Small Structures
·
2025
·
IF 11.3
Jiaojiao Fan,Jianmin Chen,Wenji Li,Zhongxing Zhao,Zhenxia Zhao
Converting CO 2 into high-value-added products via “artificial photosynthesis” under mild conditions is a promising yet challenging strategy for developing efficient photocatalysts. This study reports a simple two-step solvothermal approach to fabricate the dual-metal–organic framework (MOF) nanocomposite NH 2 -UiO-66@PCN-224 (NU-66@PCN-224) with tightly integrated interfaces, which achieves efficient CO 2 to CO photocatalytic reduction under light irradiation. The epitaxially grown PCN-224, composed of Zr 6 clusters and tetrakis (4-carboxyphenyl) porphyrin (TCPP), serves as a shell layer and a visible light-absorbing antenna, thereby broadening the light absorption range of the composite material. Moreover, the tightly integrated interfaces of NU-66@PCN-224 enhance the mobility of photogenerated charge carriers, consequently enhancing its capability for CO 2 catalytic reduction. As a result, the combination of NU-66 and PCN-224 retains their individual advantages while achieving a synergistic enhancement of both adsorption and catalysis, further improving the photocatalytic performance. The as-prepared NU-66@PCN-224 catalyst exhibits outstanding photocatalytic performance, yielding 74.6 μmol g −1 h −1 of CO under irradiation without sacrificial agents or photosensitizers. This work demonstrates a straightforward and effective method for designing MOF-on-MOF photocatalysts with enhanced photoactivity.
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Water Conservation Science and Engineering
·
2025
·Vol. 10
·期 3
·1-16
·
IF 1.9
Li Zhengjie,Fang Chunxia,Ma Xilong,Liu Yixian,Xie Juan,Li Pengfei,Zhang Zhikun,Zhao Xudong,Sun Hua,Han Jilong
Herein, a facile and rapid preparation method was developed to synthesize Ce-doped UiO-66-NH 2 through a one-pot solvothermal method. This approach simultaneously introduces functional groups onto organic ligands and incorporating a novel metal into metal clusters. The incorporation of Ce ions effectively enlarged the pore size and increased the pore volume, thereby facilitating the diffusion of specific adsorbate molecules into the inner adsorption sites provided by the –NH 2 groups. Due to the favorable pore structures and more exposed adsorption sites, the safranine T (ST) adsorption capacity of Ce-doped UiO-66-NH 2 was ten times higher than the pristine UiO-66-NH 2 and reached 1340 mg/g at optimal adsorption conditions, surpassing most of the reported porous adsorbents. The kinetic and isotherm fitting results showed that the pseudo-second-order and Langmuir models described the adsorption behaviors of ST best, indicating a homogeneous, endothermic, and spontaneous monolayer adsorption process. The adsorption mechanism showed that the hydrogen bonding interaction and pore filling effect are identified as the main mechanism whilst electrostatic attraction interaction further enhances the adsorption capacity at optimal pH. Therefore, Ce-doped UiO-66-NH 2 can serve as a promising adsorbent for the removal of cationic dyes from textile wastewater, and the developed facile and rapid method offers a viable strategy to construct novel MOF-based adsorbents.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Zhenbo Wu,Jinjuan Xue,Zhaoxia Chen,Yiting Lv,Shuaishuai Ma,Jinku Ma,Mingxin Wang
Membrane technology for wastewater remediation has generated significant interest, however, the single functionality, dull wettability and easy fouling property of the membrane hinder its practical application. Herein, a self-cleaning and multi-use superwetting nanofiber membrane was prepared by electrospinning and subsequent spraying technique. The sulfonated cobalt phthalocyanine/NH 2 -MIL-125 (CoPcS/NMIL) heterojunction was uniformly enrobed over polyethylene terephthalate (PET) electrospun membrane derived from waste PET bottles. The unique CoPcS/NMIL heterojunction exhibited a dual driving effect in photocatalytic activity and membrane wettability. Therefore, the fabricated CoPcS/NMIL@PET composite membrane demonstrated its capability to address complex water