COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
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ACS Applied Materials & Interfaces
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2022
·
IF 10.383
Qiufan Sun,Yuxiang Zhu,Xiang Zhong,Meng Jiang,Yanchen Fan,Jianfeng Yao
In this work, MIL-68(In) functionalized with various ligand substitutions including amine, hydroxyl, bromine, nitro, and methyl groups was prepared, via a one-pot solvothermal reaction for visible-light photocatalytic ammonia synthesis. The diversity of ligands tunes the morphology, geometry, pore environment, and electronic structure of MIL-68(In)-based photocatalysts due to the polarity and intraframework interactions. Amine-inserted MIL-68(In) outperforms its counterparts, presenting a boosted nitrogen photofixation rate of 140.34 μmol gcat–1 h–1 with an apparent quantum efficiency of 5.69% at 420 nm. Further, the size of the batch solvothermal reactor and the amine group content also influence the photocatalytic activity. The combined experimental and theoretical results reveal that amine substituents improve the chemisorption of nitrogen molecules and the conversion of nitrogen into ammonia follows a dual pathway, i.e., a Mars–van Krevelen process and a ligand-to-metal charge transfer mechanism. This work provides a molecular engineering strategy via dual catalysis toward efficient ammonia production.
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CHEMOSPHERE
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2023
·
IF 8.8
Jun Wang,Junxian Qin,Changqing Yang,Yun Hu
A series of functionalized X-UiO-66 (X = NH 2 , H, Br and NO 2 ) materials were prepared using a hydrothermal method and modified with various ligands. Their photocatalytic activity was evaluated by the oxidation of acetaldehyde. Experimental results show that the introduction of different ligands significantly influences the physicochemical properties of UiO-66. Br-UiO-66 exhibited the highest photocatalytic activity and CO 2 selectivity of 85.6% and 85.7%, respectively. Photochemical properties reveal that -Br functional group facilitate the separation of photogenerated electrons and holes, significantly improving their transfer and oxygen reduction. As a result, an increased number of hydroxyl and superoxide radicals can form, improving the efficiency of the photocatalytic reaction. Br-UiO-66 accumulates fewer intermediates on its surface and still shows excellent photocatalytic activity and structural stability after 24 h of dynamic reaction. This work demonstrates the excellent adsorption and catalytic oxidation performance of Br-UiO-66 towards acetaldehyde and may provide new ideas for researching catalysts in the photocatalytic degradation of pollutants.
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Molecular Catalysis
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2023
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IF 4.6
Jianhong Zheng,Xi Chen,Xiaoxiao Yin,Kai Chen,Aili Liu,Xiaochun Yu,Shun Wang,Zhongwei Chen
A highly efficient and organic solvent-free synthetic strategy for the selective oxidation of anilines to azoxybenzenes was developed by employing porous Zr-MOFs as catalysts in aqueous hydrogen peroxide solution. The impact of cluster nodes, pore size, and linker functionalities on the catalytic performance of Zr-MOFs was fully evaluated and discussed. Featuring abundant bridging Zr-OH-Zr catalytic sites and confined microenvironments, the pristine UiO-66(Zr) could create abundant reactive oxygen species (ROS) with high H 2 O 2 efficiency, affording quantitative yield of azoxybenzene under mild conditions. Furthermore, the UiO-66(Zr)/H 2 O 2 heterogeneous catalytic system exhibited broad and size-selective substrate scope and excellent stability in consecutive catalytic cycles. Mechanism studies demonstrated that the azoxybenzenes were produced through radical pathway on bridging Zr-OH-Zr sites. This study provided alternative strategies exploiting green catalytic systems with porous MOFs, which might further expand the potential application of the MOFs family.
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Journal of Environmental Chemical Engineering
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2022
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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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Advanced Science
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2023
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IF 15.1
Xinzhao Jiang,Wei Wang,Jincheng Tang,Meng Han,Yichang Xu,Lichen Zhang,Jie Wu,Yiyang Huang,Zhouye Ding,Huiwen Sun,Kun Xi,Yong Gu,Liang Chen
Although mitochondria are crucial for recovery after spinal cord injury (SCI), therapeutic strategies to modulate mitochondrial metabolic energy to coordinate the immune response and nerve regeneration are lacking. Here, a ligand-screened cerium-based metal-organic framework (MOF) with better ROS scavenging and drug-loading abilities is encapsulated with polydopamine after loading creatine to obtain microcapsules (Cr/Ce@PDA nanoparticles), which reverse the energy deficits in both macrophages and neuronal cells by combining ROS scavenging and energy supplementation. It reprogrames inflammatory macrophages to the proregenerative phenotype via the succinate/HIF-1α/IL-1β signaling axis. It also promotes the regeneration and differentiation of neural cells by activating the mTOR pathway and paracrine function of macrophages. In vivo experiments further confirm the effect of the microcapsules in regulating early ROS-inflammation positive-feedback chain reactions and continuously promoting nerve regeneration. This study provides a new strategy for correcting mitochondrial energy deficiency in the immune response and nerve regeneration following SCI.
