FUEL
·
2020
·
IF 5.578
Zhaoyang Qi,Ting Qiu,Hongxing Wang,Changshen Ye
Ionic Liquids (IL) has been recently immobilized into the pores of metal-organic framework materials (MOFs) to prepare heterogeneous catalyst. However, the IL@MOFs composites are generally prepared by impregnation method, which is unstable in polar solvents. So, we design a new strategy to immobilize IL, and a novel Fenton-like catalyst [mim(CH 2 ) 3 COO]FeCl 4 @UiO-66 has been prepared based on the post-synthetic ligand exchange (PSLE) between MOFs and monocarboxylic functional IL. The [mim(CH 2 ) 3 COO]FeCl 4 @UiO-66 was exploited to act as an efficient heterogeneous catalyst for dibenzothiophene (DBT) oxidation in a biphasic system using H 2 O 2 as the oxidant. Based on optimal conditions, the DBT removal efficiency reached up to 99.1%. Moreover, the heterogeneous catalyst had a good thermal and chemical stability, and the DBT removal efficiency still exhibited over 95% after 6 recycle runs. It is worth noting that the high DBT removal efficiency could be attributed to the synergistic effect between adsorptive and oxidative desulfurization, where [mim(CH 2 ) 3 COO]FeCl 4 @UiO-66 is both an adsorbent and a catalyst.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Yuqiong Gong,Shoujian Gao,Yangyang Tian,Yuzhang Zhu,Wangxi Fang,Zhenggong Wang,Jian Jin
In this work, ultrasmall metal-organic frameworks (MOFs) nanoparticles , UIO-66-NH 2 nanoparticles were synthesized and embedded in an ultrathin polyamide (PA) active layer via the interfacial polymerization reaction on a polydopamine-wrapped single-walled carbon nanotube film. A thin-film nanocomposite nanofiltration (TFN NF) membrane with a PA/UIO-66-NH 2 active layer as thin as 20 ± 3 nm was thus fabricated. The loading mass of the nanoparticles in the TFN NF membrane could be tuned by controlling the nanoparticles concentration in aqueous phase. Benefiting from the ultrathin thickness of active layer and the high loading mass of the MOFs nanoparticles, water permeability up to 46 L m −2 h −1 bar −1 along with a Na 2 SO 4 rejection of 97.1% was achieved, which is 53% increase of the TFC NF membrane without the addition of UIO-66-NH 2 nanoparticles. Our membrane owns the thinnest active layer in the category of TFN NF membranes reported so far and exhibits outstanding desalination performance.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 34
·14379-14388
·
IF 3.288
Fenfen Zhu,Wei Xu,Xiao Li,Hao Meng,Yide Han,Junbiao Wu,Junli Xu,Yan Xu,Xia Zhang
Enzyme immobilization engineering is considered a valid strategy to improve the insensitivity of free enzymes to extreme conditions and thus extend their utilization in actual reactions. Although metal–organic frameworks (MOFs) are extensively applied as supports in enzyme immobilization, their separation from the liquid system after catalytic processes is problematic. In comparison, MOF-based membranes show more convenience in the subsequent solid–liquid separation. In this work, we constructed hybrid membranes by incorporating UiO-66 particles into porous polyvinylidene fluoride (PVDF) and then used them to immobilize lipase for the first time. Because of the strong affinity of UiO-66 towards lipase and the large cavity of PVDF, the hybrid membranes exhibited excellent immobilization ability towards lipase, and the resulting immobilized lipase showed an elevated operating temperature in the range of 40–70 °C with preserved activity and evidently improved thermal stability even after being stored at high temperatures for a definite time. The application of PVDF membrane makes the subsequent separation of the immobilized enzyme from the solutions easier. The immobilization kinetics, isotherm, and thermodynamics were analyzed in detail, and the immobilization mechanism was proposed. Furthermore, the immobilized lipase showed reusability and retained 48.2% of its initial activity after 7 cyclic reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Chun-Shuai Cao,Jingzhen Wang,Xiaoyong Yu,Yinqing Zhang,Lingyan Zhu
Bisphenol analogues have been widely used and displayed adverse effects on human beings. Although many photocatalysts displayed remarkable performance in degrading bisphenol A (BPA) or bisphenol F (BPF), it is not clear if they may also efficiently decompose other bisphenol analogues. In this study, Bi 5 O 7 I with satisfactory photocatalytic activity was doped with metal-organic framework (UiO-67) to build up Bi 5 O 7 I/UiO-67 heterojunctions. The heterojunction enhanced the charge mobility and separation of the electron-hole pairs, which was conducive for improving the photocatalytic activity. Consequently, 4:1-Bi 5 O 7 I/UiO-67 realized highly effective degradation of seven bisphenol analogues in one hour. Density functional theory (DFT) calculations uncovered that the reaction rate constant k displayed a positive correlation with the Hirshfeld charge q (N) of tertiary butyl carbon attached with different substituent groups. This provides a prospective heterojunction catalyst to degrade a group of pollutants with similar structures, and sheds light on the structural relationship of degradation efficiency.
