Journal of Materials Chemistry A
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2024
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IF 10.7
Lingyu Zhang,Yuhao Yang,Nan Zhao,Shuang Liu,Zhe Wang,Xiangke Wang,Yuexiang Lu
Photocatalytic reduction of uranium from U(VI) to U(IV) is an effective method to remove uranium from wastewater, while it often requires anaerobic conditions and/or the addition of sacrificial agents, which hindered its further application. Herein, MOF modified C3N4 composite material was prepared for uranium removal under air atmosphere without the addition of sacrifices, achieving a notably uranium removal capacity of 1355 mg/g. The introduction of MOF enhanced the band structure and the photoelectric properties of C3N4, making it able to generate and separate electrons and holes efficiently. The electrons were applied to reduce O2 to form H2O2 and the holes could oxidize H2O to O2. The generated H2O2 could react with UO22+ to form (UO2)O2.2H2O to realize the solidification of uranium under both air and N2 atmosphere. This work may give new direction of the design of photocatalysts for highly efficient uranium removal under air atmosphere without sacrificial agent.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Shenyi Tang,Chenglian Luo,Zhi Wang,Xinlei Liu
A defect-free and stable metal–organic framework (MOF) membrane is a promising candidate for the separation of methanol/methyl tertiary butyl ether (MeOH/MTBE) mixtures. In this work, a structural-integrity and low-thickness (∼400 nm) UiO-66 membrane was fabricated by regulating the metal ion/ligand molar ratio in the synthesis solution and optimizing the preparation process using the secondary growth method with safer and more environment-friendly Zr(n-OPr)4 metal source. Based on the effective pore size and inherent amphiphilic structure of UiO-66, the membrane exhibits exceptional pervaporation (PV) performance. For the separation of MeOH/MTBE (5:95 wt/wt %) mixtures, the membrane displays an outstanding separation performance with an average separation factor of 2.23 × 104 and an average total flux of 3.61 kg·m–2·h–1 at 40 °C, which is superior to most membranes reported for the PV separation of MeOH/MTBE mixtures. In addition, a 72 h PV process was used to further confirm the structural stability of the membrane.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Kunpeng Song,Keshan Zhang,Xue Bi,Boyou Hou,Ye-Tang Pan,Xingyao Li,Jiyu He,Rongjie Yang
Metal–organic framework (MOF)-based functionalized porous liquids are promising candidates for efficient functional species, owing to their better storage stability, higher dispersibility, and convenient processing properties than solid MOF-based fillers. However, the structural design and synthesis strategy for such porous liquids have been a challenge so far. Herein, a porous flame retardant (UiO-66-NH2@PA@OAPS, U@PA@OA) was designed using UiO-66-NH2 as a precursor, 3-phosphonopropanoic acid (PA) as a flame-retardant ligand, and octa(aminophenyl) polyhedral oligomeric silsesquioxane (OAPS) as a modifier through post-synthesis modification strategies, such as ligand replacement, defect engineering, and surface modification. Later, it was utilized as a rigid guest and polysiloxane was employed as a mobile phase and a hydrophobic component to manufacture functionalized porous liquids (UiO-66-NH2@PA@OAPS PLs, U@PA@OA PLs). Advanced U@PA@OA PLs present favorable storage stability as well as compatibility with polyurea components. Impressively, U@PA@OA PLs with a 10 wt% loading (2 wt% U@PA@OA content) in polyurea can improve the limiting oxygen index value of the composites to 26.9% and pass the V-0 rating in the UL-94 test. Moreover, the peak of heat release rate, total heat release, and total smoke production of the polyurea composites are reduced by around 53.7, 36.3, and 34.0%, respectively, compared to neat polyurea. Moreover, the mechanical properties, impact resistance, and chemical resistance of PLs modified polyurea composites are also significantly enhanced. This work not only motivates researchers to design functionalized porous liquids rationally, but it is also expected to expand the application of composites in other potential fields.
