NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 29
·13855-13865
·
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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SOLAR ENERGY MATERIALS AND SOLAR CELLS
·
2024
·
IF 6.3
Junchi Wang,Hui Li,Ndzondelelo Bingwa,Hao Yu,Guoning Li,Qiangqiang Xiao,Shijie Li,Min Guo,Xiaoling Ma
In this study, UiO-66(Zr) and its derivative (UiO-66-C) are employed as supports to prepare shape stabilized PCM (U/SA-X and UC /SA-X) for resolving the melting leakage and poor thermal conductivity of stearic acid (SA). Thermal storage performance, including phase change enthalpy, supercooling degree, phase change temperature, thermal conductivity, and shape stability of U/SA-X and UC/SA-X, are compared. Preliminary characterization reveals that the physicochemical property evolution of the support impacts the thermal storage performance of SA . UiO-66 with microporous structure is unfavorable to enhance the shape stability of SA. U/SA-X exhibits low thermal storage efficiency and high supercooling degree owing to nanoconfinement and hydrogen bonding. By contrast, UiO-66-C possesses mesopores and graphitic structure that allows for a remarkable thermal storage performance of UC/SA-X. In detail, UC/SA-50 exhibits an ideal thermal storage performance, where the thermal conductivity (0.531 W/(m·K)) increases by 141 % in comparison to SA with a high phase change enthalpy of 93.6 J/g and low supercooling degree of 0.24 °C. It also shows satisfying thermal reliability that the thermal property of UC/SA-50 maintains stability even after 100 thermal cycles. In addition, the photothermal conversion efficiency of UC/SA-50 is up to 83.06 %.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Xudong Wu,Kaifu Yu,Yizhou He,Xin Cao,Tao Chen,Wenkun Zhu
The phenomenon of rapid migration of photogenerated charges in natural photosynthetic systems has motivated the design of efficient photocatalysts capable of fast charge separation and efficient reaction kinetics for photocatalytically assisted enrichment and separation of uranium U(VI) in uranium wastewater. In this study, we developed a biomimetic photocatalytic system MnOx/NH2-UiO-66-rGO (M/UiO-rGO) with spatially separated dual cocatalysts. Among them, rGO functions to capture electrons and participates in reduction reactions, while MnOx captures holes and participates in oxidation reactions. The M/UiO-rGO catalyst exhibits excellent performance in photocatalytic reduction of uranium (reaching 91.8% in 1 h), and even under natural light conditions, it exhibits excellent uranium removal ability (80.4%). Using multispectral coupling technology, we further confirmed that enriched uranium undergoes a continuous and complex reaction process of “capture-reduction-free radical oxidation–nucleation–crystallization”. This work presents a viable strategy for designing biomimetic photocatalysts with efficient charge separation and rapid reaction kinetics for environmental purification purposes.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Li Gong,Yijiao Zhang,Renlong Liu,Zuohua Liu,Siwei Jin,Li Zhang,Tengda Zhao,Huanbao Fa,Wei Yin
Due to the toxicity and corrosiveness of the ammonia gas, low-cost, portable, and accurate methods of ammonia detection are of great importance in environmental testing and disease diagnosis. In this study, flower-like UIO-66-NH 2 @MoS 2 composite modified screen-printed electrodes (SPEs) were prepared by hydrothermal treatment using ionic liquids [BMIM][BF 4 ] as electrolytes. The UIO-66-NH 2 @MoS 2 /SPEs were then combined with a miniature electrochemical workstation to construct a novel electrochemical ammonia sensor. The experimental results showed that UIO-66-NH 2 @MoS 2 had excellent adsorption capacity for ammonia, exhibiting good linearity in the range of 5–500 ppm with a low limit of detection (2.1 ppm) and a fast response time for 100 ppm ammonia (13 s). This sensor also possessed excellent stability, reproducibility, and anti-interference ability. The synthesized UIO-66-NH 2 @MoS 2 nanocomposite was demonstrated to be an excellent candidate for the construction of high-performance ammonia sensors for various applications.
