Nanoscale
·
2025
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IF 5.1
Zuyao Fu,Lingfeng Yang,Zhaoyang Ding,Jing Xie
Immobilized enzymes play a crucial role in analytical sensing due to their exceptional stability and considerable commercial importance. In this study, a stable Zr-based metal–organic framework (UiO-66-NH2) was prepared as an immobilization platform for horseradish peroxidase (HRP) through covalent binding. HRP@UiO-66-NH2 retained 75% of its activity after 10 cycles. Subsequently, a colorimetric/fluorometric dual-mode sensing strategy using HRP@UiO-66-NH2 was developed for nitrite detection. HRP@UiO-66-NH2 facilitated the transformation of the non-colored compound 3,3′,5,5′-tetramethylbenzidine (TMB) into its blue oxidized form. When nitrite is added, oxidized TMB (ox-TMB) specifically engaged with nitrite (NO2−) to generate diazotized TMB, leading to a color shift from blue to yellow. Concurrently, NO2− reacted with the amino groups of HRP@UiO-66-NH2, forming diazonium compounds and suppressing the fluorescence of HRP@UiO-66-NH2. The limits of detection were 0.21 μM and 0.19 μM for the colorimetric and fluorometric strategies, respectively. Furthermore, a portable kit for detecting nitrite was created by integrating gelatin with HRP@UiO-66-NH2. The kit could visually identify nitrite from 10–400 μM in colorimetric mode and 0–400 μM in fluorometric mode. This method provides an innovative approach for nitrite sensing, paving the way for new research into multifunctional immobilized enzymes and their potential uses in biochemical sensing applications.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yu Jiang,Si-Chao Liu,Li-Ping Zhang,Guo-Wei Guan,Yi-Tao Li,Shuang Ni,Run-Yuan Jiang,Su-Tao Zheng,Hao-Ran Liu,Hao-Ling Lan,Qing-Yuan Yang
The photocatalytic reduction of carbon dioxide (CO 2 ) to carbon-based materials is challenging because of its intricate nature and the generation of multiple byproducts. Hence, developing photocatalysts with a high CO 2 -reduction yield and selectivity is critical. In this study, new photocatalysts (U-B-M, M = Co, Ni) were synthesized by incorporating 1,2-benzisothiazolin-3-one (BIT) into NH 2 -UiO-66, to create N, N’-chelating sites via an amine–aldehyde condensation reaction, followed by metal-ion chelation. The introduction of BIT decreased the resistance of the catalyst and enhanced the separation of photogenerated carriers. The catalytic performance of U-B-Ni (rate: 3.10 mmol·g −1 ·h −1 ; selectivity: 97 %) surpasses those most of all previously reported MOF-based photocatalysts. Moreover, U-B-Ni shows high stability and negligible deactivation on catalytic cycling for over 16 h. This study expands the utility of metal–organic frameworks (MOF) in photocatalysis and highlights the importance of amine–aldehyde condensation in MOF modification.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 37
·16546-16556
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IF 2.7
Xiubin Ren,Chun Huang,Zhengxuan Gao,Ruichen Zhai,Youyu Zhu,Yingfeng Duan,Linyong Chen,Weiqin Zhao,Guofu Li
The presence of phenol in coal-chemical engineering wastewater is considered a serious environmental issue. The use of enzymes to degrade phenol has received wide attention. G-quadruplex can combine with hemin to form G-quadruplex/hemin, which shows peroxidase-like activity and can be used to degrade phenol. In this work, a novel CNTs-NH2@G-quadruplex/hemin was designed using a single-stranded DNA (ssDNA) that contained G-rich fragments and T-rich fragments. The G-rich fragments assembled with the hemin to form G-quadruplex/hemin; the pyrimidine group of the T-rich fragment could form stable chemical bonds with the amino group, which could be used for immobilization. Characterization analysis of FTIR, XRD and TEM showed that the CNTs-NH2@G-quadruplex/hemin was successfully prepared. Meanwhile, the activity and phenol degradation ability for CNTs-NH2@G-quadruplex/hemin were studied in detail, and the effects of pH, temperature, initial phenol concentration, H2O2 concentration and reusability on the degradation efficiency of phenol were also explored. The results showed that when immobilized, the CNTs-NH2@G-quadruplex/hemin presented good activity, especially under conditions of temperature 30 °C and pH 7.0. Notably, the maximum reaction velocity of CNTs-NH2@G-quadruplex/hemin was increased from 0.016 mM mg−1 min−1 (free enzyme) to 0.056 mM mg−1 min−1. For phenol degradation ability, it was observed that under the conditions of temperature 30 °C, pH 7.0, initial phenol concentration 40 mg L−1, H2O2 concentration 120 mM, enzyme dose 40 mg L−1, more than 90% of phenol could be degraded within 600 min. In addition, the CNTs-NH2@G-quadruplex/hemin still maintained high activity after 10 cycles of phenol removal, demonstrating its appealing potential for practical applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Meidan Que,Peihong Ma,Yabo Wang,Yanbo Sun,Xiangwei Bai,Lili Gao,Jin Chen,Jian Wei,Hui Li
