CATALYSIS LETTERS
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2020
·Vol. 150
·期 6
·1786-1797
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IF 2.482
Jiang Haoran,Lu Biao,Ma Lijuan,Yuan Xia
Abstract The esterification of cyclohexene with formic acid is the first step for indirect hydration to cyclohexanol. In the work reported in this study, phosphotungstic acid (HPW) was incorporated into the metal–organic framework Cu 3 (BTC) 2 through a one-step hydrothermal synthesis method to catalyze the esterification reaction. The crystal structure of composite HPW–Cu 3 (BTC) 2 was modulated during the preparation process to convert the catalyst from the {111} crystal facets of the original regular octahedral structure to the {100} crystal facets of the cubic structure using p-toluic acid (pTA) as the regulator. The conversion of the crystal facets reduces the formation through holes while exposing more active sites of HPW. When the mass ratio of the modulator to the organic ligand terephthalic acid was 20, the crystal facets of the catalyst were completely covered by the {100} crystal facets. After the crystal transformation, the conversion of cyclohexene was increased to 86.8%, and the selectivity of cyclohexyl formate was 84.2%. Agglomeration occurred after the catalyst was used twice in the esterification reaction. Graphic Abstract HPW was incorporated into the metal-organic framework Cu 3 (BTC) 2 through a one-step hydrothermal synthesis method and used for catalyzing the esterification reaction of cyclohexene with formic acid. The crystal structure of composite HPW–Cu 3 (BTC) 2 was modulated during the preparation process to convert the catalyst from the {111} crystal facets of the original regular octahedral structure to the {100} crystal facets of the cubic structure using p-toluic acid (pTA) as the modulator.
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
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2022
·
IF 6.056
Chunyun Ma,Yan Zhang,Chuankai Yang,Yuhang Zhang,Miaorong Zhang,Jianguo Tang
Cetyl trimethyl ammonium bromide (CTAB)-activated lipase-mineral hybrid microflowers (CTAB-Lip-MHFs) were fabricated via biomineralization using Cu 3 (PO 4 ) 2 ⋅3H 2 O as the mineral for olive oil hydrolysis. FT-IR spectra indicated that immobilized lipase molecules in CTAB-Lip-MHFs has good structural integrity, and XPS spectra revealed that immobilized lipase molecules were present at the surface of CTAB-Lip-MHFs. Kinetic studies suggested that CTAB-Lip-MHFs had good substrate affinity ascribed to interfacial effect caused by CTAB, meanwhile, the open conformation of lipase activated by CTAB contributed to increased reaction rate with substrate. The generated fatty acids via hydrolysis of olive oil by CTAB-Lip-MHFs were 146% of that by free lipase, moreover, CTAB-Lip-MHFs could retain 76.5% and 93.2% of initial activities after storage at 50 °C for 10 h and 4 °C for 30 days, respectively, indicating the good stability of CTAB-Lip-MHFs. In addition, after 5 recycles, CTAB-Lip-MHFs preserved 72.7% of initial activity, demonstrating the favorable reusability of CTAB-Lip-MHFs for fatty acid production.
研究领域:
生物化学
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酶工程
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-8
·
IF 14.7
Wang Guang,Fan Hongzhao,Li Jiawang,Li Zhigang,Zhou Yanguang
Improving interfacial thermal transport is crucial for heat dissipation in devices with interfaces, such as electronics, buildings, and solar panels. Here, we design a strategy by utilizing the water adsorption-desorption process in porous metal-organic frameworks (MOFs) to tune the interfacial heat transfer, which could benefit their potential in cooling or heat dissipation applications. We observe a changeable thermal conductance across the solid/porous MOF interfaces owing to the dense water channel formed by the adsorbed water molecules in MOFs. Our experimental and/or modeling results show that the interfacial thermal conductance of Au/Cu 3 (BTC) 2 , Au/Zr 6 O 4 (OH) 4 (BDC) 6 and Au/MOF-505 heterointerfaces is increased up to 7.1, 1.7 and 3.1 folds by this strategy, respectively, where Cu 3 (BTC) 2 is referred to as HKUST-1 and Zr 6 O 4 (OH) 4 (BDC) 6 is referred to as UiO-66. Our molecular dynamics simulations further show that the surface tension of Au layer will cause the adsorbed water molecules in MOFs to gather at the interfacial region. The dense water channel formed at the interfacial region can activate the high-frequency lattice vibrations and act as an additional thermal pathway, and then enhance heat transfer across the interfaces significantly. Our findings revealed the underlying mechanisms for tailoring thermal transport at the solid/porous MOF heterointerfaces by water adsorbates, which could motivate and benefit the new cooling system design based on MOFs.
