Journal of Materials Chemistry A
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2018
·Vol. 6
·期 31
·15064-15073
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IF 9.931
Xu Jiang,Songwei Li,Shanshan He,Yongping Bai,Lu Shao
Both material choice and filler/organic interface are crucial in mixed matrix membranes (MMMs) for sub-nano-size gas separations and yet, the interface–performance relationship is still a subject of intense debate due to challenging interfacial detection. Herein, two UiO-66-type MOFs (amino-functionalized UiO-66-NH2 and isopropenyl-functionalized UiO-66-MA) are incorporated in cross-linked CO2–philic polyethylene oxide (PEO) matrix based on judicious material screening for CO2 capture. The reactive material UiO-66-MA is stitched together with methacrylate-capped PEO in situ during UV-induced copolymerization to generate highly efficient gas transport passages with conceivably good interfaces. Poor interface is observed by substituting UiO-66-MA with non-reactive UiO-66-NH2 in MPCM (MOF/polymer composite membrane). The interfacial conditions of CO2–philic MPCMs are carefully assessed via advanced physicochemical characterizations for clarifying the correlation between interface and separation performance. The reactive material UiO-66-MA containing MPCM with good interface demonstrates higher gas permeability (up to 1450 barrers) with similar selectivity (up to 45.8 for CO2/N2) when compared to non-reactive UiO-66-NH2 containing MPCM. The mixed gas test also shows high CO2 permeability of 1439 barrer and CO2/N2 selectivity of 37.6 in our MPCM. We also observe unexpected suppressed plasticization/swelling behaviour in UiO-66-MA containing MPCM and enhanced plasticization in UiO-66-NH2 containing MPCM through analysis of gas separation performance in the range of 1–10 atm, which might be utilized as a potential interface assessment tool for nanocomposites. Moreover, the performances of our CO2–philic MPCMs can be optimized further to surpass the (2008) Robeson Upper Bound for highly efficient sustainable CO2 capture.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Sijia Chen,Lin Zhang,Zhao Zhang,Gang Qian,Zongjian Liu,Qun Cui,Haiyan Wang
UiO-66 (UiO for University of Oslo) is a zirconium-based metal–organic framework with reverse shape selectivity, which gives an alternative way to produce high-purity n-heptane (nHEP) used for the manufacture of high-purity pharmaceuticals. A couple of studies have shown that UiO-66 gives a high selectivity on the separation of n-/iso-alkanes. However, the microporous structure of UiO-66 causes poor mass transport during the desorption process. In this work, hierarchical-pore UiO-66 (H-UiO-66) was synthesized and utilized as an adsorbent of nHEP and methyl cyclohexane (MCH) for systematically studying the desorption process of n-/iso-alkanes. A suite of physical methods, including X-ray diffraction patterns, verified the UiO-66 structures, and high-resolution transmission electron microscopy showed the existence of hierarchical pores. N2 adsorption–desorption isotherms further confirmed the size distribution of hierarchical pores in H-UiO-66. Of particular note, the MCH/nHEP selectivity of H-UiO-66 is similar to that of UiO-66 under the same adsorption conditions, and the desorption process of nHEP/MCH from H-UiO-66 is dramatically enhanced; namely, the desorption rates for nHEP/MCH from H-UiO-66 is enhanced by 30%/23% compared with UiO-66 at most. Moreover, desorption activation energy (Ed) derived from temperature-programmed desorption experiments indicate that the Ed for nHEP/MCH is lower on H-UiO-66; that is, the Ed of MCH on H-UiO-66 is ∼37% lower than that on UiO-66 at most, leading to a milder condition for the desorption process. The introduction of hierarchical structures will be applicable for the optimization of the desorption process during separation on porous materials.
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES
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2017
·
IF 2.603
Xiaolin Cao,Zejun Jiang,Shanshan Wang,Sihui Hong,Hui Li,Chao Zhang,Yong Shao,Yongxin She,Fen Jin,Maojun Jin,Jing Wang
UIO-66 crystals were explored for the first time to adsorb neonicotinoid insecticides in environmental water samples. HPLC coupled with tandem MS was used for quantification and determination of neonicotinoid insecticides. UiO-66 crystals was successfully synthesized by a simple constant-temperature bath method. Synthesized UiO-66 was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetry and nitrogen adsorption porosimetry (NAP), which demonstrated a uniform particle size, a large Brunauer–Emmett–Teller (BET) surface area and high thermostability . The adsorbing results showed that UIO-66 crystals could be used as a promising adsorbents for rapid extraction of neonicotinoid insecticides and be reused at least 10 times. Under the optimized conditions, the limits of detection (LODs, S/N = 3) and limits of quantification (LOQs, S/N = 10) for the five insecticides were found to be 0.02–0.4 ng/mL and 0.05–1.0 ng/mL, respectively. This developed approach not only provided more simple and sensitive method, as well as possessing satisfactory recovery for neonicotinoid insecticides, but also for other traces in environmental samples.
