WATER RESEARCH
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2020
·
IF 9.13
Chenghan Ji,Daowen Wu,Junhe Lu,Chao Shan,Yi Ren,Ting Li,Lu Lv,Bingcai Pan,Weiming Zhang
Adsorption is a viable technology to remove trace heavy metals from wastewater, but regeneration of adsorbents in an economic and environmentally friendly manner often represents a limiting factor of its application. Compared with traditional strong acid desorption, developing a chemical-free method is of great significance to both economic and the environmental welfare. Herein, we synthesized a novel thermoresponsive absorbent, A-MIL-121, which could effectively remove trace Cu(II) (> 95 %) from a high-salinity ([Na + ]/[Cu 2+ ] = 20000) water at normal temperature. At elevated temperature, A-MIL-121 could quickly and efficiently desorb Cu(II), with over 90% desorption rate at 80°C within 3 h. Fourier transform infrared spectroscopy (FTIR) analysis revealed that two types of –COOH groups existed in the material. One was in free form and acted as the sites for Cu(II) adsorption; the other was in dimer connected by two H-bonds, which cleaved at elevated temperature. As a result, massive exchangeable protons were released to the solution, which caused the desorption of Cu(II). Similar temperature dependent adsorption-desorption behavior was also found to other heavy metals, such as Cd 2+ , Pb 2+ , Ni 2+ . No significant capacity loss was observed after 10 successive adsorption-desorption cycles. Finally, Column experiments using a real copper electroplating wastewater showed that a total of ~ 1650 mL of clean water was generated before breakthrough (Cu 2+ < 0.5 mg/L), while less than 45 mL of 80°C water was used for regeneration. This study indicates the potential of A-MIL-121 as a novel green adsorbent to address trace heavy metals in wastewater.
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Journal of Environmental Chemical Engineering
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2020
·
IF 4.3
Shanshan Chen,Zhongyang Zang,Shusheng Zhang,Gangfeng Ouyang,Runping Han
Metal-organic framework and nano carbon materials were widely used in separation field in recent years. In this study, nanocomposite of MIL-100(Fe) and multi-walled carbon nanotubes (MIL-100(Fe)-CNTs) was prepared and characterized and its adsorption property towards Oxytetracycline (OTC) was presented. MIL-100(Fe)-CNTs exhibits higher adsorption capacity compared to MIL-100(Fe), making this composite as one of the favorable adsorbents. The adsorption capacity of MIL-100(Fe)-CNTs reached 429 mg·g −1 at 313 K. The langmuir model and Koble-Corrigan model were better to predict the equilibrium data while the pseudo-second-order kinetic model could well describe the kinetic process. The process was endothermic and spontaneous while the ion exchange was the main adsorption mechanism of OTC on MIL-100(Fe)-CNTs. The nanocomposite is promising to effectively remove OTC from solution.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2020
·Vol. 27
·期 30
·37839-37851
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IF 3.056
Xu Jun,Xu Jinmei,Jiang Shanqing,Cao Yu,Xu Kailin,Zhang Qiuya,Wang Liping
In this work, a novel visible light–driven heterostructure Ag 3 PO 4 /MIL-100(Fe) composite photocatalyst was successfully synthesized via facile chemical deposition method at room temperature. Especially when the mass ratio of Ag 3 PO 4 was 20% of MIL-100(Fe) (APM-2), it displayed the best photocatalytic performance, for which the degradation rate of tetracycline (TC) in conventional environment was 6.8 times higher than that of bare MIL-100(Fe). In addition, the effects of the initial concentration and pH of the solution on the degradation of tetracycline were also studied, and the results showed that the degradation of tetracycline was more favorable in a weakly alkaline environment. The excellent performance of Ag 3 PO 4 /MIL-100(Fe) composites was attributed to the fact that on the basis of having adequate photocatalytic active sites, modifying MIL-100(Fe) with an appropriate amount of Ag 3 PO 4 particles can more effectively separate photogenerated electron–hole pairs. Five cycles of experiments showed that APM-2 has good photostability. Lastly, it was proved through quenching experiments that •O 2 − , h + , and •OH all played corresponding roles in the degradation process, and a possible Z-scheme heterostructure photocatalytic degradation mechanism was proposed.