研究领域:
材料科学
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热能工程
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纳米技术
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表面科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Yuli Kou,Kangkang Wang,Mailidan Wumaer,Changyan Guo,Bingren Tian,Li Zhang,Naeem Akram,Jide Wang
As an important family of semiconductors, transition metal phosphides could act as effective catalysts in the treatment of organic pollutants. Herein, a novel hollow core–shell Cu@Cu 3−x P catalyst with copper vacancies, possessing excellent properties of photocatalytic and catalytic reduction for organic pollutants, was prepared by the vapor deposition method. 4-Nitrophenol (4NP) (50 μM, 3 mL) could be degraded within 2 min under the action of catalyst (0.06 mg), and the reduction rate was approached to 99.8%. Meanwhile, this catalyst displayed prominently increased Rhodamine B (RhB) photo-oxidation performance, about 1.7 and 16 times more than the bare Cu 3 P and Cu under optimal conditions (5% Cu@Cu 3−x P). Such superior catalytic performance can be ascribed to the mutual contribution of Cu vacancy (convert the band structure and supply active sites) and Cu nanowire (prevent agglomeration of Cu 3 P nanoparticles and promote the transfer of photoelectrons) and the unique hollow core–shell architecture(the rapid separation and low recombination of photoelectron-hole). The possible pathways of 4NP reduction and RhB photo-oxidation were proposed according to the results of degradation products obtained from HPLC, LC-Q-orbitrap/MS, GC-MS, and ATR-FTIR. This study can validate the extensive application of Cu@Cu 3−x P and provide a new insight for the synthesis of dual-functional catalysts containing metal defects.
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高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Dong Zhang,Ren Ma,Haozhe Liu,Zhengqiang Xia,Gang Xie,Sanping Chen
Constructing S-scheme heterojunctions on two-dimensional (2D) conductive metal–organic frameworks (c-MOFs), which possess high specific surface area, abundant active sites, and excellent electrical conductivity, is widely regarded as an effective strategy to enhance photocatalytic performance. In this study, an S-type heterojunction was fabricated by coupling a 2D c-MOF, Cu3(HHTP)2, with In2S3 to synergistically improve photocatalytic activity. Unlike conventional flake-like heterojunctions that often block the vertical pore channels of c-MOFs, we synthesized rod-like Cu3(HHTP)2/In2S3 composites through controlled morphological engineering. Experimental results demonstrate the resulting nonplanar interfacial contact effectively preserves the intrinsic pore architecture while fully exposing the dz2 orbitals of Cu active centers. Structural analyses reveal that the rod-like Cu3(HHTP)2 interacts with In2S3 predominantly via In–O bonds formed on its lateral facets, thereby maintaining the inherent porosity and exposing a large number of active sites. Consequently, the CO2 adsorption capacity reaches 13.44 cm3·g–1, 2.18 times higher than that of the flake-like Cu3(HHTP)2/In2S3 composite that In2S3 is bonded via Cu–S bonds on the surface. Moreover, the incorporation of In2S3 enhances interlayer charge transport within the rod-like structure. As a result of these synergistic effects, the electron consumption rate of the rod-like heterojunction is 1.73 times greater than that of its flake-like counterpart. The unique architecture not only retains the in-plane charge transport advantages derived from d-π conjugation in c-MOFs but also introduces interlayer electron-bridging pathways through In2S3, leading to significantly improved electrical conductivity and charge separation efficiency.
