Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 42
·22859-22867
·
IF 11.9
Jinhong Yang,Haoran Peng,Chong Lin,Qingjiang Pan,Lixue Qi,Li Li,Keying Shi
To overcome the drawbacks of low sensitivity and limited selectivity exhibited by metal oxide sensitive materials, a metal–organic framework (MOF) derived composite (marked as UZZ) was constructed via a combined wet chemical method. UiO-66 was used as the precursor with the introduction of ZnO. The ZrO2 component in UZZ retains the unique octahedral configuration of UiO-66; on its folded surface, a large number of ZnO particles grow, whose sizes range from 20 to 40 nm. The composite exhibits excellent gas sensitivity to NO2 at room temperature. Exemplarily, the gas sensitive response to 100 ppm NO2 is 40.35, with a response time of 1.4 s and a detection limit as low as the 50 ppb level, and the stability is up to 8 weeks. The presence of numerous oxygen vacancies and n–n type heterojunctions on the surface of the UZZ composite synergistically enhances the gas-sensing performance. This finding provides a significant reference for developing new efficient and high-sensitivity metal oxide sensitive materials based on MOFs.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qian Hu,Xuejiao Wang,Yuxuan Zheng,Tianyu Zhao,Jin Qu,Zhong-Zhen Yu,Dongzhi Yang
As chemical warfare agent (CWA) is one of deadly chemicals with strong toxicity and fast action, it is imperative to develop catalytic protective materials that can quickly adsorb and efficiently detoxify CWAs. Herein, reduced graphene oxide (RGO) aerogels are decorated with UiO-66-NCS metal–organic framework with high catalytic activity by in situ growing UiO-66-NH 2 inside the RGO hydrogels, converting the UiO-66-NH 2 to more active UiO-66-NCS, and freeze-drying for realizing solar-thermally enhanced catalytic hydrolysis of dimethyl 4-nitrophenyl phosphate (DMNP), a chemical warfare agent simulant. Compared with UiO-66-NH 2 , the UiO-66-NCS is more efficient in catalytically hydrolyzing DMNP with a 30 % accelerated half-life, and the in situ decoration of the RGO aerogel with UiO-66-NCS further improves the catalytic hydrolysis efficiency because of the more exposed active sites of the UiO-66-NCS. Furthermore, the excellent solar-thermal conversion effect of the RGO porous substrate can rapidly generate heat and transfer it to the UiO-66-NCS catalyst, thereby promoting the catalytic activity of the catalyst. The UiO-66-NCS decorated RGO aerogel exhibits a great detoxification efficiency of DMNP under simulated solar light irradiation with a turnover frequency of as high as 0.0531 s −1 , ∼2.3 times higher than that under room light, and 1.5 times better than that of UiO-66-NCS powder. The solar-thermally enhanced catalytic hydrolysis of DMNP with the UiO-66-NCS decorated RGO aerogel is demonstrated by the quick detoxification of CWA simulant with great recyclability.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Fei Tong,Zan Yang,Zheng Wang,Wenya Liu,Wanqi Jiang,Lu Zhu,Lei Wang,Mingming Zheng,Ruyan Hou,Yibin Zhou,Yingnan Liu
In view of the potential hazards of organophosphorus pesticides (OPs), this paper constructed a ratiometric fluorescent probe utilizing a functionalized metal–organic framework to detect OPs. Ru(bpy) 3 Cl 2 was encapsulated inside UiO-66 as a reference signal, and MnO 2 nanosheets (MnO 2 NSs) were grown on the surface to obtain [email protected] @MnO 2 NSs. Acetylcholinesterase catalyzed the decomposition of acetylcholine into reductive thiocholine, which consumed MnO 2 NSs, thus restoring the [email protected] fluorescence. Due to the enzymatic inhibition of OPs and the redox reaction between MnO 2 NSs and thiamine, this probe emitted blue fluorescence in the presence of OPs. The probe achieved linear responses to dichlorvos and chlorpyrifos with LODs of 9.99 × 10 -6 μg mL −1 and 9.99 × 10 -5 μg mL −1 . The probe exhibited a satisfactory recovery rate for OPs in green tea. Furthermore, a hydrogel detection platform was developed by embedding the probe into sodium alginate. Overall, this work provides a visual approach to detect OPs in agricultural products.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Shiwei Tian,Yaqi Zhang,Qiankun Sha,Tian Yang,Yan Huang,Xingxiang Zhang,Wei Wang,Na Han
Highly efficient treatment of oil-water emulsions in severe environments (organic solvents, strong acids) is recognized as a challenging subject. Polyphenylene sulfide (PPS) is an ideal membrane material with superior thermal stability as well as chemical resistance that is expected to settle this challenge. However, the hydrophobicity of PPS (h-PPS) membrane inherently prevents its efficient treatment of oil-in-water (O/W) emulsions. In this study, superhydrophilic modification of PPS substrates was achieved by in situ electrostatic self-assembly of hydrophilic Zr-MOFs to obtain UiO-66-NH 2 @h-PPS membranes. The introduction of UiO-66-NH 2 crystals constructed the micro/nanoscale hierarchical structure for the substrate, which transforms the PPS substrate from a hydrophobic to a superhydrophilic state (water droplets require only 0.6 s to be completely