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SENSORS AND ACTUATORS B-CHEMICAL
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2020
·
IF 7.1
Li Hou,Yuemei Qin,Tianran Lin,Ying Sun,Fanggui Ye,Shulin Zhao
The synthesized Fe-MIL-88NH 2 was used as a nanozyme and fluorescence probe to successfully construct a selective fluorescent sensing platform for one step determination of catechol. Fe-MIL-88NH 2 exhibited excellent peroxidase mimic property as well as fluorescence property. With the addition of H 2 O 2 and catechol, Fe-MIL-88NH 2 would catalyze the H 2 O 2 to form hydroxyl radicals ( OH). Then, the oxidation of catechol would be triggered by the formed OH, which resulted in the generation of 1, 2-benzoquinone. Afterwards, Michael reaction between the oxidation products of catechol (1, 2-benzoquinone) and Fe-MIL-88NH 2 ligands was triggered and then quenched the fluorescence of Fe-MIL-88NH 2 . The principle of the selective determination of catechol was due to the assistant effect of Michael reaction. Based on the above sensing mechanism, a fluorescent sensing platform for the determination of catechol was established. The limit of detection was 0.0913 μmol L −1 (3S 0, n=8 /K) within a fast response of 10 min. This simple and selective strategy, based on the Michael reaction and the superiority of Fe-MIL-88NH 2 nanozyme, provided a concise sensing platform for catechol determination, which broadened the scope of application of nanozyme and showed a great potential application for on-site testing in food and biology analysis.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Weicheng Cui,Jianpeng Shang,Hongye Bai,Jian Hu,Dongbo Xu,Jinrui Ding,Weiqiang Fan,Weidong Shi
Realizing a highly efficient catalytic activity for photoelectrochemical (PEC) water splitting has been becoming a key challenge for fabricating TiO 2 photoanode, due to its weak light-response ability and poor electrical conductivity. For the first time, we prepared the TiO 2 nanorods decorated with NH 2 -MIL-125 film, and subsequently in-situ implanted Ag nanoparticles (Ag NPs) into NH 2 -MIL-125 film by mild reduction process with the help of amine group. The synergistic effect between NH 2 -MIL-125 and Ag NPs is aimed at efficiently improving light-response and the overall conductivity of photoanode. The PEC performance of as-prepared Ag/NH 2 -MIL-125/TiO 2 hybrid-photoanode has been systemically investigated. The photocurrent density of optimal Ag/NH 2 -MIL-125/TiO 2 has reached 1.06 mA/cm 2 at 1.23 V (vs. RHE) under illumination (100 mW/cm 2 ), which is almost 4.42 times higher than that of pristine TiO 2 . The incident photon-to-electron conversion efficiency (IPCE) value of Ag/NH 2 -MIL-125/TiO 2 has been increased to 51.0% at 390 nm. Furthermore, the desirable charge injection ( η i n j e c t i o n ) of 96.4% and charge separation ( η s e p a r a t i o n ) efficiency of 33.1% have been achieved. The in-situ introduction of Ag NPs into NH 2 -MIL-125/TiO 2 heterostructure provides a novel model for understanding the synergistic effect between metal and MOF over PEC water splitting.
