CHEMICAL ENGINEERING JOURNAL
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2023
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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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Desalination and Water Treatment
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2024
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IF 1
Honghuan Yin,Huaiwen Wang,Dongai Wang,Miaomiao Shi,Xi Xu,Jiaqi Yang
Developing low-cost and stable adsorbent is urgent and attractive to remove hazardous dye from water. In this study, zirconium based metal-organic framework (NH 2 -UiO-66) was grown on waste wool fibers and the fabricated composite adsorbent (NH 2 -UiO-66/wool) was used to remove anionic dye methyl orange (MO). After characterizing the adsorbents, we determined the effect of pH and initial concentration of MO on adsorption performance. Moreover, adsorption kinetics and isotherms were conducted to reveal the adsorption mechanism. The results showed that NH 2 -UiO-66/wool achieved the highest adsorption capacity at natural pH with the maximum adsorption of 61.0 mg/g adsorbent, which is higher than most biomass based adsorbents. Moreover, NH 2 -UiO-66/wool enabled a broad range of pH (3−11) and initial concentration of MO (10–50 mg/L). Adsorption kinetics and isotherms of NH 2 -UiO-66/wool fitted well with pseudo-second-order model and Langmuir mode, respectively. NH 2 -UiO-66/wool presented 40.3 times higher of kinetics constant than that of original wool in the presence of initial MO concentration of 10 mg/L due to the positive nature of NH 2 -UiO-66. Ultimately, NH 2 -UiO-66/wool presented excellent regeneration ability with 500 mg/L NaCl solution and regeneration efficiency remained 98% after 10 cycles. Overall, this work may provide new insights into the development of MOFs/wool adsorbents for enhanced dye removal.
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PLoS One
·
2022
·Vol. 17
·期 8
·e0271075
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IF 3.752
Bicun Jiang,Fuqiang Liu,Yang Pan,Yan Tan,Chendong Shuang,Aimin Li
Tetracycline (TC) is widely-used antibiotic pollutant with high toxicity, refractory, persistence and bacteriostasis, and its removal from water needs to be enhanced. In this work, a novel Graphite-UiO-66(Zr)/Ti electrode was successfully prepared and evaluated for electrochemical oxidation degradation of TC. The electrochemical performance tests indicate the Graphite-UiO-66(Zr)/Ti electrode had higher electrochemical oxidation activity, which achieved higher TC removal efficiency (98.1% ± 1.5%) than Ti plate (65.2% ± 3.5%), Graphite-MIL-53(Al)/Ti electrode (79.5% ± 2.9%) and Graphite-MIL-100(Fe)/Ti electrode (89.0% ± 2.6%). The influence of operating condition was also systematically studied, and the optimized condition was pH 5.0, 20 mA/cm 2 current density and 0.1 M electrolyte (Na 2 SO 4 ). Through the liquid chromatography mass spectrometry (LC-MS), the TC degradation pathway by Graphite-UiO-66(Zr)/Ti electrode oxidation was proposed. Under the •OH free radical oxidative decomposition effect, the double bond, phenolic group and amine group of TC were attacked. TC was transformed into intermediate product ① (m/z = 447), then was further degraded to intermediates ② (m/z = 401) and ③ (m/z = 417). The latter was fragmented into small fractions ④ (m/z = 194), ⑤but-2-enedioic acid (m/z = 116) and ⑥oxalic acid (m/z = 90, the proposed intermediate). In addition, TC removal remained at 89.6% ± 2.7% in the sixth cycle of operation, which confirmed the efficient reusability and stability for antibiotics removal from water.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Pengxiao Liu,Yan Jia,Yao Ning,Xiaocheng Zhang,Shuhui Tian,Fan Yang,Weiyu Song,Ying Zhang
This study demonstrates the significant effect of incorporating inexpensive transition metal nanoparticles into metal-organic frameworks (MOFs) to improve their room-temperature hydrogen storage properties. Low-cost nanoparticles (Cu, Ni, and CuNi) were incorporated into UiO-66(Zr) via the double-solvent approach (DSA) plus chemical reduction processes. All composites exhibited higher hydrogen storage capacity compared to pure UiO-66 at both room temperature and 60 bar. Notably, the hydrogen spillover efficiency of CuNi nanoparticles loaded in UiO-66 was comparable to that of MOF adsorbents embedded with noble metals such as Pd and Pt. The hydrogen storage capacity of CuNi@UiO-66 was significantly increased from 0.20 wt% to 0.74 wt%. DFT calculations showed that the CuNi alloys facilitated the adsorption and dissociation of hydrogen molecules in comparison to the single metal nanoparticles , thus favoring the hydrogen spillover effect and improving the hydrogen storage performance. This work demonstrates the potential of designing MOF loaded with inexpensive metal nanoparticles for optimized room-temperature hydrogen storage.