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高影响因子
MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Yao Jin,Xiangwei Yuan,Junchun Guo,Li Xu,Qian Wang,Xiaoli Xiong
Dopamine (DA) is a central neurotransmitter that plays a crucial role in human metabolism. Its precise detection is of great importance in disease diagnosis. Compared with single-signal detection methods, colorimetric and electrochemical dual-signal outputs can self-validate the measured data and counteract interference effects, which is expected to provide more reliable detection results. In this paper, carbon nanofiber-supported 3D bristlegrass-like π-conjugated conducting metal–organic frameworks ( c MOF) Cu 3 (HHTP) 2 nanorod arrays (Cu 3 (HHTP) 2 NRAs/CNF) catalyst with core–shell structure are synthesized by electrospinning and solvothermal reaction. The obtained catalyst possesses remarkable peroxidase-like activity which can catalyze the colorless 3,3′,5,5′ −tetramethylbenzidine (TMB) to blue oxTMB. The mechanism study showes that ·OH radicals are the main active substances. Meanwhile, the core–shell structure between π-conjugated cMOF and CNF can effectively inhibit the aggregation of Cu 3 (HHTP) 2 nanorods and generate more catalytic active sites, resulting in strong electrocatalytic activity of Cu 3 (HHTP) 2 NRAs/CNF. As a result, a novel dual-mode sensor based on colorimetric and electrochemical are constructed for detecting dopamine (DA) with a good linear relationship ranging from 2.5-60 μM and 0.1–106 μM, and the limit of detection (LOD) are 0.27 μM and 10.1 nM (S/N=3), respectively. This study opens up a new idea for the application of c MOF peroxidase-like enzyme in sensing field.
研究领域:
生物医学工程
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分析化学
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高影响因子
FOOD CHEMISTRY
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2024
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IF 8.5
Yao Jin,Xiangwei Yuan,Lian Ou,Jiaying Wu,Jiangtao Hu,Kang Xue,Xiaoli Xiong
Formaldehyde is known to harm the respiratory, nervous, and digestive systems of people. In this paper, a novel dandelion-like electrocatalyst with core–shell heterostructure arrays were fast self-assembled prepared in situ using copper foam (CF) as support substrate and 2,3,6,7,10,11 hexahydroxy-triphenyl (HHTP) as ligand (Cu(OH) 2 @Cu 3 (HHTP) 2 /CF) by a simple two-step hydrothermal reaction. The 1D Cu(OH) 2 nanorods “core” and the 2D π-conjugated conducting metal–organic frameworks (Cu 3 (HHTP) 2 c MOF) “shell” with remote delocalized electrons give the dandelion-like heterogeneous catalysts excellent electrochemical activity such as a large specific surface area, high conductivity and a fast electron transfer rate. The Cu(OH) 2 @Cu 3 (HHTP) 2 /CF exhibited excellent electrocatalytic performance for formaldehyde under alkaline conditions with a linear range of 0.2 μmol/L – 125 μmol/L and 125 μmol/L – 8 mmol/L, a detection limit as low as 15.9 nmol/L (S/N = 3), as well as good accuracy, consistency, and durability, and it effectively identified FA in food.
研究领域:
化学传感器
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材料科学
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食品安全检测
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Qinhan Wu,Pengkun Zhang,Dong-Hau Kuo,Binghong Wu,Adugna Boke Abdeta,Zhengjie Su,Longyan Chen,Osman Ahmed Zelekew,Jinguo Lin,Xiaoyun Chen
Monoclinic lindgrenite (Cu 3 (MoO 4 ) 2 (OH) 2 )-like CuMoOS oxysulfide catalyst with high catalytic activity in the dark was synthesized by a facile method. Hydrazine reduced cations to increase Cu + and Mo 4+ proportions, sulfur doping was used to diminish the problem of poor stability caused by the excessive deviations of the catalyst from electric neutrality due to the high Cu + and Mo 4+ concentrations. The ratios of Cu + /Cu 2+ and Mo 4+ /Mo 6+ ions affected the catalytic activity of CuMoOS catalysts. The CuMoOS with a Cu + /(Cu + +Cu 2+ ) ratio of 0.708 showed abundant oxygen vacancies and the best catalytic reduction effect. Through controlling the Cu + content of the catalyst, its defective structure, and electron transfer resistance, the reduction reaction with NaBH 4 can be effectively adjusted. CuMoOS-3 catalyst shows a complete catalytic reduction of 4-NP (50 ppm) within 4 min 50 ppm MB, RhB and MO organic dyes were completely reduced within 4 min, 6 min, and 8 min, respectively. At the same time, Cr 6+ , as a model heavy metal ion , was completely reduced in 12 min, and its pseudo-first-order reaction kinetic constant reached 0.1709 min −1 . Good stability was kept after six cycling experiments. Therefore, the high-efficiency CuMoOS catalyst synthesized by green procedures displays the potential for industrial application.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