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MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Xue Zhang,Shihan Kang,Wangxing Cheng,Lei Wang,Nannan Lu,Lin-Wei Chen
Establishing an efficient and sensitive electrochemical sensor for paracetamol (PCM) is of significant importance in pharmaceutical quality control and environmental protection. This paper reports a novel electrochemical sensing platform based on a ZIF-8-derived strategy for fabricating N-doped porous carbon with monodispersed Fe-N x sites (Fe-N/NPC). The introduction of iron phthalocyanine (Fe-Pc) molecules fixed within the ZIF-8 framework prevents the aggregation of metal species during high-temperature treatment, ensuring the high dispersion of Fe-N x sites. Under optimized conditions, Fe-N/NPC-10/GCE electrochemical sensor exhibits excellent performance for PCM detection, which is mainly attributed to the synergistic enhancement between Fe-N x and NPC. The high surface area of NPC with a porous structure and N doping effect, which enhances its adsorption capacity for PCM, facilitating electron transfer and thereby amplifying the response signal. At the same time, the high-density monodispersed Fe-N x provides abundant catalytic active sites, improving electrocatalytic activity. Through the investigation of how buffer solution pH affects the oxidation peak induced by PCM, a pH of 7.0 was ultimately determined to be the optimal value. Using differential pulse voltammetry (DPV), the Fe-N/NPC-10/GCE electrochemical sensor demonstrates a wide detection range (0.1–10, 10–150 μM) for PCM with a detection limit (LOD) of 0.019 μM. Furthermore, the sensor exhibits good selectivity, stability, and reproducibility, and has been successfully applied for the determination of PCM in real pharmaceutical samples, with a recovery rate close to 100 %, indicating that the analytical method performs well and is suitable for analysis of real samples.
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Regenerative Biomaterials
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2024
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IF 5.6
Dai Sheng,Jiang Lang,Liu Luying,Su Zhaogui,Yao Li,Yang Ping,Huang Nan
Poor wound healing in diabetics is primarily caused by persistently high levels of inflammation and recurrent bacterial infections. The catalytic therapy technique based on nanozyme medicine has emerged as a beacon of hope for patients with diabetic wounds. However, the use of a single-atom nanozyme may still have limitations, including nanozyme burst release, immunological clearance, and insufficient antibacterial activity. To address the aforementioned problems, we provide a new nano-catalytic therapeutic agent for diabetic skin ulcers that incorporates a single-atom nanozyme with high antioxidant activity into a metal-organic framework (ZIF-Cu/C-dots). First, a Cu single-atom nanozyme supported by ultra-small carbon dots (Cu/C-dots) with high antioxidant activity was created. A nanozyme-integrated metal-organic framework was then created, utilizing Cu/C-dots as ligands and Zn2+ as the core metal. Cu/C-dots have good oxidase-like activity, shielding the biological system from ROS damage and reducing the expression of TNF-α and IL-1β. Zn2+ also has good antibacterial activity (the antibacterial rate was more than 90%). This integrated technique prevents nanozyme aggregation, improves nanozyme biocompatibility, slows down the breakdown of ZIF, and allows for the regulated release of Cu/C-dots and Zn2+ as needed. Finally, in vivo studies have shown that ZIF-Cu/C-dots can effectively alleviate inflammation at the site of diabetic wounds, accelerate vascular regeneration, promote collagen deposition, and enhance tissue remodeling, serving as a novel nano-catalytic platform for the treatment of wounds that are difficult to heal.
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Nanomaterials
·
2024
·Vol. 14
·期 11
·944
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IF 4.4
Liping Zhao,Jinyun Xu,Ming Li,Yanyan Ji,Yu Sun,Ziqi Zhang,Xudong Hu,Zhe Peng,Yicong Wang,Chunming Zheng,Xiaohong Sun