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Journal of Materials Chemistry A
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2020
·Vol. 8
·期 29
·14644-14652
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IF 11.301
Yong-Jun Chen,Yifa Chen,Chang Miao,Yi-Rong Wang,Guang-Kuo Gao,Ru-Xin Yang,Hong-Jing Zhu,Jian-Hui Wang,Shun-Li Li,Ya-Qian Lan
Microplastics are a worldwide problem that poses a giant threat to organisms in the ecosystem and even to human health. The removal of microplastics is a severe challenge that needs to be solved urgently. Herein, a series of zirconium metal–organic framework-based foam materials with interpenetrated pores, high MOF uniformity and excellent durability have been successfully fabricated and applied in simulated microplastics removal in water or seawater conditions. They can be applied to various types and concentrations of microplastics suspensions. It is worth noting that the best of them, UiO-66-OH@MF-3, can efficiently remove microplastics with an efficiency of up to 95.5 ± 1.2% and can maintain high performance in recycling and large-quantity filtration experiments. Besides, we proposed an automatic filtration system powered by sunlight and accomplished it on the lab-scale. The high performances of these foam materials combined with the new concept of automatic filtration systems might shed some light on the development of novel techniques for microplastics removal.
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ANALYTICA CHIMICA ACTA
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2016
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IF 4.712
Lin Luo,Hong-Tao Lei,Jin-Yi Yang,Gong-Liang Liu,Yuan-Ming Sun,Wei-Dong Bai,Hong Wang,Yu-Dong Shen,Sui Chen,Zhen-Lin Xu
The widespread occurrence of ethyl carbamate (EC, 89.09 Da), a group 2A carcinogen, in fermented foods and alcoholic beverages has raised worldwide public health concern. Immunoassay for EC is unavailable due to the simple and small structure of EC. In this work, an initial attempt to produce antibody specific for EC, by using 4-((ethoxycarbonyl)amino)butanoic acid as hapten , was made but failed. However, since EC can easily react with 9-xanthydrol to form xanthyl ethyl carbamate (XEC), two haptens based on XEC structure were designed and synthesized. Polyclonal antibody against XEC, instead of EC was obtained and then used to develop a competitive indirect ELISA for EC via a pre-analysis derivatization . After optimization, the ciELISA was applied in analyzing Chinese rice wine with detection limit of 166 μg/L, and negligible cross-reactivity with EC analogs. Recoveries of EC in fortified samples were from 84.4% to 100.9%, with coefficients of variation below 10%. Results for analysis of real samples by the ci-ELISA correlated well with that by reference method GC-MS, suggesting the good accuracy and reproducibility of the proposed method. This is the first report of an immunoassay capable of detecting EC, which is suitable for monitoring EC in a large amount of samples.
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INORGANIC CHEMISTRY
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2025
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IF 4.7
Chong Lin,Shan Wang,Xuetong Zhang,Bin Xiao,Yepeng Zeng,Li Huang,Fei Luo,Kangye Liu,Jingyang Tian,Min Li,Minghui Cao,Yong Qian
The platelike nickel-terephthalate-type metal–organic framework nanoarrays (Ni-BDC NAs) on carbon cloth are obtained by employing agaric-like Ni(OH)2 NAs as sacrificial templates. The microenvironment of Ni-BDC NAs is modulated by various neighboring functional groups (−NH2, −NO2, and −Br) on the carboxylate ligand, exerting minimal destructive effects on the structure and morphology of Ni-BDC NAs. The electrochemical oxygen evolution reaction (OER) of Ni-BDC–NH2 NAs, Ni-BDC–NO2 NAs, and Ni-BDC–Br NAs exhibited a significant enhancement compared to that of Ni-BDC NAs alone, as evidenced by both experimental and theoretical assessments. The presence of neighboring groups exerts a positive influence on the electronic coupling between Ni and O atoms, thereby facilitating the thermodynamically favorable formation of *O intermediates on Ni sites and accelerating the kinetics of the OER. The findings presented here provide valuable insights for the design and utilization of carboxylic acid molecules with functional group effects, enhancing the activity of the OER across diverse Ni centers.
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