ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 1
·2283-2297
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IF 5.19
Hu Yuting,Wang Shixing,Zhang Libo,Yang Fan
In wastewater, heavy metal Hg causes serious harm to ecology, so it needs to be removed. In this paper, a novel MOF adsorbent (UiO-66-QU) was prepared by modifying UiO-66-NH 2 with 4-quinolinecarboxaldehyde, which was used to selectively remove Hg(II) from water. The adsorbent was characterized using Fourier transform infrared spectroscopy (FT-IR), field emission scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), zeta potentiometer, and X-ray photoelectron spectroscopy (XPS). In order to investigate the Hg(II) adsorption performance of UiO-66-QU, the effect of time, initial concentration, pH, and temperature were carried out. Langmuir model fitting shows that the maximum adsorption capacity of UiO-66-QU for Hg(II) is 556 mg/g at 298 K. The experimental results show that UiO-66-QU has better Hg(II) adsorption capacity than UiO-66-NH 2 . The isotherm is in accordance with pseudo-second-order models. It is indicated that the adsorption process is mainly monolayer chemical adsorption. The thermodynamic parameters also indicate that the adsorption process is spontaneous and endothermic. It has excellent reusability and selectivity. XPS and the zeta potential showed that the adsorption mechanism was the complex reaction of Hg(II) with nitrogenous group. Therefore, the adsorbent has potential application prospects in removal of Hg(II) from wastewater.
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高影响因子
Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Jiayou Liu,Xiaoxiang Huang,Linfeng Liu,Qianqian Nie,Zhongchao Tan,Hesheng Yu
UiO-66 variants are widely used for photocatalysis and adsorption, but few studies reported their combined effects in one process. This paper reports that the mechanism behind NO removal using UiO-66-NH 2 includes photocatalytic oxidation and subsequent adsorption. First, the UiO-66-NH 2 was selected out of UiO-66-X variants (X = H, NH 2 , NO 2 , OH, Br, Br 2 ) because of its high NO removal efficiency ( i.e ., 80.54%), which is 8.55–64.95 times higher than those of other UiO-66 variants. Then, the NO reaction pathway and degradation mechanisms are proposed based on the experimental results and theoretical calculations. In an anhydrous environment, the NO removal efficiency increases from 80.54% at 40–60% of humidity to 96.23%. Moreover, NO 2 emissions and catalyst deactivate are not observed. These findings indicate that the photocatalytic NO degradation includes the photocatalytic oxidation of NO into NO 2 on the surface of UiO-66-NH 2 and subsequent NO 2 adsorption in micropores. The reason is that the formation of NO x - ions without H 2 O is theoretically impossible according to the principle of electroneutrality. In-situ DRIFTS also confirms the mechanism. Furthermore, density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulations were carried out to understand the improved NO removal caused by synergistic photocatalysis and adsorption. In summary, this work proposes a new mechanism for NO removal that combines the photocatalytic oxidation and adsorption capability of UiO-66-NH 2 , the new mechanism provides a new strategy to further improve the NO removal efficiency of UiO-66-NH 2 and a new way of inhibiting the deactivation.
