which provided a novel possibility for the construction of high ECL efficiency sensors. UiO-66 presented ultrahigh surface area to improve the loading capacity of Ag 3 PO 4 and DES-specific aptamer. Notably, Ag 3 PO 4 with superb catalytic properties could immobilize DES aptamer via Ag–NH 2 bond and further ensured the distance between the ECL donor and the energy receptor. To design a novel ECL-RET system, GO nanosheets were synthesized as a suitable ECL acceptor which could be fixed through electrostatic adsorption. Owing to the superior spectral overlap, GO could significantly quench the ECL emission of Ag 3 PO 4 . Under the optimal conditions, the constructed ECL-RET aptasensor showed a satisfactory response to DES in a linear range of 1.0 × 10 −14 ∼ 1.0 × 10 −8 M and the detection limit was 7.2 × 10 −15 M (S/N = 3). This paper not only developed a novel approach for environmental water quality monitoring but also offered more opportunities for building highly sensitive ECL-RET aptasensors.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 33
·e52810
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IF 3.057
Zhirong Hu,Jiayu Miu,Xiong-Fei Zhang,Mingmin Jia,Jianfeng Yao
UiO-66-NH 2 (Zr-based metal organic framework) is integrated into cellulose acetate (CA) to fabricate mixed matrix membranes (MMMs) through solvent-casting approach. To regulate the interfacial compatibility and suppress the non-selective voids, UiO-66-NH 2 with different particle sizes are investigated. The introduction of UiO-66-NH 2 provides additional pathways for gas molecules and renders the membrane with high CO 2 affinity, substantially augmenting the separation efficiency of UiO-66-NH 2 @CA composite membrane. By optimizing the particle size of UiO-66-NH 2 , the non-selective voids and the particle agglomeration can be effectively restricted. The optimum separation performance is obtained by U-100@CA membrane (UiO-66-NH 2 : 200 nm in size), exhibiting a CO 2 permeability of 168.8 Barrer with CO 2 /N 2 and CO 2 /CH 4 ideal selectivities of 40.2 and 51.3, respectively. The separation mechanism is ascribed to the presence of sufficient amine groups, the high CO 2 solubility of CA matrix, and superior inorganic–organic interfacial property.
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ENVIRONMENTAL TECHNOLOGY
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2022
·
IF 3.475
Tong Li,Caixia Cheng,Kaifeng Zhang,Jie Yang,Guangshuo Han,Xiuju Wang,Zhongpeng Wang,Liguo Wang
In this paper, the hydrophilic UiO-66-NH2 nanomaterial was synthesized by the solvent-thermal method and characterized. Then, UiO-66-NH2 was introduced into the casting membrane solution of cellulose acetate (CA) forward osmosis (FO) membrane, and CA/UiO-66-NH2 forward osmosis membrane was prepared by the phase inversion method. The optimum preparation conditions of CA/UiO-66-NH2 mixed matrix membranes were determined as follows: the content of UiO-66-NH2 was 0.4 wt%, the coagulation bath temperature was 35°C, the mixing temperature was 50°C and the heat treatment temperature was 50°C. FTIR, SEM, water contact angle and AFM were carried out on CA/UiO-66-NH2 forward osmosis membrane prepared under the best preparation conditions. Compared to the CA forward osmosis membrane, the permeability and selectivity of the CA/UiO-66-NH2 membrane were improved. The water flux and reverse salt flux of the CA/UiO-66-NH2 forward osmosis membrane reached 52.32 L/(m2·h) and 2.43 g/(m2·h), respectively. The permeability selectivity of CA membranes and CA/UiO-66-NH2 membranes did not change much during 180 min, indicating that the two membranes had good long-term stability. This study shows a potential advantage of UiO-66-NH2 as additives for improvement in the desalination performance of forward osmosis membranes.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 6
·2653-2661
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IF 3.925
Long Jin,Feng Liu,Jian-hua Wu,San-Jian Ma,Juan-Hong Li,Yong-Jing Tian,Xin Liu,Zi-Xia Lin
A novel improved Fenton system named MHACF-UiO-66(Zr) was constructed under normal temperature and pressure based on the reduction of FeIII accelerated by hydrogen. The regeneration of FeII was enhanced by Pd/UiO-66(Zr). The hydroxyl radical could be continuously generated using only trace level FeII. 10 mg L−1 4-chlorophenol could be thoroughly degraded in the initial conditions of 75 mL min−1 H2, pH 3, 20 mM H2O2, 2 g L−1 Pd/UiO-66(Zr) and 20 μM FeII. Moreover, the removal efficiency of 15 mg L−1 sulfamethazine could be maintained at least more than 94% under the same conditions. The activity of the solid catalyst could be maintained after 6 consecutive reaction cycles. This provides new insight for improving the inherent shortcomings of the Fenton reaction, which generates large amounts of iron sludge.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Zhimin Guo,Nan Li,Shixiang Zuo,Chenghong Qiang,Wei Zhan,Zhengping Li,Jiangquan Ma
