JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiajun Yu,Xiao Wang,Yan Wang,Xiaofeng Xie,Haijiao Xie,Nat Vorayos,Jing Sun
The removal of indoor/outdoor toluene by photocatalysis has drawn much attention due to its low energy consumption and easy availability. However, light inevitably generates heat, and pollutants desorb from catalysts as the temperature rises, which is not beneficial to degradation. Contrast to the frequently occurred phenomena, we firstly found that the adsorption capacity of UiO-66 (Zr) on toluene increased with increasing temperature as adsorption isotherms and in-situ Fourier transform infrared spectra (in-situ FTIR) showed. The optimum temperature was 30 °C. This stage in which adsorption capacity was positively correlated with temperature was called heating-induced adsorption, which achieved a toluene removal efficiency of 69.6 %. By density functional theory (DFT) calculations and changing the metal centers and organic ligands of UiO-66 (Zr) respectively, we disclosed that the heating-induced adsorption was mainly related to the π-π stacking interaction of MOF ligands and toluene. The analysis of samples before and after adsorption showed that the interaction between UiO-66 (Zr) and adsorbed toluene facilitated the charge transfer and prolonged the carrier lifetime, leading to the increase of hydroxyl radicals (•OH) in photocatalysis. Therefore, a synergistic effect between heating-induced adsorption and photocatalysis was proposed by analyzing the adsorption of toluene on UiO-66 (Zr) in detail. This work provided new viewpoint to understand the role of concomitant heat contributed to the adsorption and degradation of toluene during photocatalysis.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Pengfei Li,Yingbo Chen,Fan Xiao,Ming Cao,Jingyu Pan,Jingfeng Zheng,Ke Zhao,Hao Li,Xianglin Zhang,Yuanyuan Zhang
The performance of proton exchange membranes (PEMs) can be enhanced by creating continuous proton conduction channels. In this work, PVP-UiO-66-NH-SO 3 H nanoparticles (PUNSNPs) were prepared and filled into sulfonated poly (ether ether ketone) (SPEEK) to fabricate PUNSNPs/SPEEK composite PEMs. To further improve the performance of the PEMs, phosphoric acid (PA) was doped and a continuous nanopore network was formed in PA/PUNSNPs/SPEEK porous PEMs due to the dissolution of PUNSNPs. The PA/PUNSNPs/SPEEK porous PEMs have high PA uptake ratio (96%–117 %) and dimensional stability thanks to the anchoring effect of the nitrogen-containing heterocyclic ring on the PVP chains. The acid-base pairing interaction between the chains (residual ligands from PUNSNPs) inside the unique continuous nanopore structure allows PA/PUNSNPs/SPEEK = 20 % porous PEMs to have the highest proton conductivity of 0.350 S cm −1 (80 °C/100 % RH). Furthermore, the PA/PUNSNPs/SPEEK porous PEMs retained PA up to more than 80 % (80 °C, 40 % RH, 7 days). Similarly, PA/PUNSNPs/SPEEK = 20 % porous PEMs immersed in deionized water for 45 days were able to maintain a proton conductivity of more than 83 %. Finally, PA/PUNSNPs/SPEEK porous PEMs have low methanol permeability . Thus, this study provides a new method for the preparation of porous PEMs with a continuous nanopore network structure and excellent performance.
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International Journal of Minerals Metallurgy and Materials
·
2023
·Vol. 30
·期 10
·1897-1905
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IF 4.8
Wei Tao,Zhang Qi,Wang Sijia,Wang Mengting,Liu Ye,Sun Cheng,Zhou Yanyan,Huang Qing,Qiu Xiangyun,Tian Fang
All solid-state electrolytes have the advantages of good mechanical and thermal properties for safer energy storage, but their energy density has been limited by low ionic conductivity and large interfacial resistance caused by the poor Li + transport kinetics due to the solid–solid contacts between the electrodes and the solid-state electrolytes. Herein, a novel gel polymer electrolyte (UPP-5) composed of ionic liquid incorporated metal-organic frameworks nanoparticles (IL@MOFs) is designed, it exhibits satisfying electrochemical performances, consisting of an excellent electrochemical stability window (5.5 V) and an improved Li + transference number of 0.52. Moreover, the Li/UPP-5/LiFePO 4 full cells present an ultra-stable cycling performance at 0.2C for over 100 cycles almost without any decay in capacities. This study might provide new insight to create an effective Li + conductive network for the development of all-solid-state lithium-ion batteries.
