Journal of Inorganic and Organometallic Polymers and Materials
·
2021
·Vol. 31
·期 11
·4195-4208
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IF 3.543
Wang Lulu,Zeng Xiangrui,Wang Haiyan,Wang Yujia
Abstract A series of porous confined ionic liquid phosphotungstate were synthesized by encapsulated of N-(3-sulfopropyl)morpholinium phosphotungstate ([C 3 SO 3 Hnhm] 3 -PW 12 O 40 ) into MIL-101. Then the aforementioned porous confined ionic liquid phosphotungstate as heterogeneous catalyst will be used together with H 2 O 2 for the catalytic synthesis of adipic acid from cyclohexene. During the experiment, the effect of weight content of [C 3 SO 3 Hnhm] 3 PW 12 O 40 on the catalytic performance was investigated in detail. And the chemical structure of the catalyst was also characterized by XRD, FT-IR, 1 H-NMR, SEM–EDX and N 2 adsorption–desorption isotherms. Experimental results revealed that the desired products has been successfully prepared, and the best catalytic performance (81.2% yield of the adipic acid) was obtained under the dose of [C 3 SO 3 Hnhm] 3 PW 12 O 40 was 31wt%, which was almost close to the catalytic activity of original [C 3 SO 3 Hnhm] 3 PW 12 O 40 (85.3% yield of the adipic acid), which was also proved the strategy of packaging ionic liquid phosphotungstate with MIL-101 in this research is feasible. Furthermore, recycled catalytic performance of the catalyst under repeat 6 times was evaluated and the result revealed that the yield in adipic acid was still higher than 80.0%, which also proved that the catalytic active component was stable in the catalyst. Graphic Abstract
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Jianqiu Gong,Weiwei Zhang,Tapas Sen,Yichen Yu,Yuchen Liu,Jinlong Zhang,Lingzhi Wang
Photocatalysis is a promising technology to treat dilute phenol–Cr(VI) mixture, where photoinduced electrons are commonly thought of as the main active species for Cr(VI) reduction. However, it generally depends on the surface adsorption to achieve efficient electron transfer. Meanwhile, the possible contribution of reductive quinone derivatives oxidized from phenol to Cr(VI) reduction has been rarely explored. The key is to explicitly understand the relation between the phenol oxidation pathway and Cr(VI) reduction. Herein, Ag/AgCl/MIL-101(Fe) prepared by directly loading Ag nanoparticles on MIL-101(Fe) was applied to the joint treatment of phenol and Cr(VI). The role of quinone derivatives in reducing Cr(VI) was revealed by excluding the surface adsorption. During the phenol oxidation, •OH radicals were more consumed in the initial stage for the ring opening of phenol. Meanwhile, 1O2 evolved from •O2– gradually caused the accumulation of reductive quinone intermediates, which dramatically accelerated the Cr(VI) reduction afterward. This study demonstrates the significance of controlling the evolution process of active oxygen species for the joint photocatalytic treatment of phenol–Cr(VI) mixture.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Yingpan Song,Lina He,Shuai Zhang,Xiao Liu,Kun Chen,Qiaojuan Jia,Zhihong Zhang,Miao Du
Iron-based metal-organic framework, NH 2 -MIL-101(Fe), was doped with different dosages of cobalt phthalocyanine nanoparticles (CoPc) to synthesize a series of NH 2 -MIL-101(Fe)@CoPc nanocomposites. The NH 2 -MIL-101(Fe)@CoPc nanocomposites were then employed to construct novel impedimetric aptasensors for the detection of ochratoxin A (OTA). Combining the intrinsic advantages of NH 2 -MIL-101(Fe) (highly porous structure and excellently electrochemical activity) and CoPc (good physiochemical stability and strong bioaffinity), the NH 2 -MIL-101(Fe)@CoPc nanocomposites show promising properties, which are beneficial for immobilizing OTA-targeted aptamer strands. Amongst, the developed impedimetric aptasensor based on NH 2 -MIL-101(Fe)@CoPc 6:1 , prepared using the mass ratio of NH 2 -MIL-101(Fe):CoPc of 6:1, exhibits the best amplified electrochemical signal and highest sensitivity for detecting OTA. The detection limitation is 0.063 fg·mL −1 within the OTA concentration of 0.0001–100 pg·mL −1 , accompanying with high selectivity, good reproducibility and stability, acceptable regenerability, and wide applicability in diverse real samples. Consequently, the proposed sensing strategy can be applied for detecting OTA to cope with food safety.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Xing-Zhe Guo,Shuai-Shuai Han,Ji-Min Yang,Xiao-Meng Wang,Shui-Sheng Chen,Shuai Quan
