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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
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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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
·
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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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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INORGANICA CHIMICA ACTA
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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 Water Process Engineering
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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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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yongchao Sun,Xudong Bi,Lu Bai,Tianyou Li,Fangxu Fan,Zeyuan Gao,Yijun Liu,Jianyu Guan,Fake Sun,Hongjin Li,Gaohong He,Canghai Ma
Membrane separation technology holds great potential for CO 2 capture and H 2 separation due to its simplified process, low energy consumption, and environmental benefits. Consequently, there is a pressing demand for membranes with ultra-high gas separation performance that can surpass the Robeson upper bound. To address this challenge, mixed matrix membranes (MMMs) were designed by combining rigid bridging ring polymer-Tröger’s base (TB) polymer with UiO-66 or UiO-66-Br to enhance gas separation properties of membranes. DFT calculations reveal that the interaction energy between UiO-66-Br ligands and TB is significantly lower than that of UiO-66 ligands with TB, suggesting the stronger interaction between the UiO-66-Br and TB polymer. The addition of UiO-66-Br enhances gas separation performance by providing additional gas transport pathways and increasing molecular sieving through its optimized pore size and functional groups. As a result, MMMs with a 40.0 wt% MOF loading exhibit CO 2 and H 2 permeabilities of 764.4 and 1127.8 Barrer, respectively, along with CO 2 /CH 4 , CO 2 /N 2 , H 2 /CH 4 , and H 2 /N 2 selectivities of 15.6, 19.1, 23.0, and 28.2, surpassing the 2008 Robeson upper bound. Compared to TB membranes, the permeability of H 2 and CO 2 in the MMMs increased by over 247% and 222%, demonstrating exceptional gas separation performance. The design approach in this study offers an effective pathway for fabricating MMMs with high gas separation performance for efficient CO 2 capture and H 2 separation.
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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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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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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Keli Li,Mengli Li,Changsheng Su,Long Deng,Zheng Yan,Hongxia Shen,Yang Jiao,Xuebo Cao
Abundant porosity, sufficient active sites, and appropriate stability are crucial factors for metal–organic frameworks (MOFs) designed for photocatalysis. Herein, a controllable partial pyrolysis strategy was employed to synthesize hierarchically porous UiO-66-X (X denotes the mass ratio of H2BDC-NH2 in ligands) with adjustable coordinated unsaturated zirconium sites and interconnected mesoporous structure. By taking full advantage of linker instability in MOFs, which is usually viewed as an undesirable trait of MOFs, this controllable thermolysis involved heat treatment of the original UiO-66-X, leading to selective partial decomposition and permanent mesopores within the structure. Meanwhile, dangling functional amino groups could serve as anchoring sites for cocatalyst and CO2 molecules. Cu nanoclusters were successfully incorporated into hierarchically porous MOFs by a structure engineering approach, yielding a novel photocatalyst. A mutually active mechanism was put forward and illustrated in this work. Mechanistic investigation reveals that mesoporous structures in a catalyst not only offer three-dimensional (3D) interconnected gas transport channels but also provide sufficient space for accommodating the introduced Cu nanoclusters, which served as active sites and efficiently induced a CO2 photoreduction reaction. At the optimal ratio, the photocatalyst exhibited superior photocatalytic activity, achieving a CO yield of 121.64 μmol g–1 under 5 h of the stimulated solar irradiation without any photosensitizer.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
·
IF 4.3
Wen Yun,Wanshan Wang,Yiyan Lin,Ruiqi Wang,Xia Ha,Li Yang,Yue Jiang,Xin Zhang
A catalytic hairpin self-assembly (CHA) amplification method was developed for CAP detection based on cross-shaped DNA and UiO-66. MOF was used to quench the fluorescent signal of FAM labeled DNA. Cross-shaped DNA with four fluorophore group (FAM) was utilized to enhance the fluorescent intensity. CAP could open hairpin structure of H-apt and induce CHA reaction. The product of CHA hybridized with cross-shaped DNA, resulting its leaving from the surface of UiO-66 and recovery of fluorescent signal. The limit of detection (LOD) was low to 0.87 pM. This method had been successfully applied for the detection of CAP in actual samples. Importantly, the high sensitivity was attributed to the great amplification efficiency of CHA, strong fluorescent intensity of cross-shaped DNA structure and great fluorescent quenched efficiency of UiO-66.
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JOURNAL OF POWER SOURCES
·
2024
·
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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