APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
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IF 24.319
Shihui Wang,Yuzhou Xia,Guiyang Yan,Meixia Chen,Xuxu Wang,Ling Wu,Ruowen Liang
Inspired by the concept of frustrated Lewis pairs (FLPs) from homogeneous catalysis, an organic supramolecular bridged metal-organic frameworks (MOFs) heterojunction, i.e., a perylene-3,4,9,10-tetracarboxylic diimide@MIL-125(Ti)-NH 2 (denoted PDI@MTi) composite is successfully fabricated via a two-step synthesis method. Experimental characterisations and theoretical calculations reveal that in the obtained “TiO 5−x -ligand-PDI” FLPs, the unsaturated Ti-O clusters function as a Lewis acid to accept photogenerated electrons, and the PDI sites act as a Lewis base to capture photogenerated holes. With the unique structure characteristics, the PDI@MTi shows excellent photocatalytic activity toward the disinfection of Staphylococcus aureus and Cr(VI) reduction, with 1.0- and 10.3-fold enhancements, respectively, compared with unadorned MTi. The synergic effects of the micro polarisation field, multiple active sites, and a C-N bonded interface contributed to photoactivity enhancement. This work demonstrates the potential of using MTi as a platform for constructing FLPs-containing heterogeneous photocatalysts and provides new strategies to control carrier separation.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
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IF 9
Ziheng Li,Fengting Yao,Yan Dai,Xuehua Ruan,Xiaobin Jiang,Xuemei Wu,Wenji Zheng,Gaohong He
Metal-organic frameworks (MOFs) offer exceptional pore tunability for targeted separations. Moving beyond conventional defect engineering which often sacrifices selectivity for permeability, we propose to construct functionalized defects that synergistically integrate hierarchical low-resistance gas transfer pathways with tailored ultra-CO 2 -philic molecular domains. This strategy is achieved by in-situ embedding β-cyclodextrin (β-CD) as a multifunctional modulator during the crystallization of NH 2 -UiO-66 (NUiO). The macrocyclic cavities of β-CD induced structural defects cooperatively optimize the pore architecture of NH 2 -UiO-66, significantly enhancing gas permeability. Concurrently, exposed Zr 6 clusters and hydroxyl groups from β-CD enhance CO 2 adsorption capacity. Furthermore, defect-induced incomplete coordination promotes hydrogen bonding between the β-CD@NUiO and Pebax, improving interfacial compatibility for MMMs. The prepared β-CD 20 @NUiO MMM at 5 wt.% filler loading exhibits a CO 2 permeability of 125.5 Barrer and a CO 2 /N 2 selectivity of 112.4, exceeding the 2019 McKeown upper bound. The in-situ construction of defects via functional molecules transcends the limitations of single-parameter optimization for mass transfer pathways and active sites in porous materials, establishing a universal design principle for multifunctional coupled separation materials.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Meimei Zhou,Wei Zou,Xuemei Zhu,Huachen Ma,Pengbo Wang,Jiaxin Shang,Pingping Luo
UIO-66-NH 2 was successfully deposited on electrospun polyacrylonitrile (PAN) nanofibers treated by thermal oxidative stabilization (TOS) via a simple and effective in situ growth method. Owing to the formation of acridone rings, naphthyridinering rings and hydronaphthyridine rings during the TOS process, the thermally stabilized electrospun PAN (TSPAN) nanofibers were greatly improved in stability and heat resistance and could provide adequate nucleation points for MOFs growth, indicating an ideal MOFs deposition support without additional surface modifications. The results demonstrated that UIO-66-NH 2 crystals distributed relatively uniform and dense on the TSPAN nanofibers with mass loading up to 28.1 wt%. Compared with powdered UIO-66-NH 2 , the formed UIO-66-NH 2 @TSPAN nanofibers showed enhanced visible light driven photocatalytic activity towards reduction of Cr(VI) due to the improvement of visible light response, more excellent photothermal conversion ability and the increase of exposed active sites. The photocatalytic reduction rate of Cr(VI) over UIO-66-NH 2 @TSPAN was up to 93% within 180 min and the rate constant (k = 0.1362) was 2.3 times that of powdered UIO-66-NH 2 (k = 0.00576). Significantly, the mechanical flexibility and structural stability endowed the nanofibrous photocatalyst easy operation and outstanding reusable capability. The photocatalytic activity for Cr(VI) reduction still preserved 90% after five cycles. This work proposes a facile strategy for preparation of free-standing MOFs nanofibers and provides MOFs-based photocatalysts a new opportunitie for broad applications in water treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Wei-Guang Yang,Xin-He Feng,Xuwen Wu,Zhong-Zhen Yu,Dongzhi Yang