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DESALINATION
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2022
·
IF 11.211
Xiaowen Huo,Zhaojing Jing,Haitao Wang,Na Chang
Nanofiltration membranes based on polyamide (PA) are widely used in fields such as brackish water desalination and drinking water purification due to their excellent retention of multivalent salts. However, uncontrolled and extremely fast polymerization easily produces thicker PA layers, which reduces permeability. Moreover, smooth support layer usually leads to PA layers with low roughness, which is not benefit for improving of flux. Based on these aspects, an innovative method of co -regulating interfacial polymerization based on anionic surfactant sodium dodecyl sulfate (SDS) and carbonized-UIO-66 (C-UIO-66) nanoparticles has been reported. The adsorption of anionic surfactant on the surface of C-UIO-66 slows down the diffusion rate of aqueous monomer and helps to form thin PA layer (<33 nm) which is thinner than the original thin film composite (TFC) membrane (144.29 ± 17.62 nm). Besides, C-UIO-66 nanoparticles with different sizes are deposited on the surface of the support layer, providing rougher surface for interfacial polymerization. Due to the irregular surface of SDS/C-UIO-66 intermediate layer, the prepared PA layer has folded structure. Compared with original TFC membrane, the preferred thin film nanocomposite (TFN) nanofiltration membrane possesses permeation flux of 58.59 L·m −2 ·h −1 , which increased by 114.3 % together with the maintaining the rejection rate of Na 2 SO 4 above 96 %.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Mingming Peng,Deng You,Hui Shi,Penghui Shao,Wei Ren,Liming Yang,Xin Sheng,Jiachuang Shao,Xuan Ding,Lin Ding,Haozhi Wang,Kai Yu,Xubiao Luo
Metal-organic frameworks (MOFs) with ability to create rich defects in the structures for exposed binding sites are beneficial for wastewater treatment. However, the inter-relation between the defect concentration and heavy metal removal performance still deserves the exploration. Herein, UiO-66-X crystal materials are successfully synthesized in the presence of monocarboxylic acid of acetic, benzoic, and trifluoroacetic acid, and the effect of defect concentration on Sb(V) removal performance is systematically studied. XRD, TG, EPR and XPS characterizations reveal that the addition of modulators increases the content of defects in the UiO-66-X, which is beneficial to improve the sites utilization. As expected, the Sb(V) adsorption properties of UiO-66-AA, UiO-66-BA and UiO-66-TFA are boosted by 54.1%, 140.0% and 197.7% compared to that of pristine UiO-66. Density functional theory (DFT) calculations further confirm that UiO-66-TFA with the most defects exhibits lower adsorption energy and higher charge transfer, significantly improving the uptake performance of Sb(V). Additionally, the UiO-66-TFA successfully removes antimony in actual water from the Tianyi Lake and Ganjiang River with residual concentrations below 5 μg L −1 , meeting the drinking water standard. This work provides guidance for the rational selection of modulators for efficient heavy metal removal from wastewater.
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Journal of CO2 Utilization
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2022
·
IF 8.321
Nicui Yuan,Yuxin Mei,Yuwei Liu,Yating Xie,Baining Lin,Yonghua Zhou
The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO 2 . In this paper, a composite catalyst UiO-66-NH 2 /Ce(HCOO) 3 (simplified to UNH/Ce(HCOO) 3 ) was fabricated by one pot method with CeCO 3 OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO) 3 and strongly interacted with it via Ce-N bond. The yield of CH 4 on the optimal UNH/Ce(HCOO) 3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g −1 , with the CH 4 selectivity of 71.9 %, and the R electron reached 286.46 μmol g −1 h −1 . The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO 2 reduction performance and high CH 4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO) 3 with abundant Ce 3+ , which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO 2 to CH 4 . In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO) 3 -1.80 by decreasing reaction temperature.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Shao-zhong Hu,Ting Huang,Nan Zhang,Yan-zhou Lei,Yong Wang