Aluminosilicates, abundant and crucial in both natural environments and industry, often involve uncontrollable chemical components when derived from minerals, making further chemical purification and reaction more complicated. This study utilizes pure alumina and fumed silica powders as more controllable sources, enhancing aluminosilicate reactivity through room temperature (non-firing) processing and providing a robust framework that resists mechanical stress and high temperature. By embedding iron-based metal–organic frameworks (Fe-MOF/non-firing aluminosilicate membranes) within the above matrix, these ceramic membranes not only preserve their mechanical robustness but also gain significant chemical functionality, enhancing their capacity to removing phytochromes from the vegetables. Sodium hydroxide and sodium silicate were selected as activators to successfully prepare high-strength, non-firing aluminosilicate membranes. These membranes demonstrated a flexural strength of 8.7 MPa under wet-culture conditions with a molar ratio of Al2O3:SiO2:NaOH:Na2SiO3at 1:1:0.49:0.16. The chlorophyll adsorption of spinach conducted on these membranes showed a removal rate exceeding 90% at room temperature and pH = 9, highlighting its potential for the selective adsorption of chlorophyll. This study underscores the potential of MOF-enhanced aluminosilicate ceramic membranes in environmental applications, particularly for agricultural pollution control.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yunzhe Wang,Wanyue Qian,Ganghua Zhou,Sai Zhang,Xianglin Zhu,Li Li,Xingwang Zhu,Xiaozhi Wang,Xiguang Han,Jianjian Yi
Crystal phase engineering emerges as a powerful strategy to enhance photocatalytic activity, yet controlled phase-selective synthesis and phase-dependent performance understanding remain challenging. In this study, we introduce a method for synthesizing phase-engineered In 2 O 3 via the pyrolysis of metal–organic frameworks (MOFs). We demonstrate that the functional group and pyrolysis temperatures of MOFs are critical for phase-selective synthesis. Specifically, pyrolysis of MIL-68(ln)–NH 2 at optimal temperatures yields In 2 O 3 with rhombohedral (rh-In 2 O 3 ), cubic (c-In 2 O 3 ), and rhombohedral/cubic heterophase (rh/c-In 2 O 3 ) structures. The photocatalytic CO 2 reduction tests reveal that c-In 2 O 3 outperforms rh-In 2 O 3 and rh/c-In 2 O 3 , achieving a CO production rate of 29.19 μmol g -1 h −1 with 94.47 % selectivity. Spectroscopic and theoretical analyses show that c-In 2 O 3 has superior charge transfer efficiency and lower reaction energy barriers, particularly for the rate-determining *CO intermediate, which exhibits a lower Gibbs free energy on its surface. This work provides a significant advancement in optimizing photocatalytic CO 2 reduction efficiency through precise phase engineering, underscoring the vital role of phase control in enhancing catalytic performance.
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MICROCHIMICA ACTA
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2024
·Vol. 191
·期 11
·1-9
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IF 5.3
Zhang Shengyuan,Yang Ying,Yang Dezhi,Yang Yaling
A metal–organic-framework (MOF) fluorescent sensor is reported based on NH 2 -MIL-101(Fe) propelled pesticide and alkaline phosphatase (ALP) catalytic reaction. Different from previous reports, a cascade reaction system combined with MOF structural changes to generate fluorescence was employed. The rationale is that ALP can hydrolyze L-ascorbic acid 2-phosphate (AAP) into L-ascorbic acid (AA), which can reduce Fe 3+ to decompose structurally NH 2 -MIL-101(Fe), resulting in 2-aminoterephthalic acid (NH 2 -BDC) with intense fluorescence. The fluorescence can be decreased to different degrees due to inhibition of organophosphate pesticides (OPPs) on the activity of ALP. By taking chlorpyrifos (CPY) as the model compound of an OPP pesticide and adding ALP and CPY into the NH 2 -MIL-101(Fe) framework, the resulting cascade reaction fluorescence sensors exhibit a good sensitivity for CPY and ALP sensing. The working ranges are 0.02–2 μg/L and 0.2–20 mU/mL with detection limits (LOD) of 5.31 ng/L and 0.05 mU/mL, respectively. The proposed sensor has been actually applied to satisfactory detection of CPY and ALP in food and serum samples. This fluorescence-based assay may extend the application of MOF-based biosensors. Graphical Abstract
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ACS Nano
·
2025
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IF 16
Liang Niu,Liang Zeng,Ding Yu,Situo Cheng,Guang Feng
Elucidating the charging mechanism plays an intrinsic and critical role in the development of high-performance supercapacitors; however, a deep understanding of how this mechanism varies under different charging rates remains challenging. In this study, we investigate the charging mechanism of conductive metal–organic framework (c-MOF) electrodes in ionic liquids, combining electrochemical quartz crystal microbalance and constant-potential molecular dynamics simulations. Both experimental and modeling results reveal a transition of the ion adsorption and desorption modes from anion dominance at low charging rates to ion-exchange governance at high charging rates, significantly reducing the contribution of anions to the capacitance. The dynamic structures of in-pore ions suggest that this transition stems from variations in the overscreening strength, which leads to different ion responses between the central and surface regions of c-MOF pores under polarization. This work could lay the foundation for optimizing supercapacitor design, especially under high charging rates.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Chongxi Zhang,Fengting Li,Dong Wu,Qingmeng Guo,Zhanning Liu,Zhikun Wang,Zixi Kang,Lili Fan,Daofeng Sun
