NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 24
·11840-11850
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IF 3.925
Dongying Zhu,Zhujun Huang,Haiyan Wang,Qiujun Lu,Guihua Ruan,Chenxi Zhao,Fuyou Du
The fabrication of sustainable and reusable photocatalyst materials is urgent and desirable for the removal of emerging pharmaceutical pollutants (EPPs) in environmental water samples. In this work, we described the fabrication of electrospun nitrogen-rich carbon nitrides/MIL-101(Fe)/poly(acrylonitrile-co-maleic acid) nanofibers (E-spun g-C3N5/MIL-101(Fe)/PANCMA NFs) by using electrospinning dispersion solutions of g-C3N5/MIL-101(Fe) and PANCMA, as well as their applications as sustainable and reusable photocatalysts toward a model EPP carbamazepine degradation under light irradiation. The E-spun g-C3N5/MIL-101(Fe)/PANCMA NFs exhibited the highest carbamazepine degradation efficiency of 94.2% within 40 min. The O2˙−, ˙OH, and h+ reactive species all participated in the photodegradation process, and some degradation byproducts of carbamazepine were identified by liquid chromatography-mass spectrometry. Importantly, the electrospun photocatalyst possessed high reusability (at least 15 consecutive runs) and wide applications in the degradation of other EPPs (such as tetracycline and ciprofloxacin), which suggested the great potential of the electrospun photocatalytical nanofibers in the EPPs removal.
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Advanced Composites and Hybrid Materials
·
2022
·Vol. 5
·期 4
·2896-2905
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IF 11.806
Xu Haitao,Zu Mei,Cheng Haifeng,Liu Dongqing,Xie Wei
The thermal management of electronic devices has attracted significant research attention in the recent year. However, the commonly used thermal management materials at this stage are mainly phase change materials (PCMs), which are limited by their relatively low enthalpy. In this study, the metal–organic framework MIL-101(Cr) was synthesised by an environmentally friendly and low-cost L-malic acid as the mineralising agent. The as-prepared MIL-101(Cr) composite coating was utilised as a sorbent for a passive thermal management strategy, through a vapour sorption–desorption process. By coating the as-prepared MIL-101(Cr) powder onto a metal substrate, a temperature drop for 25 min (maximum 8.6 °C) was achieved for 0.256 g of coating at a heating power of 2.5 W. The use of latent heat has emerged as an attractive method for intermittent heat dissipation. The equivalent enthalpy of the composite coating could reach as high as 1171.9 J/g coating , indicating a significant improvement in the thermal management performance compared with the conventional PCMs. Graphical abstract
Summary: A composite coating for thermal management was obtained by silicate solution and powder MIL-101(Cr).
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CHEMICAL PAPERS
·
2022
·Vol. 76
·期 7
·4379-4392
·
IF 2.146
Zhang Huixian,Hu Xizhou,Xia Hong,Zhou Youxiang,Peng Lijun,Wu Jianyuan,Peng Xitian
Phenoxy carboxylic acid herbicides (PCAs) are widely used in agricultural production. However, due to their potential threat to human health, it is necessary to develop efficient analysis method for monitoring PCA concentration in environment and food samples. Based on dispersive micro-solid phase extraction (D-μ-SPE) with amine-functionalized metal–organic framework MIL-101(Fe)-NH 2 , a selective, sensitive, and cost-efficient method was proposed for the extraction of PCAs from environmental water and rice samples in this study. From the perspective of adsorption kinetics and isotherms, interaction mechanisms between MIL-101(Fe)-NH 2 and PCAs were investigated. Key parameters of D-μ-SPE procedure including adsorbent dosage, solution pH, ionic strength, eluting solution, and washing solutions were optimized. Using of small amount of MIL-101(Fe)-NH 2 could achieve desirable extraction effect due to its large surface area and multiple interactions with PCAs. Under the optimized D-μ-SPE conditions, calibration curves of 8 PCAs were linear within a concentration range of 0.05–5 ng/mL for water samples ( r 2 > 0.9898) and 0.5–50 ng/g for rice samples ( r 2 > 0.9879). Limits of detection of water and rice samples were as low as 0.004–0.008 ng/mL and 0.05–0.1 ng/g, respectively. The recoveries of 8 PCAs ranged from 83.0 to 109.3%. Both inter- and intra-day relative standard deviations were less than 10.3%. Our proposed method was successfully employed in actual environmental water and rice samples.