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Small
·
2023
·Vol. 20
·期 7
·2306820
·
IF 13.3
Zheng Zheng,Bing Wang,Zhuo Li,Hong Hao,ChaoYang Wei,WenYu Luo,LinYu Jiao,Sheng Zhang,Bo Zhou,XiaoXun Ma
Constructing heterojunction of supramolecular arrays self-assembled on metal–organic frameworks (MOFs) with elaborate charge transfer mechanisms is a promising strategy for the photocatalytic oxidation of organic pollutants. Herein, H 12 SubPcB–Br (SubPc–Br) and UiO-66 are used to obtain the step-scheme (S-scheme) heterojunction SubPc–Br/UiO-66 for the first time, which is then applied in the photocatalytic oxidation of minocycline. Atomic-level B–O–Zr charge-transfer channels and van der Waals force connections synergistically accelerated the charge transfer at the interface of the SubPc–Br/UiO-66 heterojunction, while the establishment of the B–O–Zr bonds also led to the directional transfer of charge from SubPc–Br to UiO-66. The synergy is the key to improving the photocatalytic activity and stability of SubPc–Br/UiO-66, which is also verified by various characterization methods and theoretical calculations. The minocycline degradation efficiency of supramolecular SubPc–Br/UiO-66 arrays reach 90.9% within 30 min under visible light irradiation. The molecular dynamics simulations indicate that B–O–Zr bonds and van der Waals force contribute significantly to the stability of the SubPc–Br/UiO-66 heterojunction. This work reveals an approach for the rational design of semiconducting MOF-based heterojunctions with improved properties.
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Yuanyuan Niu,Jianfeng Zhou,Haohong Lai,Qing Zhou,Shumei Wang,Haiyun Zhai
A sensitive and selective electrochemical sensor for sensing 4-nitroquinoline N-oxide (4-NQO) by differential pulse voltammetry was designed. Poly L-histidine (P-L-his) composite and metal-organic framework UiO-66 (Zr) modified electrode was used as the working electrode which had large specific surface area, mesoporous structure and excellent conductivity. Unlike most modification methods, UiO-66 was electrodeposited in this study. Compared with drop coating, electrodeposition proceeds efficiently under mild conditions and often requires shorter time. FTIR, EDX, TEM, SEM and electrochemical assay were used to characterize the prepared materials and modified electrodes. After that, some experimental conditions like electro-polymerization time, deposition time, pH and scan rate were also improved and optimized separately. At the UiO-66/P-L-his-modified glassy carbon electrode, a good linear relationship between 4-NQO concentration and its peak current was obtained under the best conditions in a wide range from 0.2 to 50.0 μM, and the limit of detection (S/N = 3) was 66.7 nM. Moreover, multiple experiments elucidated that the as-synthesized sensor could be applied to detect 4-NQO in actual samples, and the recoveries results obtained were satisfactory.