We herein report that the morphology, size, and surface charge status of MIL-100(Fe) micro/nanoparticles can be tailored by adding a coordination modulator (HF or tetramethylammonium hydroxide) to the reaction system. Interestingly, the adsorption capacities of low-crystallinity MIL-100(Fe) and MIL-100(Fe)-TMA toward Congo red (CR) and acid chrome blue K (AC) were found to be significantly larger than that of the high-crystallinity MIL-100(Fe)-HF adsorbent, whereas there was little difference in the adsorption capacities of the three MIL-100(Fe) toward methyl orange (MO) and methylene blue (MB). The adsorption uptake of MIL-100-(Fe)-TMA toward the anionic dyes (CR, AC, and MO) was found to be highest, whereas the adsorption uptake of MIL-100(Fe) toward the cationic dye (MB) was the highest owing to different adsorption mechanisms. This adsorption behavior could be rationalized based on the morphological characteristics and crystal structure defects, zeta potential, and pore volume of MIL-100(Fe) and the adsorption characteristics and molecular structure of the dye. It was revealed that the adsorption performance of MIL-100(Fe) micro/nanoparticles is governed by the synergistic interplay between electrostatic, hydrophobic, and π–π stacking interactions, pore volume, crystal structure defects, and steric hindrance of the adsorbent.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Wen Cao,Yuhang Yuan,Cao Yang,Shichuan Wu,Jianhua Cheng
For the first time, visible-light-driven g-C 3 N 4 /MIL-68(In)-NH 2 heterojunction composites with high photocatalytic activity were prepared for the degradation of ibuprofen (IBP) using an in-situ solvothermal synthesis method assisted with ultrasonication. The composites achieved intensive visible-light absorption, enhanced separation efficiency of photogenerated carriers, and high adsorption capacity, thus achieving excellent photocatalytic degradation for IBP. Among all the composites, 10 wt% g-C 3 N 4 /MIL-68(In)-NH 2 exhibited the maximum photocatalytic rate (0.01739 min −1 ), 19.28 and 2.00 times higher than those of g-C 3 N 4 and MIL-68(In)-NH 2 , respectively. Moreover, the pH, ibuprofen concentration, and catalyst dosages played important roles both in photodegradation and adsorption. In addition, the photocatalytic mechanism was also elucidated, demonstrating that h + was the main reactive species, followed by OH and O 2 − radicals, responsible for the degradation of IBP. Finally, seven aromatic intermediates of IBP were identified, and five possible degradation pathways were proposed, mainly involving hydroxylation, aldehyde oxidation, decarboxylation, and dehydrogenization reactions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaohuan Zang,Qingyun Chang,Hongda Li,Xiaoxian Zhao,Shuaihua Zhang,Chun Wang,Zhi Wang
In this work, a ringent multi-shelled hollow MIL-88B (RMH-MIL-88B) was prepared from the original MIL-88B via etching by citric acid, and was used as the fiber (SPME) coating material for the direct-immersion solid-phase microextraction of eleven organochlorine pesticides (OCPs) from fish samples prior to gas chromatography-electron capture detection. The unique multi-shelled structure with void space between shells enables the RMH-MIL-88B to provide more adsorption sites and to have larger adsorption capacities for the OCPs than the original MIL-88B. Under the optimized experimental conditions, a wide linear range (from 3.3 to 600.0 ng g −1 ) with the coefficients of determination ( r 2 ) varying from 0.9960 to 0.9997 was obtained. The limits of detection (S/N of 3) for the analytes were in the range of 1.0–3.0 ng g −1 . In the determination of the analytes, the single fiber repeatability (n = 5) by single RMH-MIL-88B-coated fiber ranged from 4.1 % to 7.6 %, while the fiber-to-fiber reproducibility by five parallel RMH-MIL-88B-coated fibers were in the range of 8.0 %–12 %. The established method was successfully applied for the sensitive determination of the eleven OCPs in four fish samples (grass carp, crucian carp, tilapia, and mandarin fish). The relative recoveries of the analytes for spiked fish samples at three concentration levels (15.0, 80.0 and 300.0 ng g −1 ) were in the range of 82.11 %–115.7 % with the relative standard deviations of 4.4 %–12 %.