NH 2 -MIL-125 with abundant porosity and specific interactions with CO 2 molecules, has been demonstrate great potential in the field of photocatalytic CO 2 reduction. However, conventional NH 2 -MIL-125 and their composites much lower CO 2 photoreduction efficiency in aerobic environments because of the O 2 competition. To circumvent the issue, this study modifies NH 2 -MIL-125 through crystal facet engineering to enhance its selective CO 2 adsorption and photocatalytic efficiency in the environment of impurity CO 2 . The results indicate that NH 2 -MIL-125 featuring (101) crystal planes can sustain elevated catalytic activity in low-concentration CO 2 environments. In a pure CO 2 atmosphere, NM-5 achieves a CO production rate of 159.66 μmol·g −1 after 4 h, 1.85 times greater than the unmodified NH 2 -MIL-125. Under conditions simulating flue gas (5 % CO 2 ) and ultra-low CO 2 concentrations (0.15 % CO 2 ), NM-5 maintains CO production rates of 3.18 μmol·g −1 and 0.95 μmol·g −1 , respectively, representing 1.63 and 1.73 times the production rates of NM. Furthermore, theoretical calculations indicate that CO 2 exhibits a higher adsorption energy (−1.34 eV) compared to N 2 and O 2 (−0.67 eV and −0.15 eV) on the (101) crystal plane, which reveals the preferential adsorption of CO 2 on the (101) crystal planes. This study involves a novel strategy for optimizing MOFs crystal planes and provides significant insights into achieving efficient photocatalytic CO 2 reduction under aerobic conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Xingyu Zhang,Lin Chen,Longjie Jiang,Liang Zhu,Chuqing Cao,Wei Zhang,Linting Zhao,Jiaqi Xu,Han Liu
In the advent of the new energy era, the global demand for lithium is increasing rapidly. The recovery of Li + and Co 2+ from the leachate of high-quality spent lithium-ion batteries (LIBs) offers significant economic and environmental benefits. This study proposes a TFC-ON-MOF membrane prepared through a combination of in situ growth and interfacial polymerization (IP) for the recovery of Co 2+ and Li + from battery leachate. Operated in an electrodialysis (ED) system, the experimental results demonstrated that the optimum Li + membrane flux was observed to reach 1.02 μmol cm −2 min −1 at 7.5 mA cm −2 , with the selectivity remaining at 19.84, which exemplifies well-separation and permeation performance. Following several operational cycles, the separation performance remained stable, and the membrane exhibited enhanced fouling resistance relative to commercial monovalent selective cation exchange membranes (CSO). The composite membrane features sub-nanometer windows and nanometer-sized cavities, enabling selective permeation of Li + while simultaneously sequestering Co 2+ . The inclusion of auxiliary permeation groups (PSS) also enhances overall permeation performance and selectivity. The findings contribute to the design of composite metal–organic frameworks and provide a novel approach for the selective separation of heavy metal ions from spent lithium batteries, thereby promoting the efficient recycling of valuable metal resources.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Xin Li,Qi-Wen Ma,Guangning Yu,Ji Shi,Hai-Yang Chang,Rong-Rong Zheng,Hengxue Xiang,Cheng Wang
All-inorganic halide perovskite (CsPbX3) nanocrystals (NCs) have garnered significant attention due to their excellent photoelectric properties. However, their practical application has been limited by stability issues. This study presents a strategy combining physical confinement through a carrier matrix and chemical bond coupling to enhance the stability of CsPbX3 NCs significantly under UV irradiation, polar solvents, and thermal conditions. Specifically, CsPbBr3 NCs exhibited near-complete fluorescence quenching within 300 min when treated with water and ethanol. In contrast, CsPbBr3/DMSNs-NH2 nanocomposites retained 86.9% and 75.4% of their initial photoluminescence intensity after 7 days. This enhanced stability is attributed to the multilevel pore architecture of DMSNs-NH2, which effectively prevents direct interaction with water and oxygen. Furthermore, bright white light-emitting diode (LED) devices were successfully fabricated using these nanocomposites, achieving a color temperature of 6045 K and a color gamut covering 133.5% of NTSC and 99% of Rec.2020 standards. This work demonstrates a promising pathway for the development of stable, high-performance perovskite-based optoelectronic devices.