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Applied Materials Today
·
2021
·
IF 10.041
Kai Wang,Shuaishuai Ding,Lijuan Zeng,Jingrong Zhou,Yuhua Cao,Jiaqian Wu,Lu Lu,Xiu-wu Bian,Gan Tian
Hypoxia-acquired radioresitance is considered to be a major factor responsible for the clinical failure of radiotherapy. Carbonic anhydrase IX (CA IX), a hypoxia-induced cell-surface enzyme involved in pH regulation of hypoxic solid tumors, has been acknowledged as a desirable target for cancer therapy. Herein, we developed a dual exogenous/endogenous CA IX inhibition strategy using core/satellite-like metal-organic framework (UiO-66)/gold nanoparticles (Au NPs) nanohybrids as a therapeutic platform for hypoxia-relief enhanced RT of triple negative breast cancer. The UiO-66 matrix supported the Au NPs generation in situ and would decompose inside tumor cells by the high-concentration phosphates to release p -phthalic acid (PTA), a original building skeleton of the UiO-66 matrix, to inhibit CA IX, while the decorated Au NPs served as radiosensitizers to potentiate the sensitivity of tumor cells to X-ray and yet provided active sites for CA IX antisense oligonucleotide (ASO) loading via formation of stable Au-S bond to knockdown CA IX. The dual inhibitory manner, exogenous inhibition from PTA and endogenous inhibition from CA IX ASO, largely alleviated the hypoxia-induced resistance and synergized with Au NPs-mediated radiosensitization to afford super therapeutic outcome in vitro and in vivo , supporting the feasibility of our synergistic RT strategy in hypoxic tumor management.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mengmeng Zhang,Qian Sun,Yuejiao Wang,Weijun Shan,Zhenning Lou,Ying Xiong
Reported powdery adsorbents with poor adsorption efficiency and stability make it imperative to develop novel materials to extract gallium ions (Ga(III)) from effluents. Herein, UiO-66-NH 2 -based mixed matrix membranes (TPU/0.1THB/U6N-1.5 MMMs) via electrospinning is firstly reported for separation and recovery of Ga(III). TPU/0.1THB/U6N-1.5 MMMs efficiently overcomes multiple bottlenecks of powder UiO-66-NH 2 , including poor stability, reusability and adsorption capacity. Its maximum adsorption for Ga(III) is 96.18 mg·g −1 at pH 10.0. It has superiority in selective adsorption of Ga(III) from Al(III), Cu(II), Zn(II), Co(II) coexistence solution. Adsorption capacity of TPU/0.1THB/U6N-1.5 for Ga(III) reaches more than 80% after 9 cycles. Specially, it still retains excellent mechanical strength, flexibility and structural integrity after 12 h filtration, or after 9 adsorption-desorption cycles, even soaked in 5 mol·L -1 HCl for a week. TPU/0.1THB/U6N-1.5 MMMs also improves the problem of low water flux. TPU/0.1THB/U6N-1.5 with high MOFs loading possess high water flux of 382.2 L·m −2 ·h −1 with a permance of 382.2 L·m −2 ·h −1 ·bar −1 and rejection rates of 90% for Ga(III). The main adsorption mechanism of TPU/0.1THB/U6N-1.5 is based on the chelation between phenolic hydroxyl groups of MMMs and Ga(III) at pH 10.0. Overall, the as-prepared TPU/0.1THB/U6N-1.5 has potential for water treatment through the process of membrane adsorption.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhou Zhou,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu
In order to fix the photocatalyst and enhance the efficiency of NO degradation, a three-dimensional (3D) g-C 3 N 4 /NH 2 -UiO-66-rGO (CN/NU6-rGO) aerogel was devised and fabricated via solvothermal reaction and boiling-water bath. Herein, a type-II heterojunction was formed at CN/NU6 composite, and then, the composite was coupled with rGO. The resulting material significantly enhanced the nitric oxide (NO, 600 ppb) removal efficiency under visible-light irradiation. Optimizing the content of CN and rGO to a suitable mass ratio can increase the removal efficiency by 65.4%, which is 2.34 times that of pure NU6. This result is attributed to the construction of type-II heterojunction and the charge transport properties of rGO. The involvement of rGO not only provided extra pathways for charge transfer to prevent electron–hole pairs from recombining, but also fixed the catalyst. Moreover, the hybrid aerogel excellently reduced the harmful by-product NO 2 . Cycling experiments, along with transient photocurrent response measurements, verified that CN/NU6-rGO had excellent potential for recyclable and sustainable. This work might shed light on the construction of suitable photocatalytic systems with significant improvement of NO removal and convenient storage of catalyst.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Haoji Jiang,Wenxiong Shi,Qiang Liu,Heyun Wang,Jialu Li,Chunlin Wu,Yingchun Li,Zhong Wei
In order to investigate the effects of MOFs by altering ligands with various functional groups on separation selection in pervaporation dehydration, three hydrophilic UiO-66-X nanoparticles were respectively synthesized and blended into poly (vinyl alcohol) matrix to fabricate water-selective membrane for ethanol dehydration via PV technology. Both the experimental and molecular simulation results confirmed the UiO-66-X counterbalancing factors of enhanced polarity and suitable pore size gave rise to the optimal performance in ethanol dehydration. The PV performances could be tuned by the type and quantity of functional groups carried by UiO-66-X nanoparticles. As a result, the pore aperture of UiO-66-(COOH) 2 nanoparticles provided continuous channel for water diffusion, and water molecules could also be activated attributed to the strong interaction between the UiO-66-(COOH) 2 nanoparticles and water molecules which enhanced the penetration and diffusion of water molecular in hybrid membrane to increase the water flux. The optimized hybrid membranes with UiO-66-(COOH) 2 loading of 8 wt% exhibited the total flux of 979 ± 7 g/(m 2 ·h) and a separation factor of 2084 ± 21.