Integration of cobalt phosphides (Co2P and CoP) in a carbon matrix shows great promise for developing high-performance catalysts for water electrolysis. Nevertheless, the controlled synthesis of these two phases with an effective interface, uniform dispersion, and a simplified synthesis process is still challenging. Herein, we proposed a strategy that involves pre-construction of the Co/CoO@C heterostructure followed by post-conversion by phosphorization to achieve the precise synthesis of the Co2P/CoP@C heterostructure, which was realized by utilizing a MOF as the self-sacrificial template. The oxygen-coordinated MOF that shows advantages in building the Co/CoO heterostructure was employed in this work and grown into a high-quality membrane via cathodic electrodeposition on the graphite substrate (Gss). The obtained catalyst (Gss-Co2P/CoP@C-800) requires 146 and 365 mV overpotentials to achieve a current density of 100 mA cm−2 for the HER and OER, respectively, and 1.54 V to achieve a current density of 10 mA cm−2 for water electrolysis. Beyond the significantly enhanced conductivity that originates from the robust interaction between the MOF and Gss, the establishment of an effective Co2P/CoP interface also plays a pivotal role in contributing to the high performance of Gss-Co2P/CoP@C-800. As revealed by density functional theory (DFT) calculations, the unique d-orbital electron distribution of Co2P/CoP and the enhanced state density near the Fermi level facilitate its efficient electron transport and render the Co2P/CoP heterostructure region a crucial active site for water electrolysis. This study will provide new insights into the rational design and construction of heterostructures based on MOFs for efficient and green energy conversions.
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Miao Sun,Xiao Xu,Shihao Min,Jiaxin He,Kun Li,Longtian Kang
Copper-based metal-organic framework (Cu-MOF) materials with multiple active sites have attracted increasing attention to the electrocatalytic CO 2 reduction reaction (ECR), however, face the huge challenge owing to the poor stability and low C 2 selectivity. Here, the Cu 2 O/Cu-CuTCPP heterojunction (Cu 2 O/CPFs) with three Cu active sites are firstly constructed through in-situ electrodeposition method. The effect of CuSO 4 concentration and electrodeposition conditions on ECR is systematically investigated. The optimized Cu 2 O/CPFs composite achieves the ethylene Faraday efficiency (FE C2H4 ) of 61.8 % at –1.3 V vs. RHE, which is 1.9 and 3.42 times higher than those of CPFs and Cu 2 O, respectively. Meanwhile, the C 2 H 4 partial current density ( j C2H4 ) of –7.96 mA·cm −2 is 2.91 and 4.68 times higher than those of CPFs and Cu 2 O. Further experiments reveals that the formation of Cu 2+ –O–Cu + –O bond between Cu 2 O and Cu–O 4 sites in Cu 2 O/CPF heterojunction is crucial. Consequently, the hydrogen (H 2 ), formic acid (HCOOH) and methane (CH 4 ) evolution reactions are restricted, the C–C coupling reaction of *CHO and *CO intermediates is significantly enhanced, and the Cu–O 4 sites in CPFs are protected. This work provides an effective strategy to stabilize MOF structure and obtain high value-added C 2+ products.
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REACTIVE & FUNCTIONAL POLYMERS
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2024
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IF 4.5
Linlin Yu,Ruoyu Chen,Qian Jia
Oily wastewater, especially oil-water emulsions, has caused severe environmental damage. It is urgent to develop a simple, efficient superhydrophobic and superoleophilic material to address this issue. In this work, a multifunctional sponge based on MOF was proposed. The hydroxy-assisted method was employed to prepare MOF-5 with metal coordination centers. Subsequently, octadecylphosphonic acid (OPA) was used to hydrophobically modify MOF-5 to prepare stable and hydrophobic OPA-MOF-5. Polydimethylsiloxane (PDMS) with low surface energy was employed as the adhesive, and the hydrophobic OPA-MOF-5 was loaded onto the polyurethane (PU) sponge to obtain the stable superhydrophobic OPA-MOF-5@PDMS@PU with a WCA of 155.9°. The produced modified sponge exhibited high sorption capacity and oil-water separation efficiency, with a sorption capacity of 26.7 (petroleum ether)-85.6 (chloroform) g/g and a separation efficiency of over 99 %. It has also shown satisfactory emulsion purification and flame retardancy capacities.
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