The discharge of wastewater rich in heavy metals and organic substances has led to the deterioration of the ecosystem, resulting in serious environmental and food pollution, and there is an urgent need to treat the pollutants in the wastewater. Metal organic frameworks (MOFs) have the advantages of large specific surface area and pore volume, as well as the designability of their structures, and are extremely promising materials for wastewater treatment. In this work, a novel adsorbent was synthesized by grafting polyethyleneimine (PEI) onto the UiO-66-NH 2 metal framework (PEI@UiO-66-NH 2 ) via glutaraldehyde-assisted reaction. This new type of adsorbent not only exhibits improved chemical stability in water but also shows greatly increased adsorption sites in comparison with the common UiO-66-NH 2 . The various factors that possibly affect the adsorption behaviors of the PEI@UiO-66-NH 2 were systematically studied. The results show that the PEI@UiO-66-NH 2 can nearly reach the adsorption equilibrium of Pb(II) and methyl orange (MO) within 5 min. The theoretical adsorption capacities toward Pb(II) and MO achieve 692.80 mg/g and 497.51 mg/g, respectively. Specifically, the dynamic theoretical adsorption models were established through the study of the dynamic adsorption of pollutants, providing the theoretical guidance for the scale-up experiments of wastewater treatment with this adsorbent. PEI@UiO-66-NH 2 also shows excellent recycling performance for removing Pb(II) and MO. All these results suggest that PEI@UiO-66-NH 2 has a good application prospect for the removal of wastewater containing Pb(II) and MO.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Xiaodong Zhang,Fukun Bi,Zhenyuan Zhao,Yang Yang,Yintao Li,Liang Song,Ning Liu,Jingcheng Xu,Lifeng Cui
Supported single-atoms and sub-nanometre clusters have exhibited superb catalytic performance toward many reactions. However, inactivation of single-atom or cluster catalysts in complex reactive conditions poses major challenge for their practical application. Herein, we demonstrate that the prepared Pd-UiO-66 with ultra-low Pd loading (0.05 wt%) contains three robust active Pd species, (isolated Pd atom (Pd 1 ), sub-nanometre Pd clusters (Pd c ) and Pd nanoparticles (Pd n )) and presents superb activity for toluene oxidation and water resistance (10.0 vol%). Experiments and theoretical calculations firstly confirm that consecutive H 2 -O 2 and reaction gas treatment (1000 ppm toluene in 20 vol.%O 2 /Ar) induce residual N species from solvent N, N-dimethylformamide to enter UiO-66 skeleton forming Pd 1 -N 1 structures. DFT calculations reveal that the synergistic effect of Pd species (namely, the enhanced activation of O 2 and H 2 O by Pd 1 and the improved adsorption of toluene by Pd c and Pd n ) is the main factor for the excellent activity of Pd-U-H-O-reused catalyst.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Si-Yuan Fang,Ji-Lai Gong,Lin Tang,Wei-Cheng Cao,Juan Li,Zi-Kang Tan,Yu-Wen Wang,Wen-Bo Wang
Thin-film nanocomposite (TFN) membranes with efficient molecular separation and organic solvent resistance are active in demand in wastewater treatment and resource reclamation, meeting the goal of emission peaks and carbon neutrality. In this work, a simple and rational design strategy has been employed to construct a sandwich-structured membrane for removing fluoroquinolone antibiotics and recycling organic solvents. The sandwich-structured membrane is composed of a porous substrate, a hydrophilic tannic acid–polyethyleneimine (TA–PEI) interlayer, and a polyamide (PA) selective layer decorated with metal–organic framework (PA-MOF). Results manifest that the hydrophilic TA–PEI interlayer played a bridging and gutter effect to achieve effective control in amide storage, amine diffusion, and nanomaterial downward leakage at the immiscible interface. The PA-MOF selective layer has been changed to a loosely crumpled surface, endowing functionalities on the sandwich-structured membrane that included limited pores, strengthened electronegativity, and stronger hydrophilicity. Thus, an enhanced water flux of 87.23 ± 7.43 LMH was achieved by the TFN-2 membrane (0.04 mg·mL–1 UiO-66-NH2), which is more than five times that of the thin-film composite membrane (17.46 ± 3.88 LMH). The rejection against norfloxacin, ciprofloxacin, and levofloxacin is 92.94 ± 1.60%, 94.62 ± 1.29%, and 96.92 ± 1.05%, respectively, effectively breaking through the “trade-off” effect between membrane permeability and rejection efficiency. Further antifouling results showed that the sandwich-structured membrane had lower flux decay ratios (3.36∼7.07%) and higher flux recovery ratios (93.40∼98.40%), as well as superior long-term stability after 30 days of filtration. Moreover, organic solvent resistance testing confirms that the sandwich-structured membrane maintained stable solvent flux and better recovery rates in ethanol, acetone, isopropanol, and N,N-dimethylformamide. Detailed nanofiltration mechanism studies revealed that these outstanding performances are based on the joint effect of the TA–PEI interlayer and PA-MOF selective layer, proposing a new perspective to break through the bottleneck of nanofiltration application in a complex environment.