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Catalysts
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2019
·Vol. 9
·期 11
·906
·
IF 3.444
Jieyang Yang,Zequan Zeng,Zhanggen Huang,Yan Cui
In this work, the activation effect of vacuum thermal treatment on MIL-101(Fe) (MIL: Materials of Institute Lavoisier) was investigated for the first time. It demonstrated that vacuum thermal activation could accelerate the activation of persulfate (PS) by MIL-101(Fe), and the enhancement of the catalytic capacity of MIL-101(Fe) was mainly attributed to the change in the FeII/FeIII mixed-valence center. The results of the SEM and XRD showed that vacuum thermal activation had a negligible effect on the crystal structure and particle morphology of MIL-101(Fe). Meanwhile, the higher temperature of vacuum thermal activation caused a higher relative content ratio of FeII/FeIII. A widely used azo dye, X-3B, was chosen as the probe molecule to investigate the catalytic performance of all samples. The results showed that the activated samples could remove X-3B more effectively, and the sample activated at 150 °C without regeneration could effectively activate PS to remove X-3B for at least 5 runs and approximately 900 min. This work highlights the often-overlooked activation effect of vacuum thermal treatment and provides a simple way to improve the catalytic capacity and reusability of MIL-101(Fe) which is beneficial for the application of MIL-101(Fe)/PS systems in azo dye wastewater treatment.Keywords:vacuum thermal activation;MIL-101(Fe);persulfate;azo dye
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Journal of Materials Chemistry B
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2019
·Vol. 7
·期 44
·7006-7013
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IF 5.047
Li Zhang,Xiaoni Ma,Hongbo Liang,Huihui Lin,Guangyu Zhao
Non-enzymatic glucose sensors are attracting significant attention owing to their low cost, storage convenience and reusability; however, their poor anti-interference caused by their weak selectivity towards glucose limits their practicability. In the present study, a MIL-53(NiFe) metal–organic framework (MOF) was prepared on Ni foam to serve as a self-supported electrode for non-enzymatic glucose detection. Due to the abundant active sites in the MIL-53(NiFe) MOF and its good stability in an alkaline solution, the sensors exhibited a high sensitivity (41.95 mA mM−1 cm−2) and a low detection limit (0.67 μM). Moreover, the molecular sieve effect of the MIL-53(NiFe) MOF led to a remarkable anti-interference ability, even at the interference concentrations of up to 20% glucose, a higher value than that in human serum. In addition, a heat treatment was carried out to remove the residual terephthalic acid in the MOF tunnels, and this promoted the detection linear range to 2–1600 μM. The reusability, reproducibility and long-term stability of the sensors were also studied, and the results implied good practicability of the MIL-53(NiFe) MOF-based sensors. Furthermore, the good practicability of the sensors was verified by testing human serum samples. The results showed the relative standard deviation of 2.73% from the hospital results, and the standard recovery was nearly 100%.
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Beibei Zhang,Guiju Xu,Lei Li,Xiaoli Wang,Na Li,Ru-Song Zhao,Jinming Lin
Trihalomethanes (THMs) and halonitromethanes are the two most dominant categories of volatile disinfection by-products that pose considerable public health concerns. The pretreatment and determination methods of THMs in low concentrations, particularly trichloronitromethane (TCNM), have always been the focus of researchers. Metal-organic frameworks, which are effective adsorbents, have considerable potential for solid-phase microextraction (SPME) because of their tuned pore structure, large surface area, and high thermal and chemical stabilities. In this study, MIL-96 was successfully fabricated and developed as a coating fiber for SPME of THMs and TCNM in water samples. Several extraction parameters (i.e., extraction temperature, extraction time, stirring rate, pH, and ionic strength) and desorption parameters (i.e., temperature and time) were investigated and optimized in detail. Ionic strength, extraction temperature, and pH/desorption temperature were identified as key factors that affected the SPME efficiencies of THMs and TCNM. The developed method under optimal conditions obtained wide linearity (0.02–50 µg/L), low limits of detection (0.0030–0.0110 µg/L), and high enrichment factors (81–1181) for detecting THMs and TCNM. The spiked recoveries (1 and 10 µg/L) and relative standard deviations ranged from 81.0% to 109.9% and from 3.92% to 10.10%. Notably, the developed SPME method could overcome thermal degradation and showed excellent performance for TCNM. These results indicated the applicability of MIL-96 as coating fiber.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Zhenhua Hou,Libo Wang,Gang Liu,Ya Wang,Yuhan Wang,Yangyang Zhang,Xiayu Wu,Nan Li