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JOURNAL OF POWER SOURCES
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2024
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IF 8.1
Yujuan Xie,Jinghua Han,Fengchao Li,Lingfei Li,Zhenghao Li,Qian Li,Zhaoting Shang,Wangting Lu,Yazhen Wang,Fan Yu,Wei Yan,Yun Zheng,Jiujun Zhang
Introducing advanced conductive nanoparticles to combine with metal-organic frameworks (MOFs) as electrode is emergingly regarded as a practical and efficient approach to improve the capacitive performance of supercapacitors. Herein, a new MOF (ZrNi-UiO-66, Nickel-zirconium 1,4-dicarboxybenzene) is designed to combine with carbon quantum dots (CQDs) to form a composite electrode with high specific capacitance, in which the charge regulation is performed to facilitate the electronic conduction and transfer. Such constructed electrode delivers an enhanced electronic conductivity and an improved specific capacitance of 2468.75 F g −1 @ 1 A g −1 , which is four times of the contrast sample. Meanwhile, the assembled hybrid supercapacitor exhibits an increased energy density and power density, as well as a sustainable stability after 10,000 cycles with a retention rate of 91.6 %. Basing on the study of advanced characterizations and density functional theory (DFT) simulation, the mechanism of significantly improved specific capacitance can be elaborated as the promote electronic conduction caused from narrowed band gap from 3.9 eV or 0.41 eV–0.23 eV, and the increased charge accumulation at the Ni sites in designed MOFs. This work provides new insights for the design and construction of potential energy storage materials based on MOFs and/or advanced carbon-based materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2017
·
IF 4.233
Jianhao Qiu,Yi Feng,Xiongfei Zhang,Mingmin Jia,Jianfeng Yao
UiO-66 was modulated by addition of acetic acid or HCl in the precursor solution. The resulting acetic acid-promoted UiO-66 has more regular octahedral structures and high surface areas of 892–1090 m 2 /g. Anionic dyes (methyl orange (MO) and Congo red (CR)) and cationic dyes (methylene blue (MB) and rhodamine B (RhB)) were examined for the selective dye adsorption on various UiO-66. The acid-promoted UiO-66 exhibits an excellent selective adsorption to anionic dyes, where the adsorption capacities of MO and MB are 84.8 and 13.2 mg/g, respectively. However, UiO-66 prepared without acid shows similar adsorption to both anionic dye MO (70.4 mg/g) and cationic dye MB (67.5 mg/g). Mixed dyes (MO/MB and MO/RhB) adsorption on acid-promoted UiO-66 further proves the selective adsorption to anionic dyes. The adsorption mechanism was studied by testing the Zeta potential of acid-promoted UiO-66, and more positive Zeta potential (hydrogen ions) of UiO-66 is beneficial to the anionic dye adsorption.
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Nanoscale
·
2016
·Vol. 8
·期 40
·17489-17495
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IF 7.76
Zhixiang Lu,Mingjiang Wu,Shuang Wu,Shaoxiong Yang,Yuan Li,Xiaolan Liu,Liyan Zheng,Qiue Cao,Zhongtao Ding
Transformation of aggregation induced emission (AIE) molecules into functional materials can greatly tune their fluorescence properties and expand their related potential applications. Here, we demonstrate a facile strategy to modulate the fluorescence properties of AIE molecules by confining them within the nanochannels of metal–organic frameworks (MOFs). AIE molecules (4,4′-(hydrazine-1,2-diylidene bis(methanylylidene)) bis(3-hydroxybenzoic acid), HDBB) with pH-dependent emission were successfully integrated into UiO-66 resulting in a UiO-66⊃HDBB complex while maintaining the crystal structure by the host–guest process. The fluorescence properties of HDBB can be modulated by virtue of the unique nanospace confining effect. Furthermore, UiO-66⊃HDBB was used as a sensitive and selective fluorescent probe for Cu2+ detection in aqueous solution. This study provides a facile strategy for the construction of high performance AIE based luminescent materials with adjustable properties for potential applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Douhao Yang,Ruiting Jian,Jianjun Yan,Ao Zhang,Bowen Liu,Zhongwei Liu