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FUEL PROCESSING TECHNOLOGY
·
2020
·
IF 4.982
Cheng Wang,Ai-Rong Li,Yu-Ling Ma
The synthesis of highly efficient and stable catalysts for oxidative desulfurization is still a challenging task. Herein, a composite material (HPMo@UiO-66) of phosphomolybdic acid (HPMo) encapsulated in the metal-organic framework UiO-66 with missing-linker defects was prepared via a one-pot hydrothermal method . A series of as-synthesized catalysts were systematically characterized by XRD , FT-IR, SEM , BET, TGA , XPS , UV–vis and PL . Through oxidative desulfurization experimental evaluations, the catalyst 0.5-HPMo@UiO-66-D with defects shows the superior catalytic oxidative desulfurization performance and high reusability . 0.5-HPMo@UiO-66-D is able to completely remove DBT in the model fuel in 60 min, and the reaction system can be recycled 10 times with a high activity. In addition, the kinetics and the activation energy of the oxidative desulfurization were studied.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Yawen Wu,Xiaolong Chen,Xiaogang Luo,Mei Yang,Changjun Hou,Danqun Huo
Carcinoembryonic antigen (CEA) is a key serum tumor marker which is overexpressed in all types of adenocarcinomas. Therefore, establish the ultrasensitive, accurate and rapid method for CEA detection is essential for reducing the mortality of cancer. Here, a bimetallic organic framework Cu/UiO-66 was synthesized through the simple two-step hydrothermal method and used to construct a “fluorescence turn-on” analytical method for CEA detection. Cu/UiO-66 can adsorb CEA aptamers modified with FAM (CEA/FAM-Apt) and take place photoinduced electron transfer (PET) between Cu/UiO-66 and FAM, resulting in the fluorescence of the FAM is quenched. When CEA is present, CEA and CEA/FAM-Apt are tightly combined, making CEA/FAM-Apt far away from the Cu/UiO-66 surface. As a result, the fluorescence intensity of the system was significantly restored. Under optimal conditions, the proposed “fluorescence turn-on” method can detect CEA as low as 0.01 ng mL −1 in a range of 0.01–0.3 ng mL −1 . Besides, this analytical method owns good selectivity , reproducibility and serum applicability, which provides a new platform for the direct detection of clinical diagnosis-related markers.
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Mingying Ma,Tianhao Wu,Zhian Hu,Gongwei Sun,Sichun Zhang
High-throughput sample preparation is important in clinical mass spectrometry (MS) analysis. In this work, we developed a method by coupling Nano-ESI-MS with magnetic SPE using a MOF material, Fe 3 O 4 @UiO-66, as sorbent for simultaneous determination of testosterone (T) and androstenedione (4-AD) in serum samples. The proposed method presented good linearity in the range of 0.1–5 μg/L and the recoveries of serum samples were 90.7%-110.0% and 101.7%-108.7% for T and 4-AD, respectively. The results indicated that the Fe 3 O 4 @UiO-66 is an ideal sorbent for androgens extraction and the method is reliable for high-throughput quantitation of T and 4-AD in clinical applications.
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