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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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MOLECULES
·
2021
·Vol. 26
·期 19
·5736
·
IF 4.412
Chunhua Wang,Zhiquan Yu,Yuhao Yang,Zhichao Sun,Yao Wang,Chuan Shi,Ying-Ya Liu,Anjie Wang,Karen Leus,Pascal Van Der Voort
Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2reduction. The obtained Pd/UiO-66-NO2catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.Keywords:Pd/UiO-66-NO2;furfural;hydrogenative ring-rearrangement;cyclopentanone;double-solvent method
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiuling Zhang,Xiaoke Hao,Zhenyu Zhai,Jiaona Wang,Huiyu Li,Yaxin Sun,Yue Qin,Ben Niu,Congju Li
Wearable electronics based on metal–organic frameworks (MOFs) capable of monitoring various environmental pollutants is a promising approach for realizing gas sensing of chemical information. However, their sensing application combined with electronic textile with breathable, washable and flexible features has not been completely established yet. Herein, we describe a facile and effective strategy to fabricate flexible gas sensor for rapidly detecting hydrogen sulfide (H 2 S) through integrating NO 2 -UiO-66 on electrospun nanofibers membrane (NO 2 -UiO-66 NM) firmly and uniformly. Different from the inherent brittleness and poor processability of powder MOFs, the achieved NO 2 -UiO-66 NM delivers enhanced porosity and surface area, outstanding flexibility, desirable breathability, stable to washing and strong accessibility, more suitable for practical applications. Consequently, the fabricated NO 2 -UiO-66 NM sensor exhibits a significantly high detection selectivity for H 2 S among various analytes (H 2 S, SO 2 , C 6 H 6 , CO and NH 3 ) and remarkable sensitivity for H 2 S with unprecedentedly ultralow detection limit reaching down to 10 ppb. Moreover, the sensing performance can be greatly remained after around five weeks at concentration down to 1 ppm; also, there are slight impact of deformation on sensing activities, revealing superior H 2 S sensing stability. This study offers a feasible solution to develop electronic textiles for chemical sensing application.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Run-dong Ding,Dan-dan Li,Yu-lin Li,Jie-hui Yu,Ming-jun Jia,Ji-qing Xu
Ultrafine and well-dispersed PdAu bimetallic nanoparticles (ca. 1.4 nm) are successfully immobilized on amine-containing UiO-66 frameworks (NH2-UiO-66) via a double-solvent impregnation method. By virtue of the double-solvent strategy, the incorporated PdAu nanoparticles (NPs) are mainly present in the alloy state and distributed inside the cavities of NH2-UiO-66 near the window of the cages. The resulting PdAu/UiO-66 catalysts exhibit much higher catalytic activity and stability for the dehydrogenation of formic acid than the catalyst prepared by the conventional single-solvent impregnation method. The composition-optimized Pd0.8Au0.2/UiO-66-D catalyst affords a very high turnover frequency value of 722 h–1 at 298 K, which is among the highest one in the metal–organic framework-supported Pd-based NP catalysts ever reported under similar reaction conditions. The exceptional catalytic activity and stability of Pd0.8Au0.2/UiO-66-D could be mainly attributed to the formation of highly dispersed PdAu alloy NPs, the suitable electronic structure of Pd species adjusted by the alloy effect, and the metal–support interaction, as well as the abundant amine groups that can promote the activation of the formic acid molecule by forming HCOO– under mild conditions.
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危险品化学品经营许可证（带存储）