pollution issues effectively. The composite membrane exhibited notable flux permeation ability (538–3180 L m −2 h −1 ) and achieved excellent separation efficiency of over 99 % for diverse oil-in-water emulsions under the gravity filtration condition. Notably, the membrane can efficiently deal with stubborn high-viscosity crude oil fouling profiting from the photocatalytic self-cleaning function. A high flux recovery ratio of 93.6 % and a low irreversible fouling resistance ratio of 6.4 % can be obtained after 30 min of visible light irradiation. Impressively, CoPcS/NMIL@PET membrane exhibited enhanced permeation flux, separation efficiency and self-cleaning capacity compared to NMIL@PET membrane. Meanwhile, the CoPcS/NMIL@PET-activated peroxomonosulfate (PMS) system exhibited extremely high degradation performance for RhB under visible light with the degradation efficiency of 98 % within 10 min, suggesting its potential in the rapid purification of water-soluble organic pollutants . In addition, the CoPcS/NMIL@PET membrane has good chemical stability and mechanical properties for potential long-term use. Moreover, the demulsification mechanism in oil-water separation and PMS-photocatalysis synergetic mechanism over the fabricated CoPcS/NMIL@PET membrane were also investigated in detail. The research offers a promising approach for the design and fabrication of novel nanofiber membranes that incorporate photosensitizers and MOFs functional surfaces to address the challenges associated with such wastewater treatment .
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Shuna Jia,Zhijiang Dong,Zhiqiang Wang,Boxiong Shen,Honghong Lyu
Efficient catalytic reduction of the main greenhouse gas CO 2 into high value-added chemicals is an important measure to alleviate the greenhouse effect and energy depletion. Metal nitrogen (M-N 4 ) macrocyclic complexes have attracted increasing attention in the field of electrocatalytic CO 2 reduction (CO 2 RR) due to the precise adjustment of the catalytic active site according to the requirements and the flexible modification of the external ligand structure. Nevertheless, the poor activity and low selectivity of reduction products restrict their widespread application in electrocatalytic CO 2 RR. Herein, a combination of nanoscale and molecular level method has been developed to construct easily obtainable 4NH 2 -NiPc/NH 2 -CNT hybrid material, in which amino groups are connected to provide electrons toward the central Ni-N 4 site to promote the electrocatalytic CO 2 RR catalytic activity. As a result, the catalyst 4NH 2 -NiPc/NH 2 -CNT mainly produces CO in the electrocatalytic CO 2 RR, which exhibits a Faradaic efficiency of CO (FE CO ) higher than 92 % within a wide overpotential range of −0.70 to −0.95 V vs. RHE, and provides excellent stability with a current density of 12 mA cm −2 at −0.80 V vs. RHE. In addition, 4NH 2 -NiPc/NH 2 -CNT reaches its maximum FE CO value of 96 % at −0.8 V vs. RHE, which is approximately 3.1 times that of the original unmodified NiPc/CNT, demonstrating excellent promotion of electrochemical performance. Similarly, compared to NiPc/CNT without amino modification, the current density of 4NH 2 -NiPc/NH 2 -CNT exceeds it by more than twice. The research results indicate that promoting role of electron substituted amino groups in catalysis dispersion and electronic environment coordination. This study proposes a promising strategy of introducing amino groups into molecular catalysts and hybridizing with carbon nanotube to enhance the electrocatalytic conversion of CO 2 to deep reduction products.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Hua Yu,Xuan Wang,Lijun Yang,Qirui Wu,Houming Shen,Geming Wang,Peng Fan