Two typical chemical warfare agents—nerve agents and blister agents—pose a serious threat to human life. Under atmospheric conditions devoid of free water, however, the rapid degradation and complete elimination of these agents using anhydrous catalysts remain significant challenges. To overcome this limitation, a LiCl+AC-MOF composite catalyst with moisture-induced wetting surface is prepared by in-situ growing UiO-66-NH 2 on the activated carbon particles, and then confining LiCl crystallization in the nanocavities of UiO-66-NH 2 . In humid atmosphere (RH = 90%), the confined LiCl undergoes deliquescence within the UiO-66-NH 2 nanocavities, thereby generating a continuous wetting surface. This mechanism yields an impressive water uptake of 1.61 g g −1 , which significantly enhances the equilibrium water content at the gas-solid boundary of the composite catalyst. Leveraging the abundance of free water to the Zr sites, the composite catalyst facilitates the rapid hydrolytic degradation of the nerve agent simulant dimethyl 4-nitrophenyl phosphate with a half-life of 1.9 h at RH = 90%. For the blister agent simulant 2-chloroethyl ethyl sulfide, the catalyst not only cleaves the C S and C Cl bonds but also utilizes its wetting surface to accelerate the recombination of intermediate into final products (half-life = 0.4 min at RH = 70%). In summary, the highly efficient catalyst designed in this work spontaneously harvests atmospheric moisture to create a self-wetting surface. This distinctive surface chemistry enhances both the mass transfer of chemical warfare agent simulants and their subsequent active degradation at Zr sites, thereby substantially broadening the design scope for advanced chemical protective materials applicable to next-generation respirators and gas masks.
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TALANTA
·
2026
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IF 6.7
Wanyi Zhang,Chenyu Zhou,Hanbo Wang,Yuhan Chen,Tingting Xia,Xingguang Su
Quercetin, a potent natural antioxidant, is gaining widespread attention for its remarkable health benefits, including the prevention of cardiovascular diseases, allergies, diabetes, and cancer. As a promising functional food ingredient, there is an urgent need for fast, sensitive, and portable methods to monitor quercetin levels in various products. In this study, we present a portable dual-mode nanozyme-driven sensor based on cerium dioxide nanoparticle-anchored metal-organic framework (CeO 2 @UiO-66-NH 2 ) nanocomposite. This nanocomposite exhibits impressive oxidase-like activity and intrinsic fluorescence properties, enabling it to catalyze the oxidation of colorless N, N-diethyl-p-phenylenediamine to a pink product, which in turn quenches the fluorescence of CeO 2 @UiO-66-NH 2 at 458 nm via an inner filter effect (IFE). The presence of quercetin inhibits reactive oxygen species generation, thus attenuating the oxidation and restoring fluorescence. A paper-based fluorescent-colorimetric dual-mode sensing platform was established for quercetin detection, enabling rapid and visual evaluation without complex instruments. The proposed method exhibited a broad linear response range of 1-60 μM. The limits of detection for the colorimetric/fluorescent and paper-based colorimetric/fluorescent were 0.35, 0.27, 0.37, and 0.29 μM, respectively. This dual-mode sensor demonstrates excellent analytical sensitivity and selectivity, with successful application in real vegetable and juice samples, offering a reliable, efficient tool for quercetin monitoring in food and functional food ingredients.
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Catalysis Science & Technology
·
2026
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IF 4
Hurunqing Liu,Lin Ye,Yun Yuan,Quanyuan Wang,Dengrong Sun,Zhaohui Li
Light-driven one-pot tandem/cascade reactions have attracted increasing interest due to their green process and atomic efficiency. In addition to active sites, the adsorption behavior of reaction substrates also plays a critical role on the catalytic process, but is always overlooked. Herein, we report that modulating the reaction substrates to regulate the adsorption behavior of intermediates can effectively facilitate one-pot multi-step reactions. O-Nitroaniline is strategically selected to replace the commonly used o-phenylenediamine for reaction with benzyl alcohol to synthesize benzimidazole in a one-pot process under visible-light irradiation. The use of o-nitroaniline effectively promotes the adsorption of the benzyl alcohol-derived aldehyde intermediate on the catalyst but weakens the adsorption of o-nitroaniline-derived o-phenylenediamine. Thus, the condensation between these two intermediates can proceed smoothly, alleviating the fatal polymerization side reaction of o-phenylenediamine, affording high efficiency in light-driven benzimidazole production. Departing from the conventional catalyst design, this work underscores an effective way to modulate the reaction substrates for accelerated one-pot synthesis, signifying an important contribution to the design of one-pot synthesis systems.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124516