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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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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiayou Liu,Xiaoxiang Huang,Lizhen Hu,Penglei Liu,Liuhu Jia,Keiko Sasaki,Zhongchao Tan,Hesheng Yu
Simultaneous avoidance of secondary air pollution and catalyst deactivation remains a challenge for existing photocatalytic removal of nitric oxide (NO). Herein, a photocatalysis-adsorption (P-A) heterojunction is synthesized for eco-friendly NO removal by facilely grinding Pd single atoms (Pd 1 ) anchored g-C 3 N 4 (48CN/Pd) with UiO-66-NH 2 (UION). Under visible-light irradiation, the 40UION-CN/Pd composite shows 93.91 % of NO removal efficiency with only 2.73 % of NO 2 emissions and negligible catalyst deactivation. The DeNO x index increases remarkably from −0.66 for 48CN/Pd to 0.86 for 40UION-CN/Pd. Furthermore, the synthesized P-A heterojunction efficiently removes NO from real flue gases produced by a domestic coal-fired stove and from SO 2 -rich flue gases. The mechanism exploration based on experimental investigations and density functional theory (DFT) calculations reveals that UION captures the NO 2 selectively produced by 48CN/Pd, simultaneously suppressing NO 2 emissions and refreshing active sites for NO photooxidation. Moreover, the results of X-ray photoelectron spectroscopy (XPS), charge density difference calculation, energy-resolved distribution of electron traps (ERDT) and in-situ Kelvin probe force microscopy (KPFM) reveal that the built-in electric field and Type-II heterojunction formed between 48CN/Pd and UION promote the separation of photogenerated carriers, enhancing the catalytic activity of the composite. This work provides an innovative strategy to avoid NO 2 emission and catalyst deactivation during photocatalytic NO removal.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Siyu Liu,Jianhua Zu,Gang Han,Xiaohan Pan,Yi Xue,Jingjie Diao,Qing Tang,Mingjie Jin
137 Cs is a radioactive pollutant in the production of wastewater from nuclear power plants. In this study, a rapid and simple in-situ synthesis new method was employed to prepare a novel AMP-functionalized UiO-66 composite material for the selective capture of 137 Cs from low-level radioactive wastewater. Characterization techniques such as SEM-EDS, FTIR, XRD, TG, and BET were used to confirm the successful loading of AMP on the surface of UiO-66. UiO-66/AMP showed a good removal effect in pH4-11. At pH7, the effects of different parameters, such as the initial Cs concentration, the ratio of the amount of adsorbent to the volume of solution, and the adsorption time were investigated. The adsorption efficiency is 96.7%, the maximum adsorption capacity is 94.9 mg/g and has fast adsorption kinetics (90% Cs + removal within 5 min). The adsorption data conformed to the pseudo-second-order kinetic model and Langmuir isotherm model, suggesting a monolayer homogeneous adsorption process. XPS helps confirm that the adsorption mechanism is the ion exchange between Cs + and NH 4+ ions. Particularly, in the adsorption experiments of 137 Cs, UiO-66/AMP demonstrated good selectivity (K d Cs : 5.8 × 10 3 ∼ 1.26 × 10 4 mL/g) towards trace Cs + in a mixed ion solution with a molar ratio of 1 (Cs): 2.18 × 10 15 (Na): 4.6 × 10 14 (K): 2 × 10 14 (Mg): 2 × 10 14 (Ca), indicating its potential for selective capture of 137 Cs from low-level liquid waste (LLLW).