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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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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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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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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
·
IF 3.615
Huiyan Pan,Xiaohong Li,Yin Yu,Junrui Li,Jun Hu,Yejun Guan,Peng Wu
Metal organic-framework MIL-101 and inorganic mesoporous composites Al 2 O 3 @SBA-15 supported Pt catalysts, Pt/MIL-101 and Pt/Al 2 O 3 @SBA-15 catalysts, were prepared and characterized by means of X-ray diffraction (XRD), N 2 adsorption–desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), CO chemisorption and thermo-gravimetric (TG) analysis. Pt nanoparticles were highly dispersed on both supports. In liquid-phase hydrogenation of nitrobenzene, benzaldehyde and their derivatives, the Pt/MIL-101 catalyst was superior to the Pt/Al 2 O 3 @SBA-15 catalyst in water. For liquid-phase hydrogenation of nitrobenzene with the Pt/MIL-101 catalyst, owing to high solubility of nitrobenzene in ethanol, the reaction in ethanol went much faster than that in water, furnishing a turnover frequency (TOF) in ethanol up to 18,053 h −1 , almost triple of that obtained in water under similar conditions. The highest TOF of 25,438 h −1 was obtained in ethanol for hydrogenation of 3-chloro-nitrobenzene with the Pt/MIL-101 catalyst. As for hydrogenation of benzaldehyde series, 2-fluoro-benzaldehyde and 3-fluoro-benzaldehyde gave the highest TOFs of 5146 h −1 and 3165 h −1 in water with the Pt/MIL-101 and Pt/Al 2 O 3 @SBA-15 catalysts, respectively. We deduce that surface property of MIL-101 with high hydrophobicity is helpful to enrich reactants around the Pt/MIL-101 catalyst in water, where nitrobenzene or benzaldehyde and its derivatives have a limited solubility, so that high catalytic performance was achieved with the Pt/MIL-101 catalyst in water. Of particular note is that the Pt/MIL-101 catalyst can be reused at least four times without loss in activity or selectivity.
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APPLIED CATALYSIS A-GENERAL
·
2013
·
IF 3.41
Zhiguo Sun,Gang Li,Hai-ou Liu,Liping Liu
A series of MOF-based catalysts, metal-salen complexes incorporated into amino-functionalized MIL-101 matrices by salicylaldehyde condensing to amino group and coordinating metal ion through one pot method, have been prepared and characterized. The successful preparation of catalysts demonstrates that postsynthetic modification (PSM) is a practical and powerful route to generate MOF-based catalyst with multiple active sites. The catalytic performances of prepared catalysts were investigated via selective oxidation of cyclohexane to cyclohexanone and cyclohexanol (KA-oil) by molecular oxygen in the absence of solvent. It was found that NH 2 -MIL-101(Cr)-Sal-Co, as a typical case, behaves as cooperative catalyst for cyclohexane selective oxidation. That is, salen-Co(II) attached to framework of MOF is able to assist in the generation of new radicals from peroxides via a Haber–Weiss catalytic cycle to promote conversion of cyclohexane while framework Cr ion is able to catalyze the dehydration of intermediate product cyclohexyl hydroperoxide (CHHP) to improve KA-oil selectivity. Furthermore, this catalyst exhibits good recyclability and behaves as truely heterogeneous catalyst.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yan Chen,Xiaojuan Yang,Zhonggang Liu,Guohua Liu,Zheng Guo
Resolving the issue of poor conductivity and easy aggregation of MOFs is recognized as one important factor for their successful applications in electrochemical sensors and electrocatalysis. In this work, we propose an assembly of NH 2 -MIL-101(Fe) onto a nanoporous gold (NPG) microelectrode surface. The nanoporous gold could greatly improve the conductivity and reduce the aggregation of NH 2 -MIL-101(Fe). The proposed NH 2 -MIL-101(Fe)/NPG microelectrode was developed for the electroanalysis of ascorbic acid (AA) and uric acid (UA). It exhibited excellent electrochemical performance for the individual and simultaneous sensing of AA and UA in a 0.1 M PBS solution (pH 7.4). High sensitivities (2.03 μA μM −1 cm −2 for AA; 29.30 μA μM −1 cm −2 for UA) were achieved in the simultaneous analysis process. The improved electrochemical performance was attributed to the electrocatalytic properties and large specific surface area of NH 2 -MIL-101(Fe)/NPG, as well as the electrostatic interaction between NH 2 -MIL-101(Fe) and analytes. Moreover, the NH 2 -MIL-101(Fe)/NPG microelectrode was successfully used for the simultaneous detection of AA and UA in complicated environment (human sweat and advanced DMEM). This work shows great promise for the simultaneous detection of AA and UA and extends the applications of MOFs in electrochemical devices.