The development of high-performance separator materials has become crucial with the ever-increasing demands for enhanced safety and energy density of lithium-ion batteries in electric vehicles and large-scale energy storage systems. Here, a novel high-safety functionalized separator was prepared by synthesizing a composite material that encapsulates phosphorus‑nitrogen-containing ionic liquid (P/N-IL) within NH 2 -UIO-66-Zr metal-organic framework (MOF), and then combining this composite with a polyvinylidene fluoride (PVDF) P/N-IL@NH 2 -UIO-66/PVDF separator. This functionalized P/N-IL@NH 2 -UIO-66/PVDF separator significantly improves the flame-retardant performance of NCM811 batteries, effectively mitigating the risks of electrolyte combustion and explosion. Meanwhile, the porous structure of P/N-IL@NH 2 -UIO-66 material optimizes the Li + transport pathways, resulting in an increase in the ionic conductivity of NCM811 battery o 3.1 × 10 −4 S/cm (compared to only 3.4 × 10 −6 S/cm for the pure PVDF separator). The Li + transference number is also elevated to 0.68. Moreover, after 600 cycles at a 1C current density, the capacity retention rate reaches as high as 71 %, with an average coulombic efficiency of 96 %, substantially enhancing the electrochemical performance and cycling stability of the battery. This work offers a novel technological pathway for the development of high-safety, high-performance lithium-ion batteries, as well as for the application of ionic liquids and MOFs.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Xian-Yu Shen,Ya-Nan Wang,Ya-Ting Zheng,Ye Wang,Wen-Wen Dong,Jun Zhao,Dong-Sheng Li
Formaldehyde (HCHO), a crucial industrial chemical, finds extensive applications across diverse sectors, including household products, commercial materials, aviation, and medical supplies. Methane (CH4), as an abundant C1 resource, presents a promising feedstock for HCHO synthesis. However, the direct conversion of CH4 to HCHO remains challenging due to its inherent chemical inertness, characterized by low polarizability and high C–H bond dissociation energy (439 kJ mol–1), coupled with the high reactivity of intermediate products. The development of efficient strategies for selective CH4 oxidation to high-value HCHO under mild conditions is therefore of significant practical importance. In this study, we developed a series of MIL-125-NH2@FeOOH-x heterostructured photocatalysts (FM-x) through the controlled deposition of FeOOH nanoparticles on MIL-125-NH2 surfaces. Comprehensive characterization and photocatalytic evaluations reveal that the optimized FM-1 catalyst facilitates in situ H2O2 generation and subsequent decomposition into hydroxyl radicals (•OH), enabling efficient CH4 photooxidation. Remarkably, the FM-1 catalyst achieves an exceptional HCHO production rate of 197.79 μmol·gcat–1 with >99.99% selectivity in water vapor, significantly outperforming both pristine FeOOH and MIL-125-NH2 components. This work presents a promising photocatalytic system for selective CH4 conversion, offering new insights into the design of efficient catalysts for C1 chemistry.
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高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Chen Li,Chuncai Zhou,David French,Ian T. Graham,Zixuan Wang,Yunfei Li,Feng Wang,Guijian Liu
As strategic emerging industries represented by clean energy technologies develop rapidly, gallium (Ga), one of the critical elements due to its use in these technologies and limited supply, has attracted worldwide attention. The discovery of appropriate materials to adsorb Ga is crucial for improving the utilization of Ga resources. With the goal to recover Ga ions more efficiently and selectively, carbon nanotubes (CNTs) and amino-functionalized MIL-53 series metal–organic skeletons were hydrothermally synthesized into CNT/NH2-MIL-53(Fe) composite adsorbents. The composite's morphology, structure, chemistry and other physicochemical features were characterized, and the adsorption conditions including pH, initial Ga concentration, along with adsorbent dosage were optimized. The outcomes suggest that 2-CNT/NH2-MIL-53(Fe) performs better than the unmodified material in adsorption, and the theoretical maximum adsorption amount of Ga is 1483.8 mg g−1. The adsorption exhibited a single layer chemisorption with an endothermic spontaneous reaction. The adsorption mechanism for Ga onto 2-CNT/NH2-MIL-53(Fe) was mainly via ion exchange and chelation, accompanied by hydrogen bond interaction. The outstanding adsorption capacity and reproducibility using CNT/NH2-MIL-53(Fe) composites provide a novel method for adsorbing Ga from aqueous solutions.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Shuaitian Jia,Zan Chen,Yinhui Li,Claudia Li,Cuijia Duan,Kang Hui Lim,Sibudjing Kawi