Ammonia has important application value in agriculture and industry as a raw material for producing nitrogen fertilizers and organic chemicals. The Haber-Bosch method is generally utilized to synthesize ammonia through N 2 and H 2 as raw materials in industry, but the process generates serious energy consumption and pollution. In the paper, a heterojunction catalyst is constructed that adopts NH 2 -MIL-125 and Fe-doped W 18 O 49 (Fe-W 18 O 49 ) for photocatalytic nitrogen fixation. Fe-W 18 O 49 is a nanowire containing oxygen vacancies (OVs). OVs can provide active sites for the adsorption and activation of nitrogen gas. The 3D plate-like morphology of NH 2 -MIL-125 can observably reduce the occurrence of nanowires aggregation. This phenomenon can be attributed to NH 2 -MIL-125 playing a supporting role in the fixation of nanowires. New mesoporous are formed between NH 2 -MIL-125 and Fe-W 18 O 49 in the constructed compound catalyst, which can realize efficient mass transfer between the inside and outside of the catalyst. EPR characterization discovers that Fe-W 18 O 49 /NH 2 -MIL-125 cannot produce •O 2 ˗ and •OH radicals. The type II heterojunction forms between Fe-W 18 O 49 and NH 2 -MIL-125. The heterojunction improves the carrier migration path, and the photocurrent intensity is significantly increased. Under simulated sunlight, Fe-W 18 O 49 /NH 2 -MIL-125–2 emerges the best catalytic performance with an ammonia formation rate of 128.2 µmol g −1 h −1 . The yield of ammonia is boosted in comparing with NH 2 -MIL-125 (13 times) and Fe-W 18 O 49 (1.7 times). After several cycles, Fe-W 18 O 49 /NH 2 -MIL-125 remain maintains good stability during the catalytic process. This paper provides a possibility for constructing low-cost heterojunction catalysts in the territory of photocatalytic nitrogen fixation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinqi Luan,Syed Jalil Shah,Xin Yu,Ruimeng Wang,Jingyu Bao,Liming Liu,Jiguang Deng,Zhongxing Zhao,Zhenxia Zhao
Highly efficient capture of volatile organic compounds (VOCs) under humid conditions is a significant yet formidable task for metal–organic frameworks (MOFs). Based on the material simulation technique, we proposed implanting a significantly positive-density ligand (DABA) to modify MIL-101 and constructing dual positive-charging centers to improve MIL-101 competitive adsorption of benzene VOCs over H 2 O vapors both thermodynamically and kinetically. The introduction of DABA containing two –NH 2 groups with electrostatically positive charges into MIL-101 resulted in the formation of an open tetrahedral cage with a dual positive charging center. This facilitated strong N-H…π interactions with toluene molecules, leading them to accumulate firmly in MOF pores, and thus dramatically enhanced its adsorption capacity from 17 to 31 toluene molecules per unit cell compared to pristine MIL-101. Moreover, the open tetrahedral cage in D-MIL-101 preferentially captured toluene and occupied the strongest adsorption sites first, thus effectively preventing H 2 O entry into MOF pores to contact with hydrophilic metal sites. This realized high water resistance and toluene adsorption uptake under high humidity conditions. Results showed that D-MIL-101 had a high specific surface area of 2558 m 2 /g and a new microporous structure of 9.5 Å size. It presented higher toluene uptake of 4.69 mmol/g at lower vapor pressure of P / P 0 = 0.013 and 298 K temperature, as well as 3.3 folds higher working capacity of toluene compared to pristine MIL-101 under 80 % RH. This study presents a novel approach for constructing hydrophobic MOFs using new positive charging ligands and delves deeper into the competitive adsorption of VOCs/H 2 O in MOF composites for large-scale applications.