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RSC Advances
·
2024
·Vol. 14
·期 24
·16727-16735
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IF 3.9
Huizhong Wu,Qiong Yi,Xiang Li,Yingxi Wang,Ling Li
Low catalytic efficiency and catalyst recovery are the key factors limiting the practical application of advanced oxidation processes. In this work, a core–shell magnetic nanostructure Fe3O4@MIL-101(Fe, Co) was prepared via a simple solvothermal method. The core–shell structure and magnetic recovery performance were characterized by various technologies. The results of dye degradation experiments proved that within 10 minutes, the Fe3O4@MIL-101(Fe, Co)/PMS system can degrade more than 95% of 10 mg per L Rhodamine (RhB) at an initial pH of 7, which possesses higher catalytic activity than the Fe3O4/PMS system and the MIL-101(Fe, Co)/PMS system. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that Fe3O4@MIL-101(Fe, Co) displayed excellent degradation efficiency in a wide pH range of 3–11 and capability of resisting coexisting anions. It is worth mentioning that after five cycles, the RhB removal rate can still be maintained at over 90% after 10 minutes of reaction. Free radical quenching experiments were further studied, confirming that ˙OH and SO4−˙ were involved in the degradation of RhB, while the dominating active free radical was SO4−˙. The possible reaction mechanism of the RhB degradation process was also inferred.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinqi Luan,Xuehui Jia,Syed Jalil Shah,Jingyu Bao,Shunxiang Qin,Ruimeng Wang,Jiguang Deng,Zhongxing Zhao,Zhenxia Zhao
Low adsorption efficiency and secondary pollution release pose a bottleneck for the efficient capture of radioactive iodine vapor during nuclear utilization via adsorption. In addition, the simultaneous adsorption of iodine vapor alongside other harmful vapors in complex systems has been rarely reported. In this work, an electron/H-donating defective pore construction strategy involving MIL-101 modification via amino acids (AAs) was proposed to enhance its simultaneous adsorption efficiency for iodine and formaldehyde vapors. These defective microenvironments possessed microporous property with 11.3 Å, which not only formed strong affinity for I 2 molecules itself but also enhanced its adsorption interaction towards polyiodide anion (I 3 - and I 5 - ) through electron donation of AAs. Moreover, these adsorbed polyiodide anions and AAs-SL within the MOFs, resulting in multisite capture of FA via NH…O-H…I hydrogen bonding. The results revealed that AAs coordinated MIL-101 exhibited superior removal rate ( k 80% = 0.61–1.15 g g −1 h −1 ) for iodine vapor than that of the original MIL-101, which was 3.6–30.8 times higher that of state-of-the-art adsorbents under similar conditions. Notably, a high-capacity superior retention rate of 94.8 % was achieved for its I 2 adsorption after exposure to air for 7 days. After adsorption of iodine, AAs coordinated MIL-101 retained high FA adsorption capacity up to 9.7–12.9 mg/g, representing 75.1 %–87.7 % of the original AAs@MIL adsorption capacity for FA. This defective engineering strategy in MOFs supplied an efficient method for removing multiple harmful gases from the surrounding nuclear waste atmosphere.
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