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Materials Today Chemistry
·
2025
·
IF 6.7
Liang Chu,Teng Zhao,Zhaokun Wang,Xinyu Zhao,Zhiyong Zhu,Mu Yang,Ge Wang
The development of efficient oxidative desulfurization (ODS) catalysts is of great importance for clean energy. In this study, we report a method for the preparation of defect-enriched UiO-66(Zr) materials via a high-energy ball-milling pretreatment-assisted followed by rapid ethanol crystallization. This method significantly enhances ligand deficiency (46.1 %) and average pore diameter (4.1 nm) without using toxic solvents or pre-synthesized clusters, distinguishing it from conventional solvothermal and one-step mechanochemical approaches. Under the optimal parameters, the resulting UiO-66-BM catalyst exhibits excellent ODS performance, achieving full conversion of dibenzothiophene (DBT, 1000 ppm) within 6 min at 50 °C and 20 min at 30 °C using only 20 mg of catalyst and an O/S molar ratio of 5. The turnover frequency (19.85 h −1 ) and mass specific activity (53 mmol g −1 h −1 ) surpass those of most reported pristine MOFs-based catalysts. Moreover, the catalyst reaction activity maintains high activity over six consecutive cycles, showing excellent stability. The superior performance is attributed to the synergistic effect of ball milling and ethanol crystallization, which generates the enriched structural defects and enlarged mesopores, facilitating mass transfer and active site accessibility. This work presents an effective and eco-friendly strategy for the scalable synthesis of high-performance MOF catalysts for deep desulfurization.
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RENEWABLE ENERGY
·
2021
·
IF 8.001
Hui Li,Yongbo Wang,Xiaoling Ma,Min Guo,Yan Li,Guoning Li,Ping Cui,Shoujun Zhou,Mingzhi Yu
Ca 2+ ion leaching and poor pore structure are obstacles of CaO for biodiesel production . To this end, a typical Zr–based metal organic framework, UiO–66(Zr) is adopted to support calcium acetate to prepare CaO/ZrO 2 catalyst. For comparison, catalyst precursor is activated in nitrogen (UCN) and air (UCA) atmosphere, respectively. Preparation factors including calcium acetate addition and activation temperature are evaluated. Moreover, effects of transesterification parameters on oil conversion are investigated and the optimized parameters are further used to examine catalyst reusability . Meanwhile, catalysts are characterized with TG, XRD, XPS , FTIR, Hammett indicator titration, N 2 adsorption and desorption. Results reveal UCN calcined at 650 °C (UCN650) and UCA calcined at 700 °C (UCA700) separately exhibits the best catalytic performance. The maximum conversion of 96.99% is achieved by UCN650 with catalyst amount of 6 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min. Even after being used 3 cycles, conversion of 92.76% is still achieved by UCN650. By contrast, UCA700 shows lower conversion of 92.94% at the first cycle with catalyst amount of 8 wt% and molar ratio of methanol to oil of 9 at 65 °C for 60 min.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Huan-Yu Chen,Xing-Biao Liu,Qi-Xin Guan,Can-Jun Zou,Ping-Ping Fang
The detection of antibiotics has attracted great attention among scientists and health researchers in the past decades. However, it is still difficult to realize the sensitive and selective detection of antibiotics with similar structures. Herein, the antibiotic molecules of oxytetracycline (OTC) can be sensitively and selectively detected by surface-enhanced Raman spectroscopy (SERS) on NH2–UiO-66(Zr)@Au nanoparticles (NPs). The SERS substrate of NH2–UiO-66(Zr)@Au NPs realizes a detection sensitivity of 1 × 10–12 g·L–1 for 4-mercaptobenzoic acid, indicating its high