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CHEMOSPHERE
·
2023
·
IF 8.8
Xiule Wang,Fanyong Yan,Ying Chen,Xinyi Bai,Yang Fu
Metal organic frameworks (MOFs) possess a large surface area, inherent porosity and high crystallinity . Nevertheless, they lack electron acceptors, which limit the exploitation of their photocatalytic properties. Carbon dots (CDs) known for excellent optical properties can serve as localized electron acceptors. As a novel hybrid nanomaterial , the structure of CDs@MOFs effectively facilitates charge separation and carrier transfer, bring about a marked improvement of photocatalytic activity. In this study, yellow-emission carbon dots (YCDs) were encapsulated within zirconium-based metal organic framework (UiO-66) via a dynamic adsorption method. Compared with blue carbon dots (BCDs), the YCDs@UiO-66 exhibited superior degradation performance. It demonstrates that incorporation of YCDs broadens the UV absorption range of UiO-66, thereby enhancing light utilization. The degradation efficiency of YCDs@UiO-66 was 92.6%, whereas UiO-66 alone achieved only 63.1%. Notably, the results of the radical quenching experiment and electron paramagnetic resonance (EPR) revealed that h + and •O 2 − played a prominent role in the photodegradation of tetracycline hydrochloride (TCH). This study highlights that the introducing YCDs in MOFs-mediated photocatalytic reactions is a viable strategy to improve catalytic efficiency.
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·111039-111050
·
IF 5.8
Dong Shiwen,Liu Xuan,Kong Xianxian,Dong Feilong,Yu Yan,Wang Lizhang,Wang Da,He Zhiqiao,Song Shuang
Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have been proved as efficient catalysts for photocatalytic hydrogen (H 2 ) evolution, thanks to their tunable functionalities, permanent porosity, excellent visible light response, and physicochemical stability. Herein, a series of photocatalysts (termed NUBC) was fabricated by loading different amounts of Zr-UiO-66-NH 2 (NU) onto a benzoic acid–modified covalent triazine–based framework (BC) based on post-synthetic covalent modification. The resulting NUBC catalysts exhibited a type-II Z-scheme heterojunction structure formed via the amide covalent bonds between the amine groups on NU and carboxyl groups on BC. The optimal loading of NU on BC is 30 wt.% (30NUBC) and the corresponding photocatalytic H 2 evolution rate was 378 μmol h −1 g −1 , almost 445 and 2 times than that of NU and BC, respectively. The synergistic effect between the type-II Z-scheme heterojunctions and amide bonds was conducive to boosting visible light harvesting and facilitating charge transportation and separation. Furthermore, the prepared NUBC catalysts show great reusability and stability. Overall, this work sheds light on the design of novel MOF/COF hybrid materials and provides a systematic exploration of their photocatalytic H 2 evolution properties.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Mengshuo Du,Youyu Cao,Xueli Luo,Weixia Yang,Wanmei Lin,Yingying Wang,Wenzhi Tang,Zhonghong Li
Threats caused by heavy metal ions have prompted people to develop porous and functionalized materials to remove them. Metal–organic frameworks (MOFs) show potential for heavy metal ions removal due to the high specific surface area, tunable pore size, flexible designability and favorable stability. However, the intrinsic microporous structure and powder form limit their applications. Herein, we designed a shapeable aerogel bead incorporated with L-cysteine-modified defective UiO-67 for Pb(II), Cd(II) and Cu(II) adsorption. The pristine UiO-67 powders were firstly modified by introducing the modulator (octanoic