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Yuwei Sun,Xin Qi,Chou Chen,Wenyu Liu,Qian Tang,Honghui Teng,Baixiang Ren
In this work, AgI nanoparticles were anchored on decahedron-like MIL-125(Ti) through wet precipitation method, and the photocatalytic activities were analyzed by tetracycline (TC) degradation rates under simulated sunlight. The structures, morphologies, valence bonds, optical absorption properties, charge separation efficiencies of the prepared samples were tested by XRD , SEM, EDS , XPS, UV–Vis DRS and PL spectroscopy. Compared with pure MIL-125(Ti), AgI@MIL-125(Ti) displayed excellent photocatalytic performance on TC degradation. When the mass fraction of AgI in AgI@MIL-125(Ti) was 10 %, AgI@MIL-125(Ti)-10 % displayed the best photocatalytic efficiency, which 96.9 % of TC was removed under simulated sunlight for 30 min. The results of active species trapping experiments and ESR tests showed that the Z-Scheme heterojunction between AgI and MIL-125(Ti) promoted the separation of photogenerated charges. Furthermore, a part of Ag + were reduced to Ag NPs in the process of photocatalytic reaction, which constructed a cross-linking bridge for the charges at the interface of AgI and MIL-125(Ti) and further accelerated the electron transmission. The intermediate toxicity experiments proved that the toxic structures are destroyed in TC solution after MIL-125(Ti)-10 % photocatalytic degradation, and the toxicity of the reaction system was reduced effectively.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Liyuan Wang,Liyuan Xie,Lingli Dong,Zhitao Wang,Linpo Li,Enbo Shangguan,Jing Li,Shengbo Gao
Novel structural designs for metal organic frameworks (MOFs) are expected to improve ion-transport behavior in composite solid electrolytes . Herein, upper-dimensional MIL-53(Al) nanofibers (MNFs, MIL-53 belongs to the MIL (Material Institute Lavoisier) group) with flower-like nanoflake structures have been designed and constructed via modified hydrothermal coordination. The optimized MNFs with high surface area and porosity can form abundant interfaces with poly(ethylene oxide) (PEO) matrix. The plasticization of MNFs to the PEO matrix will facilitate segmental movement of PEO chains to facilitate Li + conduction. The unsaturated open metal centers of MNFs can effectively capture bis(trifluoromethanesulfonyl)imide anions (TFSI − ) to deliver more free lithium ions for transfer. Moreover, the upper-dimensional nanofiber structure endows lithium ions with a long-range and consecutive transport pathway. The obtained composite solid electrolyte (MNFs@PEO) presents a high ionic conductivity of 4.1 × 10 −4 S cm −1 and a great Li + transference number of 0.4 at 60 °C. The electrolyte also exhibits a stable Li plating/stripping behavior over 1000 h at 0.1 mA cm −1 with inhibited Li dendrite growth. Furthermore, the Li/LiFePO 4 and Li/LiNi 0.8 Mn 0.1 Co 0.1 O 2 batteries with MNFs@PEO as electrolytes both display great cycling stabilities with high-capacity retention, indicating their potential applications in lithium metal batteries . The study will put forward new inspirations for designing advanced MOF-based composite solid electrolytes.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Dedong Jia,Zelong Shen,Yaohui Lv,Zhipeng Chen,Hongqiang Li,Yan Yu,Jieshan Qiu,Xiaojun He
The design and fabrication of advanced cathode materials with excellent electrochemical properties to match the Zn anode is crucial for the development of aqueous zinc-ion batteries (ZIBs). Herein the synthesis of MIL-88B(V)@rGO composites is reported, in which MIL-88B(V) nanorods are anchored on reduced graphene oxide (rGO) sheets, as cathode for ZIBs, where the graphene oxide induces the formation of small-size nanorods instead of typical prism morphology. During the initial charge/discharge process, the cathode undergoes an in situ irreversible transformation from MIL-88B(V) to amorphous V 2 O 5 that acts as active site for the subsequent Zn 2+ insertion/extraction. The hierarchical structure of the composites and the amorphous V 2 O 5 provide abundant channels and active sites for Zn 2+ diffusion and adsorption. The density functional theory calculation reveals that the rGO sheets have two functions, i.e., to improve the conductivity and to reduce the Zn 2+ migration energy barrier. Consequently, the MIL-88B(V)@rGO cathode exhibits an ultrahigh reversible capacity of 479.6 mAh g −1 at 50 mA g −1 and good rate performance of 263.6 mAh g −1 at 5000 mA g −1 , which are superior to metal–organic frameworks (MOFs) cathodes reported in literature. This work may shed a new light to the design and fabrication of MOFs-based cathodes for aqueous ZIBs.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 31