Defect engineering has a great effect on the properties of metal–organic frameworks (MOFs). In this study, the defective UiO-66-NH2 MOFs are successfully prepared by a rapid Ar plasma modification method. At certain experimental conditions (15 W radio frequency input power, 20 Pa working pressure, and 120 s Ar plasma modification time), the afforded UiO-66-NH2 shows significant enhancement in photocatalytic reduction of Cr(VI), and a maximum reduction efficiency of 68.5% is obtained. Advanced characterizations show that the plasma treatment generates missing-linker defects within the UiO-66-NH2 structure, which can enhance the separation of photogenerated electrons and holes and improve the photoreduction capability. The findings not only contribute to a better understanding of the relationship between the structure and performance of MOFs but also provide a simple approach for defect engineering of MOFs.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xingmao Zhang,Hang Wang,Qi Wang,Longyu Wang,Hongxiang Cui,Xiaopeng Sun,Jialong Ling,Dongmin Bian,Ziyi Zhang,Chuan-De Wu
Salinity gradient energy (SGE) harvesting from water has long been sought as a clean energy source. Commercial ion exchange membranes often face high energy barriers, inadequate ion transport ability, and chemical instability, thus displaying low power outputs. In this study, a series of continuous, flexible, zirconium-based metal–organic frameworks (Zr-MOFs) were synthesized on reduced graphene oxide membranes via electrochemical synthesis for highly efficient SGE harvesting are developed. The well-defined nanoscale channels and functional groups act as ionic filters and conductors, enhancing the ion selectivity for highly efficient SGE harvesting. Notably, the SO 3 H-UiO-66 membrane achieved a power density of 57.5 W/m −2 in neutral solution under a 1000-fold KCl concentration gradient, with a high K + transference number of 0.92, outperforming most reported membranes. Furthermore, the SO 3 H-UiO-66 membrane demonstrates a high output power density of 16.2 W/m −2 when tested with real seawater (Huang Hai) and domestic water, and is also effective in harvesting energy from wastewater, achieving a power density of 17.3 W/m −2 . This study opens new avenues for fabricating continuous Zr-MOF membranes as a platform for utilizing seawater and wastewater sources in SGE harvesting.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Guowei Shan,Xiao Xiao,Hong Gao,Qi Zhang,Houyi Peng,Weixing Li
Heavy metal ion (HMI)-contaminated wastewater is a great threat to public health. Membrane separation is an efficient and green technology for HMI removal. Here, the strategy of nanoparticle in-situ growth combined with molecule grafting was proposed to fabricate the UiO-66-NH 2 -g-DTPA/PES composite membrane. The UiO-66-NH 2 nanoparticles bound within the PES membrane substrate uniformly brought a significant number of primary amino groups, providing abundant graft sites for DTPA molecule. Numerous carboxyl groups and tertiary amine groups were introduced as the result of DTPA grafting, enabling the formation of M−DTPA complexes with HMIs. The fabricated UiO-66-NH 2 -g-DTPA/PES membranes exhibited excellent performances. The pure water flux arrived at 6208 L·m −2 ·h −1 and the efficiencies of removing Cu 2+ , Pb 2+ , Cr 3+ and Cd 2+ were 99.73%, 99.79%, 96.91% and 98.33%, respectively. Moreover, the UiO-66-NH 2 -g-DTPA/PES membrane also showed a remarkable stability in pH conditions ranging from 3 to 10 and remained a relatively high performance in the cyclic test.
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INORGANICA CHIMICA ACTA
·
2024
·
IF 2.7
Guang-Li Zhou,Bo-Wen Liu,Guang-Yu Cui,Wei Zhang,Ji-Min Yang
Radioactive iodine waste from the nuclear industry poses a critical threat to human health, and its effective capture has become an important research topic. In this study, modified UiO-66-X adsorbents (where X is ATA, BTA, or STA) were used to investigate the effects of the free functional groups in the UiO-66 skeleton on iodine capture in the vapor and solution states. The adsorption behavior revealed that the capture efficiency of UiO-66-ATA was substantially higher than that of UiO-66-BTA and UiO-66-STA because the electron-donating amino groups could enhance the I − I···π halogen bond interactions compared with the electron-withdrawing carboxyl and sulfonic acid groups. In addition, the pore volume of UiO-66-ATA was significantly higher than those of UiO-66-BTA and UiO-66-STA. In particular, the removal uptakes of UiO-66-ATA were 1108.1 mg/g (vapor phase) and 3601.9 mg/g (aqueous solution). This study is the first to investigate the effects of functional groups on the adsorption uptake of UiO-66 toward iodine. This efficient functional group modification strategy holds significant promise for the development of novel metal–organic framework adsorbents.
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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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