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TALANTA
·
2024
·
IF 5.6
Kexin Xu,Jinhui Zhu,Tong Zhang,Guodong Sui
Wastewater-based epidemiology (WBE) is a powerful tool for early warning of infectious disease outbreaks. Hence, a rapid and portable pathogen monitoring system is urgent needed for on-site detection. In this work, we first reported synthesis of an artificial modulated wide-spectrum bacteria capture nanoparticle (Arg-CSP@UiO@Fe 3 O 4 ). Arginine-modified phosphorylated chitosan (Arg-CSP) coating could provide strongly positive charged guanidinium group for pathogen interaction by electrostatic attraction, and UiO-66-NH 2 layer could help Arg-CSP graft onto Fe 3 O 4 magnetic particles. The capture efficiency of Arg-CSP@UiO@Fe 3 O 4 reached 92.2 % and 97.3 % for Escherichia coli ( E.coli ) and Staphylococcus epidermidis ( S.epidermidis )within 40 min, in 10 mL sample. To prevent pathogen degradation in sewage, a portable nucleic acid extraction-free method was also developed. UiO-66-NH 2 could disintegrate in buffer with high concentration of PO 4 3− for bacterium desorption, and then nucleic acid of the bacteria was released by heating. The DNA template concentration obtained by this method was 779.28 times higher than that of the direct thermal lysis product and 8.63 times higher than that of the commercial kit. Afterwards, multiple detection of bacteria was realized by loop-mediated isothermal amplification (LAMP). Artificial regulated pathogen desorption could prevent non-specific adsorption of nucleic acid by nanoparticles. The detection limit of Arg-CSP@UiO@Fe 3 O 4 -LAMP method was 80 cfu/mL for E.coli and 300 cfu/mL for S.epidermidis . The accuracy and reliability of the method was validated by spiked sewage samples. In conclusion, this bio-monitoring system was able to detect multiple bacteria in environment conveniently and have good potential to become an alternative solution for rapid on-site pathogen detection.
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GREEN CHEMISTRY
·
2017
·Vol. 19
·期 9
·2201-2211
·
IF 9.125
Wenxiu Cao,Wenhao Luo,Hongguang Ge,Yang Su,Aiqin Wang,Tao Zhang
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a crucial reaction included in many biorefinery schemes for the production of renewable chemicals and fuels. The development of highly stable supported Ru-based catalysts in the polar protic liquid phase under hydrothermal conditions is still a major challenge. Here, we prepared a 0.85 wt% Ru/ZrO2@C catalyst using a new stabilization strategy based on the UiO-66 (Zr-MOF) material. The catalytic performance of this Ru/ZrO2@C in LA-to-GVL was tested and compared with commercial 5 wt% Ru/C at 10 bar H2, 413 K in water and also in high protic aqueous solution (pH = 1). The full conversion of LA and quantitative yield of GVL were achieved with both catalysts. However, the 5 wt% Ru/C showed poor resistance to deactivation already after the first run. ICP, XPS, HRTEM, AC-STEM, TPR and physisorption data showed that quick deactivation of Ru/C was mainly caused by the leaching of ruthenium in addition to the loss of surface area via carbonaceous deposition in micro-pores. In contrast, the self-prepared Ru/ZrO2@C catalyst showed no apparent drop in catalytic performance either in water or in high protic aqueous solution upon multiple recycling, and no leaching of ruthenium was found even under harsh conditions (pH = 1). Remarkably, in the Ru/ZrO2@C catalyst, Ru (probable single-atom) was highly dispersed on nanotetragonal ZrO2 (3.3 nm), embedded in the amorphous carbon, and no apparent Ru nanoclusters were observed even after reactions. TPR results indicated that this excellent stability might be attributed to strong metal–support interaction between Ru and nanotetragonal ZrO2.
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