SERS activity. A high detection sensitivity of 10–11 g·L–1 is obtained for OTC on such a SERS substrate. Besides the high sensitivity, NH2–UiO-66(Zr)@Au NPs can also selectively detect OTC from streptomycin sulfate, salicylic acid, and ofloxacin by SERS on NH2–UiO-66(Zr)@Au NPs, with a selective detection limit of 10–10 g·L–1. Furthermore, OTC can be selectively detected in a real sample of river water with a detection limit of 1.0 × 10–10 g·L–1. Therefore, this study provides an effective way to enrich and detect antibiotics in real samples in the environment.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
·
IF 8
Yijun Chen,Meina Cheng,Long Jin,Hailiang Yang,Sanjian Ma,Zixia Lin,Guoliang Dai,Xin Liu
The Fenton reaction is recognized as an effective technique for degrading persistent organic pollutants , such as the emerging pollutant trimethoprim (TMP). Recently, due to the excellent reducibility of active hydrogen ([H]), Pd–H 2 has been preferred for Fenton-like reactions and the specific H 2 activation of Pd-based catalysts. Herein, a heterogeneous Fenton catalyst named the hydrogen-accelerated oxygen reduction Fenton (MHORF@UiO-66(Zr)) system was prepared through the strategy of building ships in the bottle. The [H] has been used for the acceleration of the reduction of Fe(III) and self-generate H 2 O 2 . The systematic characterization demonstrated that the nano Pd 0 particle was highly dispersed into the UiO-66(Zr). The results found that 20 mg L −1 of TMP was thoroughly degraded within 90 min in the MHORF@UiO-66(Zr) system under conditions of initial pH 3, 30 mL min −1 H 2 , 2 g L −1 Pd@UiO-66(Zr) and 25 μM Fe 2+ . The hydroxyl radical as well as the singlet oxygen were evidenced to be the main reactive oxygen species by scavenging experiments and electron spin resonance . In addition, both reducing Fe(III) and self-generating H 2 O 2 could be achieved due to the strong metal-support interaction (SMSI) between the nano Pd 0 particles and UiO-66(Zr) confirmed by the correlation results of XPS and calculation of density functional theory. Finally, the working mechanism of the MHORF@UiO-66(Zr) system and the possible degradation pathway of the TMP have been proposed. The novel system exhibited excellent reusability and stability after six cyclic reaction processes.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Yijun Chen,Hailiang Yang,Sanjian Ma,Meina Cheng,Zixia Lin,Long Jin,Xin Liu
As a representative antibiotic, trimethoprim (TMP), the emerging pollutant has been frequently detected in water bodies, and its potential harm has aroused the attention of society. Although the emerging pollutant could be efficiently degraded by the advanced oxidation process (AOP) represented by the Fenton reaction , both the problem of iron sludge disposal and the safe use of H 2 O 2 have plagued the further promotion of this technology. The H 2 (precursor of the active hydrogen [H]) and catalyst Pd/UiO-66(Zr) were introduced into the Fenton reaction in this paper. It was found that the process of reducing Fe(III) and self-generating H 2 O 2 could be facilitated due to the reduction of [H]. Under certain reaction conditions (initial pH 3, trace total iron 25 μM, H 2 30 mL·min −1 , catalyst 2 g·L −1 ) and without H 2 O 2 , a Fenton-like system was constructed, named MHORF-UiO-66(Zr). While achieving zero iron sludge discharge, 100 % of 20 mg·L −1 TMP was rapidly degraded within 1 h. It was found that the degradation of TMP could be attributed to the attack of singlet oxygen and hydroxyl radical . Furthermore, the performance changes of catalyst before and after six rounds of reactions were studied and it was found that Pd/UiO-66(Zr) had excellent and stable catalytic performance.