Piezoelectric materials, which could collect and convert mechanical energy into electrical energy, have recently emerged as promising catalysts for pollutants removal sustainably. Unfortunately, it remains a challenge to enhance the intrinsic piezoelectric property of piezoelectric materials. Herein, for the first time, the polar molecule adenine was introduced as a linking agent in the synthesis process of Zr-based UiO-66 (denoted as AD-U) to enhance the structure asymmetry and piezoelectric properties of UiO-66. The piezoresponse force microscopy (PFM) and ferroelectric hysteresis loop demonstrated that AD-U catalyst exhibited significantly enhanced piezoelectric potential than UiO-66. Furthermore, a series of electrochemical characterization evidenced that AD-U displayed higher charge separation efficiency than UiO-66. As expect, the optimized AD-U shown promoted diclofenac sodium (DCF) piezoelectric degradation efficiency by harvesting stirring energy compared with pure UiO-66. The electron paramagnetic resonance (EPR) spectra and trapping agent experiments convinced that h + play the major role for destroying the DCF molecules. Moreover, three possible degradation pathways of DCF were put forward by DFT and liquid chromatography mass system (LC-MS). Our work offers a new pathway to enhance piezoelectric property of MOFs and extend the application of MOFs in the field of piezocatalysis.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Rui Duan,Hongjuan Wu,Jiahe Li,Zhaoxi Zhou,Weihua Meng,Lei Liu,Hongqiang Qu,Jianzhong Xu
Phosphor nitrile functionalized UiO-66-NH 2 /graphene (G-U-H) was prepared combined a green mechanochemical method and microwave-assisted rapid method to improve the fire safety of epoxy resin (EP). The scanning electronic microscopy, transmission electron microscope and X-ray diffraction results indicated that the G-U-H exhibited sandwich-like hybrid structure. And the -OH from graphene nanoplatelets and -NH 2 from UiO-66-NH 2 were grafted with hexachlorocyclotriphosphazene to form covalent bonds . The obtained flame retardant was added to the EP at a different content. The flame retardancy index and cure index of EP composites were calculated, and those of EP-3 were both good. The cone calorimetry test showed that the flame retardancy of EP was improved and the flame retardant mechanism is the combination of condensed phase and gas phase with the synergistic of P, N and other elements. The physical barrier of graphene nanoplatelets and the generated more stable and denser residual char in condensed phase can effectively cut off the heat and mass transmission. In gas phase, the non-flammable gases were generated to help reduce the heat released.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Yi Zhang,Di Liu,Zhaoli Wang,Junjian Yu,Yanyin Cheng,Wenjing Li,Zhe Wang,Hongzhe Ni,Yuchao Wang
For the reduction of bovine serum proteins from wastewater, a novel mixed matrix membrane was prepared by functionalizing the substrate material poly aryl ether ketone followed with carboxyl groups(C-SPAEKS) and then addition of amino-functionalized UiO-66-NH 2 (Am-UiO-66-NH 2 ). Amino-functionalization of UiO-66 was accomplished by melamine, followed by an amidation reaction to immobilize Am-UiO-66-NH 2 was immobilized on the surface of the membrane as well as in the pore channels, which enhanced the hydrophilicity of the membrane surface while increasing the negative potential of the membrane surface. This nanoparticle-loaded ultrafiltration membrane has good permeation performance with a pure water flux of up to 482.3 L·m –2 ·h –1 for C-SPAEKS/Am-UiO-66-NH 2 and a retention rate of up to 98.7% for BSA-contaminated solutions. Meanwhile, after several hydrophilic modifications, the flux recovery of BSA contaminants by this series of membranes was increased from 56.2% to 80.55% of pure membranes. The results of ultrafiltration flux time tests performed at room temperature showed that the series of ultrafiltration membranes remained relatively stable over a test time of 300 min. Thus, the newly developed mixed matrix membrane showed potential for high efficiency and stability in the wastewater treatment containing bovine serum proteins.
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