immersed in the membrane). Meanwhile, the UiO-66-NH 2 @h-PPS membranes gain under-water superhydrophobicity (the under-water oil contact angle exceeds 150° for toluene, hexane , dichloromethane , and carbon tetrachloride , of which toluene reaches 163.1°), thereby improving wettability selectivity and decreasing oil adhesion, permitting the fabricated UiO-66-NH 2 @h-PPS membranes to effectively separate different types of O/W emulsions. The UiO-66-NH 2 @h-PPS membranes acquire excellent permeate fluxes (for the surfactant-free toluene-in-water emulsion, it reaches up to 7638.1 L m −2 h −1 ) and separation accuracy (99.1% oil rejection). Moreover, the UiO-66-NH 2 @h-PPS membrane exhibited outstanding harsh environment resistance. Interestingly, the combination of UiO-66-NH 2 and h-PPS substrate was applicable to degrade the organic compound in water, and the degradation efficiency of the methylene blue achieved 85.7% under visible light within 120 min. In summary, loading Zr-MOFs onto h-PPS substrates provides a novel strategy for the efficient treatment of wastewater under complex conditions with great potential for practical applications.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 30
·10472-10480
·
IF 4
Pingping Teng,Ying Liu,Zhongqiao Sun,Hao Meng,Yide Han,Xia Zhang
Development of binary MOF-on-MOF heterostructures is a research hotspot in MOFs chemistry due to the advantages elicited by a closely connected interface, which may endow more abundant functionality and even broader applications in interface chemistry. A MOF-on-MOF heterostructure was constructed by in situ growth of MIL-88B on the outer surface of UiO-66. The resultant MIL-88B@UiO-66 produced had an interesting flower-like morphology composed of MIL-88B (petal) on tetrahedral UiO-66 (core). The MIL-88B@UiO-66 heterostructure showed adsorption and Fenton-like oxidation abilities, with distinctly improved structural stability in aqueous solution compared with that of single MIL-88B. Methylene blue (MB) was selected as the target molecule to evaluate the adsorption and Fenton-like oxidation activities. The efficiency of total removal of MB was studied systematically under various operating conditions and the influencing factors were optimized. The kinetics of adsorption and catalytic oxidation were simulated to explore the interactions between MB and MIL-88B@UiO-66. The mechanisms of enhanced adsorption and Fenton-like oxidation were suggested. The cyclic removal performance and structural stability of MIL-88B@UiO-66 were also determined.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 29
·13855-13865
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IF 3.3
Yong Cheng,Lin Deng,Dan Wang,Changchun Ji,Ying-Hua Zhou
The development of advanced catalysts is essential for efficient elimination of the emerging organic pollutants in water. Herein, Cu9S5 and Cu9S5@UiO-66-NH2 were prepared and both exhibited high Fenton-like photocatalytic activities for the degradation of organic contaminants. Removal efficiencies of 85% and 92% were achieved for Congo red (CR) and Rhodamine B (Rh B), respectively. It is found from active species trapping experiments and electron spin resonance (ESR) analysis that ˙O2−/h+ and ˙O2−/˙OH played key roles in the oxidation reaction of these two pollutants, respectively. The mechanisms were discussed on the basis of the cycles of Cu+/Cu2+.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Sijia Liu,Xifei Zhou,Changqing Yang,Chaohai Wei,Yun Hu
The extensive use of sacrificial agents and the low carrier separation and utilization efficiency remain important factors limiting the development of photocatalytic hydrogen production . We report a three-layered, dual-functional photocatalysts of Cu atomics@UiO-66-NH 2 (U6N)/ZnIn 2 S 4 nanosheets (ZIS), for the simultaneous production of photocatalytic hydrogen and degradation of organic pollutants . When common and highly toxic organic pollutants (phenolic compounds and antibiotics) were substituted for the sacrificial agents, Cu@U6N/ZIS exhibited superior sustained hydrogen production, approximately 28 times greater than that of pure ZIS. The experimental results suggested that the window size of U6N (< organic pollutants molecular size) separates the reaction sites of organic pollutants oxidation and reduction of hydrogen ions (H + ), thereby achieving spatial separation of redox sites. Besides, the structure of Cu@U6N/ZIS, which was anchored Cu within U6N and encapsulated by ZIS nanosheets, forming Z-type heterojunctions, achieved the control of the directional transfer of photogenerated electrons. And the coupled system can effectively enhance water quality by reducing the biological toxicity of the wastewater. This study suggests new avenues for environmental restoration and non-fossil fuel production.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 3.9
Chang Liu,Xiaoyue Zhang,Yu Zhou,Lin Zhu,Chengyu Zhang,Xiaohui Yan,Shengping You,Wei Qi,Rongxin Su