FOOD CHEMISTRY
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2024
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IF 8.5
Xin Zhang,Shuyan Miao,Wenjie Song,Xian Liu,Can Wu,Tian Gan
It is highly desirable to develop a low-cost and rapid detection method for trace levels of carbendazim fungicide residues, which would be beneficial for improving human health and mitigating environmental issues. Herein, isolated single tungsten atoms were implanted onto well-organized metal–organic framework (MOF)-derived N-doped carbons to form W-N-C single-site heterojunctions with ultrahigh electrocatalytic activity . The coupling of W-N-C with Cu 3 (HHTP) 2 , an electronically conductive MOF with a large surface area and porous structure, exhibited enhanced electrocatalytic performance for the oxidation of carbendazim (CBZ) when they were used for decorating graphene nanoplatelet flexible electrode arrays fabricated via template-assisted scalable filtration. A wide linear range (3.0 nM–50 μM) with an ultra-low detection limit of 0.97 nM and fast response was achieved for CBZ analysis. Moreover, the sensing platform has been utilised to monitor CBZ levels in vegetable samples with satisfactory recovery rates of 97.2–102% and a low relative standard deviation of 1.9%.
研究领域:
环境科学
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分析化学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2014
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IF 4.908
Cuijia Duan,Xingming Jie,Dandan Liu,Yiming Cao,Quan Yuan
In this work a series of mixed matrix membranes (MMMs) containing metal organic frameworks (MOFs) were fabricated to investigate the influence of post-treatment on their gas separation properties. It was revealed that gas permeabilities increased considerably as treatment temperature increased from 150 °C to 180 °C and remained almost unchanged after 200 °C; gas permeability of MMMs from 200 °C treatment was about 3 times higher when compared with MMMs treated at 150 °C. From results of physical characterization including TGA , XRD , SEM, ATR-FTIR and nitrogen absorption it was inferred that higher temperature treatment induced gas permeability increase should be mainly attributed to more effective removal of residual solvent in micro-pores of MOFs; and gas permeation properties of MMMs with different treatment durations from 24 h to 96 h further confirmed our conclusion. This heat treatment induced permeability increase phenomenon was further verified by varying the polymer and MOF combinations. At the end Cu 3 (BTC) 2 /ODPA–TMPDA MMMs with different MOF loadings were prepared and the one with best performance appeared at 40 wt% loading: a dramatic increase of CO 2 permeability from 47.7 Barrer to 260.7 Barrer with almost unchanged CO 2 /CH 4 selectivity from 29.26 to 27.75.
研究领域:
化学工程
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材料科学
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膜技术
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DOI
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Jiani Yang,Chao Xiong,Mi Zhou,Xianglin Luo,Xikui Liu,Chong Cheng,Chao He,Xiaohui Xu
Considering the intrinsic limitations of natural enzymes, the development of efficient, cost-effective artificial enzyme alternatives has become imperative. Covalent metal-organic frameworks (CMOFs), as a new type of open framework materials with precise crystalline structures, clear metal catalytic sites, ordered pores and strong designability, can be considered as an ideal platform to develop efficient artificial enzyme materials. Here, we report two distinct enzyme-mimetic CMOFs, Tbpa-Ag3 and Tbpa-Cu3, which featured cyclic trinuclear metal clusters (Ag3/Cu3) as functional nodes respectively. Among the two CMOFs, Tbpa-Ag3 achieved precise spatial integration of photoactive Tbpa ligands with catalytic Ag3 clusters, establishing a more efficient electron transfer pathway that delivered superior oxidase-like activity under visible-light irradiation. Based on Tbpa-Ag3, we engineered a biomarker detection platform for physiological antioxidants (L-Cysteine and GSH) and a sustainable photocatalytic system for benzylamine oxidative coupling (yield > 99%, 4 h), validating Tbpa-Ag3’s dual functionality in analytical chemistry and green catalysis.
研究领域:
材料科学
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纳米技术
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催化
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分析化学
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绿色化学
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生物无机化学
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配位化学
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传感器技术
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有机合成
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高影响因子
危险品化学品经营许可证（带存储）