The disposal of waste lithium batteries , especially waste separators, has always been a problem, incineration and burial will cause environmental pollution, therefore, the development of degradable and high-performance separators has become an important challenge. Herein, UiO-66-NH 2 particles were successfully anchored onto bacterial cellulose (BC) separators by epichlorohydrin (ECH) as a crosslinker, then a BC/UiO-66-NH 2 composite separator was prepared by vacuum filtration. The ammonia groups (−NH 2 ) from UiO-66-NH 2 can form hydrogen bonds with PF 6 − in the electrolyte, promoting lithium-ion transference. Additionally, UiO-66-NH 2 can store the electrolyte and tune the porosity of the separator. The lithium ion migration number (0.62) of the battery assembled with BC/UiO-66-NH 2 composite separator increased by 50 % compared to the battery assembled with commercial PP separator (0.45). The discharge specific capacity of the battery assembled with BC/UIO-66-NH 2 composite separator after 50 charge and discharge cycles is 145.4 mAh/g, which is higher than the average discharge specific capacity of 114.3 mAh/g of the battery assembled with PP separator. When the current density is 2C, the minimum discharge capacity of the battery assembled with BC/UiO-66-NH 2 composite separator is 85.3 mAh/g. The electrochemical performance of the BC/UiO-66-NH 2 composite separator is significantly better than that of the commercial PP separator. In addition, -NH 2 can offer a nitrogen source to facilitate degradation of the BC separators, whereby the BC/UiO-66-NH 2 composite separator could be completely degraded in 15 days.
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高影响因子
TALANTA
·
2025
·
IF 6.1
Mengting Liu,Zuncai Gu,Lu Qian,Kawtar Ettayri,Tao Deng,Chenhao Zhang,Jing Qian,Xingyi Huang,Chengquan Wang
Oxytetracycline (OTC), a broad class of antibacterial medication, has been widely utilized in poultry husbandry and fish farming. However, the presence of OTC residues in the food has become a matter of great concern. These residues have the potential to induce the emergence and spread of bacterial resistance, which can have far-reaching consequences for public health. In this work, we focused on the comparison of the quenching efficiency of UiO-66 and its amino group-modified counterpart UiO-66-NH 2 , towards the fluorescence of nitrogen-doped graphene quantum dots (NGQDs) labeled aptamer (NGQDs-apt). It was found that UiO-66-NH 2 demonstrated a more potent fluorescence quenching ability towards NGQDs-apt, as high as 98.8 %, compared to 69.7 % for UiO-66 without amino functionalization. This enhanced performance is attributed to the improved interaction between the amino groups on UiO-66-NH 2 and the NGQDs-apt, facilitating more effective electron transfer. Consequently, UiO-66-NH 2 was selected as the optimal quencher for the development of a highly sensitive aptasensor. This aptasensor demonstrates a quantitative detection range for OTC spanning from 0.001 to 200 μM with an exceptionally low detection limit of 0.25 nM, showing simplicity, accuracy, stability and great potential for antibiotic residue detection in food samples. This work addresses the urgent need to develop reliable methods for detecting OTC residues in food due to the potential of OTC to trigger bacterial resistance, which is crucial for food safety and public health.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
An-qi Tang,Xuechao Xu,Cao-wei Chen,Mengyuan Tan,Lu Gao,Zhen-quan Yang