The enzyme leakage in physical adsorption dramatically limits the application of immobilized laccase (Lac) in environmental treatment. Therefore, a leakage-proof Zr-based metal-organic framework (MOF) carrier, UiO-66-NH 2 (30), was constructed for the stable loading of Lac and efficient antibiotic biodegradation, which could fix the Lac inside the carrier rather than only adsorbed on the surface. Based on the aperture modulation strategy, the pore size distribution of MOFs at about 10 nm was significantly increased to match the diameter of Lac (7.6 nm), by which Lac@UiO-66-NH 2 (30) was successfully prepared with a high enzyme loading amount (275.96 mg/g) and high enzyme recovery (618 %). The immobilized Lac@UiO-66-NH 2 (30) could nearly 100 % biodegrade rifampicin and lincomycin in 6 min and 6 h, respectively, and after 8 times reuse, the degradation rates of antibiotics remained at 81.46 % and 76.12 %, which showed excellent reusability and stability. Overall, Lac@UiO-66-NH 2 (30) is expected to be an ideal candidate for pollution control.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenqing Hou,Chen Chen,Diya Xie,Yiming Xu
Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH2 (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl4, followed by amination. The solid had a high surface area (828–937 m2/g) and a large pore volume (0.451–0.507 m3/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H2O reduction and oxidation on a film electrode, respectively. However, such a change for H2 evolution in a Na2S/Na2SO3 aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Chuan Yu,Hongxu Liu,Jiafei Lyu,Zixing Xiao,Peng Bai,Xianghai Guo
A series of alkoxy groups are introduced to the UiO-66 structure to enhance its adsorption performance toward acetic acid in water. The adsorption kinetics, isotherm, thermodynamics, and regeneration of these adsorbents have been investigated, and the excellent adsorption capacity of n-propyloxy-substituted adsorbent (UiO-66-3) is illustrated. The adsorption of acetic acid on UiO-66-3 was a complex multistep process, and the close contact between O of the ether bond of the adsorbent and H of the carboxyl group of acetic acid played an important role in adsorption. The kinetic results could be fitted well to the pseudo-second-order model. The adsorption isotherm followed the Langmuir isotherm, which indicated that the adsorption process involved a strong interaction between adsorbate and adsorbent. The thermodynamic parameters (ΔG, ΔH, and ΔS) had also been calculated, which verified that acetic acid adsorption on UiO-66-3 was a spontaneously endothermic process. The adsorbent exhibited good stability under specified experimental conditions, which consolidated its potential as a solution to wastewater containing dilute acetic acid.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 20
·7770-7777
·
IF 3.069
Shi-Wen Lv,Jing-Min Liu,Chun-Yang Li,Hui Ma,Zhi-Hao Wang,Ning Zhao,Shuo Wang
A novel magnetic nanocomposite named Fe3O4@UiO-66-SO3H with a core–shell structure was first synthesized via a feasible step-by-step assembly strategy, and then employed as an adsorbent to remove methylene blue (MB) from aqueous solution. The characterization by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and Fourier transform infrared (FT-IR) spectroscopy proved that the Fe3O4@UiO-66-SO3H core–shell nanocomposite was successfully prepared. And the as-synthesized Fe3O4@UiO-66-SO3H had a strong affinity towards MB and the maximum adsorption capacity was 297.3 mg g−1. The adsorption of MB could be basically completed within 15 min. The kinetic and isotherm studies indicated that adsorption data could be well fitted to the pseudo-second-order model and Langmuir model. Significantly, Fe3O4@UiO-66-SO3H could selectively adsorb MB from a mixed solution due to the charge-selectivity effect and possessed good reusability. The electrostatic interaction and the π–π interaction were assumed to play a vital role in the adsorption process. All in all, the current study provided a promising sorbent for the efficient and selective removal of MB from dye-containing wastewater.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 2
·1-11
·
IF 5.3
Sun Xueqin,Fan Yan,Zhang Wenyuan,Yang Xiaogang,Liu Jiacheng
A pentafluoropropionic acid–functionalized fluorescent metal–organic framework material (UiO-66-NH 2 -PFPA) is prepared by a simple post-synthetic modification (PSM) strategy for the sensitive and selective detection of dichloran (DCN). The results of fluorescence experiments demonstrate that the sensitivity of UiO-66-NH 2 -PFPA (limit of detection, LOD = 0.478 μM) to DCN is nearly 10.93 times higher than that of UiO-66-NH 2 (LOD = 5.225 μM) and the material has good selectivity and anti-interference ability. After the addition of DCN, the blue fluorescence of UiO-66-NH 2 -PFPA is obviously quenched. Therefore, the possible quenching mechanism is further discussed in combination with relevant experiments and density functional theory calculations. Moreover, the sensor is applied to the detection of DCN in fruit samples with a satisfactory recovery of 101.1—107.9%, which implies that UiO-66-NH 2 -PFPA is expected to be a candidate material for the detection of DCN in food. Graphical abstract
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