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Separations
·
2023
·Vol. 10
·期 12
·580
·
IF 2.6
Jinmei Zhu,Xiaofei Wen,Yuanhui Feng,Shuaibing Ren,Zimo Lou,Jiansheng Li
Cathodic reduction is a green and promising remediation strategy for reducing the antibacterial activity of antibiotic contaminants and increasing their biodegradability. However, the lack of cost-effective electrocatalysts has restricted its application. In this study, we upcycled textile white mud by separating 1,4-dicarboxybenzene (BDC) and fabricating MIL-125(Ti)-derived amorphous TiO2@C (TiO2@C-W) as a functional electrocatalyst. The separated BDC from white mud shows lower crystallinity than BDC chemicals, but the resulting TiO2@C-W features a much higher degree of oxygen vacancies and a 25-fold higher specific surface area than that of TiO2@C derived from BDC chemicals. With florfenicol (FLO) as a probe, TiO2@C-W exhibits similar cathodic reductive activity (0.017 min−1) as commercial Pd(3 wt.%)/C (0.018 min−1) does, which was 1.4 and 3.7 times higher than that of oxygen vacancy-engineered TiO2and TiO2@C, respectively. The as-fabricated TiO2@C-W could not easily remove FLO via the oxygen reduction reaction-based pathway with the applied bias for cathodic reduction. Though the activity of TiO2@C-W undergoes a slight decline with continuous running, more than 80% of 20 mg L−1FLO can still be reduced in the eighth run. Water chemistry studies suggest that a lower initial solution pH boosts the cathodic reduction process, while common co-existing anions such as Cl−, NO3−, HCO3−, and SO32−show a limited negative impact. Finally, TiO2@C-W shows reductive activity against several representative antibiotics, including nitrofurazone, metronidazole, and levofloxacin, clarifying its potential scope of application for antibiotics (e.g., molecules with structures like furan rings, nitro groups, and halogens). This study couples the upcycling of textile white mud with the remediation of antibiotics by developing functional electrocatalysts, and offers new insights for converting wastes from the printing and dyeing industry into value-added products.Keywords:textile white mud;1,4-dicarboxybenzene;electrocatalyst;cathodic reduction;antibiotics
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Bo Xue,Chuanruo Yang,Miao Chang,Dahuan Liu
The development of a green, efficient, and reusable photocatalyst is of great importance for pollution remediation. Herein, a series of core-shell ZIF-8@NH 2 -MIL-125 composites (ZM-X) were prepared by epitaxial growth method. The in-situ homogeneous encapsulation of NH 2 -MIL-125 by ZIF-8 was achieved through the structural modulation, and the formed core-shell architecture exhibited outstanding synergistic effect of adsorption and photocatalysis for eliminating tetracycline hydrochloride (TCH), which dramatically enhanced the photocatalytic reaction rate. The results show that the TCH adsorption capacity of optimized ZIF-8@NH 2 -MIL-125 (ZM-2) is 70.25 mg g –1 , which can be fitted well the pseudo-second-order and Langmuir isotherm modes. Under 100 min of visible light irradiation, the ZM-2 has the best synergistic removal rate on TCH (92.9%) compared with other samples, which is 6.5 times higher than of pristine NH 2 -MIL-125 (14.3%). The results of quenching experiments and ESR analysis clearly demonstrate that the superoxide radical ( · O 2 – ) dominates the TCH photodegradation reaction. In addition, ZM-2 can effectively remove TCH in different types of water systems (e.g., ultrapure water, tap water, lake water and actual pharmaceutical wastewater) through adsorption-photocatalytic synergy. Therefore, the novel core-shell material designed in this study has significant potential for environmental purification applications.
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