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RSC Advances
·
2020
·Vol. 10
·期 68
·41283-41295
·
IF 3.119
Ahmed S. Abou-Elyazed,Yinyong Sun,Ahmed M. El-Nahas,Ahmed M. Yousif
Recently, the incorporation of hydrophobicity on the surface of UiO-66(Zr) has received much attention due to the deactivation of hydrophilic active sites of UiO-66(Zr) upon water adsorption. In this work, we report UiO-66(Zr) catalysts with an assortment of surface hydrophobicities fabricated by the solvent-free method to elucidate the impact of the environment framing Lewis acid sites on their catalytic activity in the production of fatty acid methyl ester (biodiesel) via the esterification of fatty acids at room temperature with high selectivity (100%) and good recyclability. A detailed structural analysis of the materials by N2 sorption, FT-IR, SEM, XRD, water contact angle measurement, dynamic liquid scattering (DLS), NMR and TGA revealed the fabrication of stearic acid-grafted UiO-66(Zr) catalysts (10SA/UiO-66) with fine particle size and a highly hydrophobic network. 10SA/UiO-66(Zr) with enhanced hydrophobicity exhibited superior catalytic performance in the esterification of a fatty acid with a long alkyl chain compared with conventional solid acid catalysts and even liquid acid catalysts. Detailed kinetic studies corroborated that the adsorption of lipophilic acids at the Lewis acid sites besides the enhancement of wettability between the reactants was facilitated by the hydrophobic environment, thus significantly motivating the esterification reaction at room temperature. Furthermore, 10SA/UiO-66(Zr) showed good catalytic activity in the esterification of oleic acid in the presence of water (∼10% in the light of acid weight).
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 43
·16981-16989
·
IF 3.069
Bingying Jia,Miaojiang Wu,Hua Zhang,Yi Zeng,Gongying Wang
Titanates are frequently used as precursors to prepare transesterification catalysts with TiIV species. Unfortunately, it is challenging to control the dispersity of TiIV active sites on supports. Herein, a series of TiIV species is anchored on abundant linker vacancy sites by introducing point and large scale defects in UiO-66(Zr/Ti) with hierarchical-pore structure. The catalyst functionalized by titanium(IV) oxide bis(2,4-pentanedionate) shows excellent catalytic performance in the transesterification of dimethyl carbonate with phenyl acetate. The catalysts are characterized by XRD, FT-IR, N2 adsorption–desorption, XPS, SEM and STEM-HAADF techniques. The results demonstrate that the delicate mesopores in the support can not only exhibit a large surface area for the distribution of the active sites, but also provide better mass transfer performance. Meanwhile, the introduction of octahedral TiIV ions raises the activity of the catalyst via more coordinatively unsaturated ZrIV sites. Furthermore, using titanium(IV) oxide bis(2,4-pentanedionate) as a Ti source can effectively prevent the condensation of tetrahedral TiIV species anchored on the hierarchical-pore UiO-66(Zr/Ti) support.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Qingqing Wang,Wei Zhou,Claudia Li,Sibudjing Kawi,Yinhui Li
The application of photocatalysts in environmental field has emerged as a prominent research topic. Nevertheless, the efficiency of photocatalysts is reduced as the recombination of photogenerated chargers significantly, restricting their extensive use in this domain. In the present study, photocatalysts composed of bismuth molybdate/NH 2 -UiO-66(Zr) (Bi 2 MoO 6 /NH 2 -UiO-66(Zr)) featuring Z-scheme heterojunctions were effectively synthesized using a two-step hydrothermal technique. These photocatalysts exhibit remarkable photocatalytic degradation under visible light conditions. Notably, the broad planar configuration of Bi 2 MoO 6 sheets improves the separation of the photogenerated charge carriers. NH 2 -UiO-66(Zr) layered atop Bi 2 MoO 6 sheets enhances the availability of catalytically active sites, reduces charge recombination, and promotes charge transfer through the interface. The kinetic rate constant for Bi 2 MoO 6 /NH 2 -UiO-66(Zr) is around 0.00329 L mg −1 min −1 , indicating the increase of 3.78 and 41.13 times compared with pure Bi 2 MoO 6 and NH 2 -UiO-66(Zr), respectively. The efficiency for photocatalytic degradation of tetracycline using Bi 2 MoO 6 /NH 2 -UiO-66(Zr) reaches 81.72 % under visible light. Importantly, this efficiency exhibits a reduction of 10 % after five recycling cycles, demonstrating notable stability. The photocatalytic mechanism involved in tetracycline degradation was uncovered through trapping experiments and EPR, indicating that it is predominantly facilitated by the active oxidation of ·O 2 - and ·OH. The intermediates of the photocatalytic process as well as the possible degradation pathways were discussed. The creation of Bi 2 MoO 6 sheets/NH 2 -UiO-66(Zr) heterojunction photocatalysts provides a fresh approach to the development of novel catalysts, which may lead to significant advancements in environmental remediation efforts.
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