Energy Technology
·
2025
·
IF 3.6
Hui Huang,Qi Xu,Liangyun Yu,Lidong Li,Ying Zhang,Fennv Han,Qi Zhang
Currently, there is a thermodynamic and kinetic mismatch between carbon dioxide methanation. Carbon dioxide is stable in nature and requires a highly active catalyst to facilitate its reduction reaction. In this article, Ru/ZrO 2 catalysts are prepared by a structure-directed derivatization strategy using zirconium-based metal-organic frameworks (MOFs) (UiO-66) as precursors. The porous framework structure of MOFs was utilized to construct Ru nanoparticles with a large size (≈9.7 nm). Photothermal catalysis is employed, and the photoexcitation induced the transfer of electrons from the conduction band of ZrO 2 to Ru, which elevated the electron density of Ru to the enriched state and promoted the activation of CO 2 adsorption, while the photothermal effect facilitated the warming of the catalyst bureau, which provided a favorable condition for CO 2 methanation. The compositional valence, morphology, specific surface area, bandgap and other properties of the catalysts were evaluated by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscpe, Brunner-Emmet-Teller measurements, hydrogen temperature-programmed reduction, CO 2 -TPD, ultraviolet–visible, photoluminescence, and photocurrent response characterization. The experimental results showed that 99% methane selectivity and 120.354 mmol g cat −1 h −1 methane yield were achieved at 1 MPa and photothermal (250 °C) conditions.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Yongtong Lei,Jinglong Zhao,Haiming Song,Fanhang Yang,Luli Shen,Lijing Zhu,Zhixiang Zeng,Xiaocheng Li,Gang Wang
UiO-66-based metal-organic framework (MOF) materials are a class of porous crystalline materials consisting of Zr metal clusters compounded with organic ligands of terephthalic acid group. In this study, functionalized UiO-66-X ( X =H , NH 2 , (COOH) 2 ) nanoparticles were synthesized. The morphology of UiO-66-X nanoparticles were characterized by SEM, while the crystal structure was analyzed using XRD and TGA . Chemical composition of UiO-66-X nanoparticles were analyzed through TFIR and XPS . The adsorption capacities of UiO-66-X nanoparticles for anionic dye of Congo red (CR), and cationic dyes of methylene blue (MB) and rhodamine B (Rh B) dyes were evaluated. Furthermore, the adsorption mechanisms of UiO-66-X nanoparticles for dyes were analyzed and summarized. Results showed that the adsorption capacities of UiO-66 and UiO-66-NH 2 on CR were 93.05 mg/g and 94.20 mg/g, respectively. In particular, the adsorption capacities of UiO-66-(COOH) 2 on MB and Rh B were significantly increased with the adsorption capacities of 80.66 mg/g and 72.64 mg/g, respectively. Due to the strong π-π effect and hydrogen bonding interactions between UiO-66 and CR dyes. UiO-66-NH 2 has stronger hydrophilicity and has electrostatic interactions , Lewis acid-base interactions and hydrogen bonds with CR. The abundant -COOH groups and higher negative Zeta potential (-23.43 mV) in UiO-66-(COOH) 2 led to strong electrostatic interactions and Lewis acid-base interactions with the cationic dyes MB and Rh B. Therefore, the adsorption performance of UiO-66-(COOH) 2 on cationic dyes was improved.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2024
·
IF 3.9
Jingwei Yuan,Wanyin Xu,Yirong Wang,Shao Wang,Ronghui Hao,Yubing Dong,Qianqian Li,Yufeng Zhao
Metal-organic frameworks (MOFs), characterized with highly ordered porous structures and relatively high surface area, exhibit significant application potential in the field of electrochemistry catalysis. In this study, we successfully prepared UiO-66(Ce) particles with uniform nanocube morphology and the size distribution ranging from 90 to 156 nm. Both morphology and size can be precisely tuned by directly adjusting detailed synthesis parameters, including solvent concentration and reaction time. Moreover, the crystal growth mechanism of UiO-66(Ce) was comprehensively investigated through the microstructure characterization. Such uniform particles demonstrated a desirable electrocatalytic performance with hydrogen evolution reaction (HER) overpotential of 118.6 mV (at 10 mA cm −2 ) in alkaline electrolyte (1 M KOH). This study not only introduces a novel approach for the morphological manipulation of UiO-66(Ce), but also presents new material candidates for the advancement of high-performance electrochemical energy conversion systems.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Qiuzheng Du,Pu Wu,Yiyang Sun,Jingyi Zhang,Hua He