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IF 7.5
Bingkun Liu,Juncheng Guo,Hongda Huang,Yuhan Yang,Jingtao Zhang,Junling Zhang,Yonghui Zhang
Constructing a robust interfacial electric field is crucial for efficient spatial separation and directional migration of photogenerated carriers, which further boosts the performance of photocatalytic systems. In this study, a novel CF-supported SnS 2 /UiO-66-NH 2 high-low junction with intimate interface was fabricated via an in-situ solvothermal process. The optimal CF@SnS 2 /UiO-66-NH 2 -2 catalyst shows the best photocatalytic efficiency of 99.5% Cr(VI) removal at pH of 2.0 and nearly complete E. coli inactivation within 150 min, revealing its good photocatalytic redox capability. Moreover, the as-prepared composite possesses remarkable stability and desirable recycling performance. Mechanism analysis reveals that the intense internal electric field (IEF) and energy band bending are pivotal for promoting the separation and migration of charge carriers in the CF@SnS 2 /UiO-66-NH 2 high-low junction. This work offers new insights into the preparation and application of high-low junction photocatalysts.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
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IF 4.182
Weina Shi,Yanqing Zhu,Cong Shen,Jifu Shi,Gang Xu,Xiudi Xiao,Runqiang Cao
Thermochemical heat storage based on inorganic salt hydrates is a promising approach to relieve the heat energy supply and demand conflicts, but there exist lots of defects of pure salts when applied to the thermochemical. This paper attempted to use functionalized Metal-Organic Frameworks (MOFs) as the porous matrices to improve the heat storage performance of inorganic salt hydrates. A series of MOFs/CaCl 2 composites based on MIL-101(Cr)-X (X = -NH 2 , –SO 3 H, H, –CH 3 , –F) were successfully synthesized and fully characterized by combining multiple techniques (i.e. powder X-ray diffraction, scanning electron microscopy , energy-dispersive X-ray analysis, N 2 adsorption-desorption, Fourier transform infrared spectroscopy , thermogravimetric and differential scanning calorimetry). The water sorption properties of the series of MOFs/CaCl 2 composites were studied during the hydration process, and a continuous adsorption/desorption experiment was also performed to investigate the cycle stability of the MOFs/CaCl 2 composites. The results show that the hydrophilic MOFs based composites have higher water sorption capacity (0.6 g(H 2 O)/g(sample) for MIL-101(Cr)–SO 3 H/CaCl 2 ) accompanied with higher heat storage density (1274 J/g for MIL-101(Cr)–SO 3 H/CaCl 2 ). Moreover, the series of MOFs all presented excellent cycle performance with little loss after continuous 17 adsorption/desorption cycles.
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高影响因子
Journal of Environmental Sciences
·
2026
·
IF 6.5
Xiaoxia Liang,Zewan Qin,Siwei Zhang,Rong Hai,Lingqing Gu,Xia Yang
30CNQDs@NMT/PMS achieved almost complete degradation of malathion within 30 min simulated sunlight irradiation. • CNQDs was integrated successfully to promote the charge separation efficiency as electron bridges and enhance the adsorption energy of PMS for activation revealed by DFT. • •OH and •SO 4 – were generated to attack the identified sites of malathion computed via Fukui function. • The intermediate products in the photocatalytic process were less toxic than malathion assessed by T.E.S.T. Malathion, an organophosphate pesticide widely used in agricultural fields across the world, has raised environmental concerns due to its persistence and toxicity. Thus, a novel photocatalyst was synthesized by integrating carbon nitrogen quantum dots (CNQDs) onto NH 2 -MIL-125(Ti) (NMT) via a solid-phase thermal polycondensation method. It was demonstrated that CNQDs served a dual function as electron bridges to facilitate charge separation and as peroxymonosulfate (PMS) adsorption activation sites substantially enhancing the photocatalytic activity, which was revealed by Density Functional Theory (DFT). Under simulated sunlight, 30CNQDs@NMT achieved nearly 100 % malathion removal within 30 min via PMS activation, exhibiting 8.1 times higher than NMT. While •OH and •SO 4 – acted as the dominant reactive species to attack the malathion sites. The toxicity of the intermediate products assessed by T.E.S.T. (Toxicity Estimation Software Tool) were much lower than malathion. Moreover, 30CNQDs@NMT performed effectively in real water matrices, demonstrating its potential for practical environmental applications. Download: Download high-res image (233KB) Download: Download full-size image
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Catalysts
·
2026
·Vol. 16
·期 5
·397
·
IF 4.5
Henan Shang,Qi Jia,Shilei Zhang,Sijia Li,Jinsheng Liang