acid) and an extra ligand (2,2′-bipyridine-5,5′-dicarboxylic acid) to construct defects, both of them competed with the original ligand to coordinate to Zr clusters, resulting in an increased BET surface area (from 337.66 to 1,037.14 m 2 /g) and mesoporous ratio (from 34 % to 74 %) of the pristine UiO-67. Then, the graft of L-cysteine containing –COOH and –SH introduced more active adsorption sites. Moreover, the powder material was incorporated into sodium alginate aerogel beads which enhanced the recyclability and further improved the adsorption capacity for Pb(II), Cd(II) and Cu(II). These appealing advantages endow the adsorbent with quicker adsorption equilibrium (240 min), and outstanding removal capacities for Pb(II) of 661.2 mg/g, Cd(II) of 296.2 mg/g and Cu(II) of 326.4 mg/g. The chelation and ions exchange between the numerous functional groups including –COOH, –OH and –SH and the heavy metal ions are the main mechanisms for effective adsorption. This work provided a novel approach for the application of MOFs in environmental remediation.
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Journal of Materials Chemistry A
·
2023
·Vol. 12
·期 6
·3565-3574
·
IF 11.9
Ling-Chan Tian,Geqian Fang,Yun Zhou,Wenjun Yu,Lin Li,Jin-Nian Hu,Haiyan Wang,Jin-Xia Liang,Chun Zhu,Xiaodong Wang,Jian Lin
Direct selective oxidation of methane (DSOM) to oxygenates under mild conditions is garnering increasing interest. UiO-66-H MOFs are effective for this reaction, while the active configuration of Zr-oxo nodes with adsorbed ˙OH species need further clarification from the atomic/molecular viewpoint. Here, we detect the evolution of the geometric and electronic structures of adsorbed oxygenic species on Zr-oxo nodes of UiO-66-H via the controlled ˙OH species. DFT calculations reveal a volcano-like curve relationship between the quantity of ˙OH species and the DSOM performance, which is further corroborated by experimental tests. Zroxo-˙OH is the main active configuration on Zr-oxo nodes of UiO-66-H at low ˙OH concentration, while it evolves to other oxygenic species (˙OOH, O2, and H2O) due to the self-reaction with the increase of ˙OH concentration, which leads to performance decrease. Furthermore, a critical descriptor of the p-band centers of O atoms in these oxygenic species on the Zr-oxo nodes is established, which can well represent the catalytic activity for the DSOM reaction.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Xiangyu Wang,Min Jiang,Iseult Lynch,Zhiling Guo,Peng Zhang,Lisi Wu,Jun Ma
Although Fe/Fe 2 O 3 has potential application compared with nanoscale zero-valent iron (nZVI), its smooth structure largely limits the catalytic performance. To address this challenge, we innovatively constructed highly efficient composite Fe/Fe 2 O 3 @UiO-66 via employing an urchin-like core-shell structure of Fe/Fe 2 O 3 onto UiO-66 through a facile ion exchange precipitation method without inert gas protection. The characterization results show the urchin-like core-shell configuration can extend the life span of Fe 0 and produce more active sites. Besides, the absorption spectrum is broadened by Fe 2 O 3 which has narrow band gap and the high-efficiency separation of photogenerated electron-hole pairs is obtained with the load of Fe/Fe 2 O 3 . Moreover, Two-parameter pseudo-first-order decay model fits well with the reduction and adsorption of composites in the dark reaction, and a plausible pathway for tetracycline (TC) degradation is also proposed. The findings of this research provide a promising method for promoting the catalytic properties of MOF-based materials and Fe/Fe 2 O 3 .
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