A simple and recyclable imprinted catalytic composite (ZnO@NH 2 -UiO-66, ZUM) was synthesized by postsynthetic modification method with tetracycline (TC) as molecular template. A series of ZUM-n composites with different NH 2 -UiO-66 dopants from 0.1 to 0.7 g had been prepared and compared. The characterization results showed that ZUM-1 possessed the advantages of uniform size, high surface area and wide absorption spectrum. Further research results indicated that ZUM-1 composite has the ability of selective adsorption and the higher photocatalytic degradation efficiency to TC without secondary pollution. Under visible light irradiation, the ZUM-1 could degrade 61.9% of TC within 30 min, which may relate to the inhibition effect of composite materials on electron-hole recombination. The degradation selectivity of ZUM-1 was investigated by comparing the degradation efficiency of TC, tetracycline hydrochloride and ciprofloxacin. The high degradation efficiency and selectivity of ZUM-1 were also confirmed in real samples. The stability experiments showed that the ZUM-1 possessed excellent recyclability and stability in the photocatalytic degradation process, and the recycled process was environmentally friendly. The mechanism of TC photodegradation by ZUM-1 was investigated by UV–vis spectra, photoelectrochemical and radical scavenger experiment. And the possible degradation products were analyzed by HPLC-MS. All in all, this method provided a simple and promising perspective for preparing visible-light-responsive molecular imprinting composites with high specificity and photocatalytic activity.
研究领域:
环境科学
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材料科学
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光催化
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 10
·1-12
·
IF 2.4
Huang Qiuyun,Liu Shiyu,Shen Weihua,Fang Yunjin
Due to the modifiable properties and excellent stability, metal-organic frameworks (MOFs) are considered potential catalyst supports in heterogeneous reactions. UiO-66 with varying water contents were synthesized as supports of Pd for the carbonylation of methyl nitrite (MN) to dimethyl carbonate (DMC). In accordance with XRD, NH 3 -TPD, and SEM, the water contents showed a negative correlation on the amounts of acid sites and accelerated crystal aggregation. The Pd/UiO-66(x) demonstrated perfect selectivity of DMC (> 99%) and good CO conversion which were increased with the decrease of water contents. Moreover, the catalysts deactivated at the beginning of the reaction, and the catalytic deactivation was due to the damage of the C = O structure in UiO-66 frameworks. This work revealed the influence of water contents on the synthesis of UiO-66 and the deactivation process of MOF-based catalysts in MN carbonylation to DMC. Graphical
研究领域:
材料化学
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催化化学
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无机化学
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多孔材料
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工业催化
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Guowei Shan,Xiao Xiao,Hong Gao,Qi Zhang,Houyi Peng,Weixing Li
Heavy metal ion (HMI)-contaminated wastewater is a great threat to public health. Membrane separation is an efficient and green technology for HMI removal. Here, the strategy of nanoparticle in-situ growth combined with molecule grafting was proposed to fabricate the UiO-66-NH 2 -g-DTPA/PES composite membrane. The UiO-66-NH 2 nanoparticles bound within the PES membrane substrate uniformly brought a significant number of primary amino groups, providing abundant graft sites for DTPA molecule. Numerous carboxyl groups and tertiary amine groups were introduced as the result of DTPA grafting, enabling the formation of M−DTPA complexes with HMIs. The fabricated UiO-66-NH 2 -g-DTPA/PES membranes exhibited excellent performances. The pure water flux arrived at 6208 L·m −2 ·h −1 and the efficiencies of removing Cu 2+ , Pb 2+ , Cr 3+ and Cd 2+ were 99.73%, 99.79%, 96.91% and 98.33%, respectively. Moreover, the UiO-66-NH 2 -g-DTPA/PES membrane also showed a remarkable stability in pH conditions ranging from 3 to 10 and remained a relatively high performance in the cyclic test.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