A novel citric acid-assisted in situ reduction method has been developed for the synthesis of bimetallic AuPd alloy nanoparticles supported on amine–phosphate-functionalized carbon nanotubes (AuPd/NH2-P-CNTs). In this strategy, formic acid acts not only as the reducing agent for reducing metal precursors, but also as the hydrogen source for the subsequent catalytic dehydrogenation. The introduction of citric acid significantly accelerates the reduction kinetics and promotes the uniform formation of ultrafine AuPd nanoparticles (∼1.8 nm). As a result, the optimized Au0.5Pd0.5/NH2-P-CNTs exhibit an extraordinary catalytic activity and 100% H2selectivity during hydrogen generation from FA with sodium formate as an additive, affording a remarkable initial turnover frequency of 5663.94 mol H2mol Pd−1h−1at 303 K. The experimental results reveal that the -NH2and -P functional groups on the support are crucial for stabilizing and uniformly dispersing the alloy nanoparticles. Furthermore, the enhanced reaction rate can be attributed to the strong metal–support interaction established between AuPd nanoparticles and -NH2-P-CNT supports. This work provides a new perspective on the design of highly efficient Pd-based catalysts for hydrogen production from formic acid.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Jun-Chuan Wang,Peng-Liang Zhang,Wen-Bo Zhang,Tai-Sen Zhang,Zi-Yan Zhen,Tian-Yu Wang,Xiang-Xiang Jia,Gang Yu
Modulating localized electronic structures and interfacial charge-transfer pathways in metal-organic framework (MOF)-based heterogeneous catalysts remains a critical challenge for achieving efficient and durable advanced oxidation processes. Herein, a highly crystalline S-scheme NH₂-MIL-101(Fe)@DQ-TFP (NM@DT) core-shell heterojunction was constructed through a microwave-assisted MOF-first in situ growth strategy. Distinct from conventional physical assembly, the anthraquinone-based β-ketoenamine covalent organic framework (COF) shell was integrated with the amino-functionalized MOF core through chemically coupled growth and interfacial hydrogen-bonding interactions, generating a robust core-shell interface. This intimate interfacial coupling induces spontaneous electronic redistribution and charge polarization, which are verified by X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and density functional theory calculations, thereby providing the electronic basis for an internal electric field-assisted S-scheme charge-transfer pathway. The optimized NM@DT-3 heterostructure exhibits enhanced photocatalytic tetracycline degradation performance, achieving 90.70% removal efficiency within 180 min without external H₂O₂ addition. The core-shell configuration not only promotes interfacial charge separation but also creates a spatially confined catalytic microenvironment, enabling efficient oxygen activation and reactive oxygen species evolution coupled with localized H₂O₂ activation at adjacent Fe centers. Mechanistic investigations reveal that freely diffusing hydroxyl radicals (·OH) make only a minor contribution under the tested conditions, whereas superoxide radicals (·O₂⁻), photogenerated holes (h⁺), and singlet oxygen (¹O₂) participate in TC oxidation. In this reaction network, ·O₂⁻ acts as a key intermediate linking photocatalytic O₂ reduction to both H₂O₂ formation and a proposed h⁺-mediated ¹O₂ generation pathway. The reduced reliance on conventional bulk ·OH-dependent chemistry is consistent with the retained catalytic activity of NM@DT-3 under alkaline conditions, with a TC removal efficiency of 77.74% at pH 10. Meanwhile, the chemically integrated core-shell structure effectively suppresses iron leaching, with only 0.107 mg L⁻¹ Fe released during the photocatalytic process. This work provides new insights into engineering chemically coupled MOF/COF interfaces for regulating interfacial charge migration and ROS evolution, offering an effective strategy for constructing stable photo-self-Fenton catalysts for environmental remediation.
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FOOD CHEMISTRY
·
2026
·
IF 10.4
Ruyue Zhang,Xuan Liu,Bini Wang,Fuxin Zhang,Yufang Liu
Lactoferrin (LF) is widely used in healthcare and food industry as an antibacterial and functional additive. Its complex structure makes rapid detection challenging. Here, an antibody-free molecularly imprinted (MIP) electrochemical sensor was developed using Ti 3 C 2 MXene and UiO-66-NH 2 nanomaterials to construct an imprinted layer for the rapid and efficient detection of LF in dairy products. The incorporation of Ti 3 C 2 MXene@UiO-66-NH 2 @PPy (TiPU) enhanced the surface area and conductivity of the material, and MIP provided specific cavities that were precisely matched to LF in terms of size, shape, and chemical functional groups. Molecular docking simulations confirmed the reliability of LF MIP compound formation. The synthesized nanocomposites (MIP-TiPU) were characterized by various methods, including their morphology, structure, and electrochemical properties. The MIP-TiPU modified electrochemical sensor displayed an outstanding sensing performance for LF detection, with a wide linear response range from 5 ng/mL to 500 ng/mL and a low detection limit (0.98 ng/mL).
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