·14828-14839
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IF 3.3
Lin Dong,Yunlan Xu,Dengjie Zhong,Nianbing Zhong,Zhuofan Han,Yi Liu,Haixing Chang
The low electron–hole separation in the photoanode generally restricts the visible light response of photocatalytic fuel cell (PFCs). In this study, 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode was synthesized and assembled with a PFC with Cu cathode to degrade rhodamine B and generate electricity. With visible light irritation, the maximum photocurrent density, maximum power density, and degradation rate of the PFC were 0.59 mA cm−2, 29.88 μW cm−2, and 97.48% (1 h), respectively. The major active species in the PFC were h+, ˙O2−, and ˙OH. The good performance of the PFC was ascribed to the formation of a double Z-type heterojunction in the 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode so that the photoelectrons of NH2-MIL-125 and Bi2O3 directly combine with the photoholes of g-C3N4, making the photoholes of NH2-MIL-125 and Bi2O3 and the photoelectrons of g-C3N4 directly or indirectly involved in the RhB degradation process and generating electricity. Thus, the separation rate of the e−–h+ pairs in the photoanode and the capability of the PFC are greatly improved.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2023
·
IF 4.1
Lin He,Jiabin Zhou,Dan Liu,Yajie Wen,Yuxin Gan
The combination of photocatalysis and Fenton oxidation technology is an efficient strategy to improve the efficiency of oxytetracycline hydrochloride (OTC-HCl) degradation. Herein, a Fe 3 O 4 @GO@MIL-101 composite catalyst bridged with graphene oxide (GO) was obtained by a two-stage hydrothermal method . The introduced graphene oxide layer could inhibit the recombination of electron hole (e − - h + ) pairs by attracting photo-generated electrons from MIL-101 and transferring them to Fe 3 O 4 , observably enhancing the photocatalytic performance of the composite Fe 3 O 4 /MOFs. Under the optimal conditions (initial pH, 10 mmol H 2 O 2 , 0.01 g/L catalyst), the Fe 3 O 4 @GO@MIL-101 + H 2 O 2 +Vis system could achieve a degradation effect of 97.26 % on 70 mg/L OTC-HCl within 50 min Fe 3 O 4 @GO@MIL-101 nanocomposites exhibited good recyclability , were easy to recover after multiple uses, and maintained excellent removal efficiency for pollutants. A series of data demonstrated that in Fe 3 O 4 @GO@MIL-101 + H 2 O 2 +Vis system, the primary active substances involved in OTC-HCl degradation were holes and superoxide radicals , while the contributions of hydroxyl radicals and photo generated electrons were relatively weak. Finally, based on various characterization results and catalyst activity performance, a feasible mechanism for the removal of OTC-HCl by Fenton-like system was proposed.
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ANALYST
·
2023
·Vol. 148
·期 12
·2725-2731
·
IF 4.2
Yuhan Ji,Yupu Wei,Jinghui Shen,Jinlong Zhuo,Mingqi Xu,Yunliang Wang,Jingquan Sha
To improve the peroxidase-like activities of metal–organic frameworks (MOFs) as nanozymes, a ternary MIL-100(Fe)@PMo12@3DGO nanocomposite was designed and fabricated by encapsulating Keggin-type H3PMo12O40 (PMo12) with fast and reversible multi-electron redox processes and an electron-rich structure into MIL-100(Fe), then being covered by three-dimensional graphene (3DGO) with higher conductivity, larger surface area, higher porosity, and better chemical stability. As a consequence, the as-prepared MIL-100(Fe)@PMo12@3DGO nanocomposite exhibits excellent peroxidase-like activities, namely, the lowest limit of detection (0.14 μM) in the range of 1–100 μM for glucose to date, to the best of our knowledge, attributed to the individual and synergistic effects of H3PMo12O40, 3DGO and MIL-100(Fe).
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