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Desalination and Water Treatment
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2024
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IF 1
Yang Shen,Fatoye Sawyerr,Lunbo Xu,Shusu Shen,Xiaoji Zhou
The preparation of modified membranes utilizing the UiO-66 framework for wastewater filtration is regarded as one of the most promising approaches to wastewater treatment, owing to its high efficiency and cost-effectiveness. In this study, a post-modified MOF, UiO-66-RSA, was synthesized via the condensation reaction of UiO-66-NH 2 and 2,4-dihydroxybenzaldehyde. PVDF mixed matrix membranes (MMMs) were fabricated for the first time by mixing UiO-66-RSA into PVDF using the non-solvent induced phase separation (NIPS) method. Compared to pure PVDF membranes, the newly developed membrane, M4, demonstrated enhanced compatibility and superior mechanical strength. In dyeing wastewater treatment applications, M4 showed excellent separation efficiency for dye and heavy metal mixed wastewater, achieving rejection rates exceeding 90 %. Additionally, it maintained a high flux recovery rate (FRR > 90 %) and rejection rate (Rejection > 90 %) after six filtration cycles of dye-containing wastewater, indicating strong recyclability. These findings suggest that MMMs embedded with UiO-66-RSA hold significant promise for dyeing wastewater treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Qiufan Sun,Yuxiang Zhu,Yan Wang,Zhengtao Jia,Xiang Zhong,Jianfeng Yao
Three isostructural MIL-68(M)-NH 2 frameworks (M = In, Fe, or Al) featuring different metal centers were synthesized to investigate their photocatalytic activities for nitrogen fixation. The influence of the metal oxo clusters on the crystalline structures, morphologies, and optical characteristics was examined. MIL-68(In)-NH 2 (MNI) with one-dimensional microrod structures has a larger surface area than bulk MIL-68(Fe)-NH 2 (MNF) and spherical MIL-68(Al)-NH 2 (MNA), and achieves an ammonia generation rate (140.34 μmol g cat −1 h −1 ) ca . 3.4 and 1.6 times higher than those of MNF (37.25 μmol g cat −1 h −1 ) and MNA (87.5 μmol g cat −1 h −1 ), respectively. The superior performance can be attributed to its high crystallinity, strong coordination between the In−oxo clusters and ligands, and microrod morphology, which enhance electron transfer, improve mass transport, and extend visible light absorption. Moreover, MNI shows greater stability in ethanol aqueous solution than other sacrificial reagents, such as methanol, potassium sulfite, and triethanolamine. While slight surface corrosion of the microrods occurs in methanol and potassium sulfite solutions, complete collapse is observed in triethanolamine.
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Desalination and Water Treatment
·
2024
·
IF 1
Honghuan Yin,Huaiwen Wang,Dongai Wang,Miaomiao Shi,Xi Xu,Jiaqi Yang
Developing low-cost and stable adsorbent is urgent and attractive to remove hazardous dye from water. In this study, zirconium based metal-organic framework (NH 2 -UiO-66) was grown on waste wool fibers and the fabricated composite adsorbent (NH 2 -UiO-66/wool) was used to remove anionic dye methyl orange (MO). After characterizing the adsorbents, we determined the effect of pH and initial concentration of MO on adsorption performance. Moreover, adsorption kinetics and isotherms were conducted to reveal the adsorption mechanism. The results showed that NH 2 -UiO-66/wool achieved the highest adsorption capacity at natural pH with the maximum adsorption of 61.0 mg/g adsorbent, which is higher than most biomass based adsorbents. Moreover, NH 2 -UiO-66/wool enabled a broad range of pH (3−11) and initial concentration of MO (10–50 mg/L). Adsorption kinetics and isotherms of NH 2 -UiO-66/wool fitted well with pseudo-second-order model and Langmuir mode, respectively. NH 2 -UiO-66/wool presented 40.3 times higher of kinetics constant than that of original wool in the presence of initial MO concentration of 10 mg/L due to the positive nature of NH 2 -UiO-66. Ultimately, NH 2 -UiO-66/wool presented excellent regeneration ability with 500 mg/L NaCl solution and regeneration efficiency remained 98% after 10 cycles. Overall, this work may provide new insights into the development of MOFs/wool adsorbents for enhanced dye removal.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Xuanhao Liang,Guangyuan Chen,Hao Zhang,Ling Zhang,Tao Duan,Lin Zhu
Ti-based MOFs exhibit ultra-high stability in radioactive waste gases containing nitrogen oxides (NO X ) and are effective in capturing radioactive iodine. In this study, NH 2 -MIL-125 was synthesized via a one-pot solvothermal method and its adsorption performance for iodine was investigated using batch adsorption experiments, the stability of materials was tested by simulating post-processing conditions. The results indicated that NH 2 -MIL-125 had a maximum iodine adsorption capacity of 1.61 g/g at 75 ℃ and reached adsorption equilibrium within 60 min, and the adsorption capacity of methyl iodine reached 776.9 mg/g. The material also exhibited excellent stability and iodine adsorption performance in the presence of NO X . After soaking in NO 2 for 24 h, its structure remained stable and the adsorption capacity for iodine remained at 231.5 mg/g. The excellent co-adsorption performance of NH 2 -MIL-125 on iodine and NO X was attributed to the synergistic effects of Ti-OH groups and amino functional groups. These findings provide a reference for the capture of radioactive iodine and also demonstrate the potential of NH 2 -MIL-125 for iodine capture during spent fuel reprocessing .