Enterobacter hormaechei , A zoonotic pathogen with escalating prevalence in global food sources, severely jeopardizes food safety, necessitating the development of high-performance detection methods. Herein, a novel colorimetric detection strategy integrating phages and nanozymes was proposed for foodborne E. hormaechei . Initially, four homologous phages (EhpYZU05, EhpYZU08, EhpYZU9–1 and EhpYZU10), which were isolated using E. hormaechei YZU05 as the host bacterium, were modified on the surface of NH 2 -MIL-88B(Fe) to fabricate four phage@NH 2 -MIL-88B(Fe) nanozymes. These nanozymes exhibit peroxidase-like activity, catalyzing 3,3′,5,5′-tetramethylbenzidine (TMB) chromogenic reaction in presence of H 2 O 2 . With introduction of multiple host or non-host E. hormaechei strains, TMB chromogenic reaction catalyzed by phage@NH 2 -MIL-88B(Fe) nanozymes can be specifically inhibited. This inhibition occurs due to the specific phage adsorption of phage@NH 2 -MIL-88B(Fe) nanozymes towards these host or non-host E. hormaechei strains, indirectly blocking their catalytic sites. Leveraging this principle, colorimetric broad-spectrum detection of E. hormaechei was achieved. Additionally, this method demonstrated reliable recoveries (96.7 % ~ 103.3 %) when applied to detect real food matrices, highlighting its high reliability in practical scenarios. This approach not only clarifies the intrinsic mechanism of phage-modified nanozymes for target bacteria detection but also provides a robust and reliable method for early pathogen detection, thereby significantly contributing to food safety enhancement
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Jin Chai,Chunpeng Liu,Hongtian Yang,Yide Han,Yufeng Liu,Ying Zhang,Xia Zhang
The bifunctions of fluorescence activity and peroxidase mimics were well-integrated by a hemin chloride-modified Zr-based metal–organic framework (Hemin@NH2-UiO-66), which can catalyze the oxidation of o-phenylenediamine (OPD) to generate 2,3-diaminophenazine (DAP), presenting typical peroxidase mimic properties. The influence of the introduction of hemin chloride upon the enhanced peroxidase mimic activity was clarified, and the nanozyme catalytic parameters were optimized. Interestingly, the oxidized product of DAP presents strong fluorescence emission at 564 nm; combining it with the intrinsic fluorescence emission of NH2-UiO-66 at 452 nm, a dual-emission system could be built up by the resulting Hemin@NH2-UiO-66 in the presence of definite OPD and H2O2. Moreover, the fluorescence quenching effect (564 nm) was observed by adding l-cysteine (l-Cys); based on that, a straight-line dependence of the fluorescence intensity ratio (I452/I564) upon the concentrations of l-Cys was established. The detection limit was 0.21 μmol, and the analytical selectivity for l-Cys was also demonstrated. The work highlights the idea of combining the intrinsic fluorescence property and nanozyme catalytic activity in a functional MOF, and its special usability is found in the ratiometric fluorescence sensing analyses.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 13
·期 6
·120451
·
IF 7.2
Yang Li,Guozhe Sui,Mingna Chu,Yan Zhuang,Dongxuan Guo,Shuang Meng,Dantong Zhang,Yue Li,Jinlong Li
Photocatalytic water splitting is a highly promising approach for sustainable hydrogen production. However, a critical challenge lies in developing photocatalysts that simultaneously achieve efficient charge separation and abundant catalytic active sites. Herein, a novel heterojunction system composed of ZnIn 2 S 4 integrated with copper-modified UiO-66-NH 2 (ZnIn 2 S 4 /Cu-UiO-66-NH 2 ) is developed as an efficient photocatalyst for hydrogen production. The optimal ZnIn 2 S 4 /Cu-UiO-66-NH 2 exhibits a hydrogen evolution rate of 630.25 μmol g −1 h −1 under visible-light irradiation, demonstrating a remarkable 114-fold enhancement compared to pristine UiO-66-NH 2 . The excellent photocatalytic performance originates from the novel Z-scheme charge transfer mechanism between ZnIn 2 S 4 and Cu-UiO-66-NH 2 , which facilitates efficient charge separation while maintaining strong redox capabilities. Furthermore, the incorporated Cu species serve as highly efficient active sites for hydrogen evolution. This work provides a rational design strategy for constructing Z-scheme heterojunctions, advancing the development of efficient artificial photosynthesis systems for sustainable energy applications.
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