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CARBON
·
2024
·
IF 10.5
Jiarong Zhang,Long Yu,Ya'nan Zhao,Tianran Zhao,Yi'na Yang,Chunna Yu,Chang Zhao,Guangjian Xing
The urgent need for multifunctional, high-performance materials is critical in addressing environmental pollution and energy shortages faced by contemporary society. This research presents innovative NH 2 -MIL-88B/Ta 4 C 3 T X /graphene aerogels that exhibit exceptional capabilities in photocatalysis and thermal energy storage utilizing solar energy. Synthesized through a combination of hydrothermal and freeze-drying methods, these aerogels feature unique structural characteristics, including a hierarchical porous structure, low density, and a large specific surface area. Furthermore, the synergistic effects of NH 2 -MIL-88B, Ta 4 C 3 T X MXene, and the aerogel matrix contribute to remarkable physicochemical properties, such as high sunlight absorptivity and an optimal optical band gap that aligns well with the solar spectrum. These attributes enable the aerogels to photodegrade various dye and antibiotic drug solutions with high concentrations. The photodegradation efficiencies achieved were 75.57 % for Congo red, 61.56 % for methylene blue, and 58.57 % for tetracycline hydrochloride. Additionally, these aerogels exhibit significant adsorption capacities for various dyes and drugs. Moreover, when the phase change material polyethylene glycol is successfully integrated into the aerogels, they exhibit excellent thermal energy storage performance with leak-proof capabilities. A high photothermal conversion efficiency of 90.15 %, a phase enthalpy of 202.13 J g −1 , and an enthalpy efficiency of 98.55 % provide evidence for this. This work provides valuable insights into the development of multifunctional aerogels aimed at addressing the challenges of wastewater treatment and energy shortages.
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CRYSTENGCOMM
·
2024
·
IF 2.6
Hao He,Xiao-kai Liu,Bai-yun Zhao,Li-juan Zhou,Xuan Zhao,Chen-xu Wang,Ji-yuan Zhang,Yuan-fang Zhang,Li Wang
In this study, UiO-66-NH2 nanoparticles were synthesized via a hydrothermal method, using acetic acid and hydrochloric acid as modulators to optimize the specific surface area and pore width. Oxytetracycline (OTC) was chosen as the test compound to evaluate the adsorption efficiency of UiO-66-NH2.The material was thoroughly characterized under varying conditions, and the adsorption mechanism was systematically explored through adsorption kinetics, isotherms, and thermodynamic analyses. The results demonstrated that UiO-66-NH2 exhibited a high OTC adsorption capacity, achieving a maximum of 312.5 mg g−1 under optimal conditions. XRD, TGA, and BET analyses revealed that acetic acid and hydrochloric acid significantly improved the crystallinity and thermal stability of UiO-66-NH2, increasing the specific surface area from 8.023 m2 g−1 to 998.663 m2 g−1 and reducing the pore width from 18.783 nm to 2.129 nm. FTIR, XPS, adsorption kinetics, and isotherm studies indicated that the main forces driving OTC adsorption by CMC-Fe were hydrogen bonding, π–π stacking, weak electrostatic interactions, and pore filling. Cyclic adsorption experiments further demonstrated the excellent reusability of UiO-66-NH2. In summary, the use of acetic acid and hydrochloric acid significantly increased the specific surface area of UiO-66-NH2, exposing more adsorption sites and playing a critical role in pollutant removal.
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