INORGANICA CHIMICA ACTA
·
2024
·
IF 2.7
Guang-Li Zhou,Bo-Wen Liu,Guang-Yu Cui,Wei Zhang,Ji-Min Yang
Radioactive iodine waste from the nuclear industry poses a critical threat to human health, and its effective capture has become an important research topic. In this study, modified UiO-66-X adsorbents (where X is ATA, BTA, or STA) were used to investigate the effects of the free functional groups in the UiO-66 skeleton on iodine capture in the vapor and solution states. The adsorption behavior revealed that the capture efficiency of UiO-66-ATA was substantially higher than that of UiO-66-BTA and UiO-66-STA because the electron-donating amino groups could enhance the I − I···π halogen bond interactions compared with the electron-withdrawing carboxyl and sulfonic acid groups. In addition, the pore volume of UiO-66-ATA was significantly higher than those of UiO-66-BTA and UiO-66-STA. In particular, the removal uptakes of UiO-66-ATA were 1108.1 mg/g (vapor phase) and 3601.9 mg/g (aqueous solution). This study is the first to investigate the effects of functional groups on the adsorption uptake of UiO-66 toward iodine. This efficient functional group modification strategy holds significant promise for the development of novel metal–organic framework adsorbents.
研究领域:
材料科学
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环境科学
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核能工程
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DOI
高影响因子
Advanced Composites and Hybrid Materials
·
2021
·Vol. 4
·期 3
·562-573
·
IF 5.693
Cheng Xi Quan,Li Songwei,Bao Hongfei,Yang Xiaobin,Li Zhixing,Zhang Yingjie,Wang Kai,Ma Jun,Ullah Asmat,Shao Lu
The lack of highly permeable and selective separation membranes hampers the application of the energy-efficient membrane separation process for water remediation and CO 2 capture in molecular scale. Nanoparticles have been widely applied for tailoring pore structures and surface properties of the molecular separation membranes, thereby enhancing separation performance. However, limited by non-ideal nanoparticle aggregation, it remains a big challenge to fabricate such membranes on a large scale. Herein, we designed a kind of highly dispersed nanoparticles through grafting poly(sodium-p-styrenesulfonate) (PSS) on metal organic frameworks UiO-66 and deployed them for tailoring structure of polyelectrolyte membrane (PEM) for water remediation and Pebax (PEBA) symmetrical membranes for CO 2 capture, respectively. Because of electrostatic interaction, the PSS-grafted-UiO-66 (UiO-66-PSS) demonstrated nearly 100% dispersion in water and had an average particle size around 200 nm. Most interestingly, the introduction of the UiO-66-PSS finely tailored the affinity between membranes and target molecules, and the molecular structure of both PEM and PEBA membranes, thereby tripling the permeances of the membranes and slightly improving the selectivity of the membranes meanwhile. The PEM/UiO-66-PSS membranes demonstrated pure water permeance as high as 27.3 L m −2 h −1 bar −1 with MgSO 4 rejection above 98.7%. For CO 2 capture, the PEBA/UiO-66-PSS membranes exhibited 414.5 barrer with selectivity about 53.8. Taken together, the highly dispersed UiO-66-PSS shows strong promise in constructing molecular separation membranes with high separation performance for environmental remediation. Graphical abstract The highly dispersed PSS-grafted-UiO-66 finely tailored membrane structures of PEM membranes and the PEBA membranes and enhanced affinity between the target molecules and the aforementioned membranes, thereby tripling membrane permeances and improving the membrane selectivity slightly. The obtained PEM/UiO-66-PSS membranes and PEBA/UiO-66-PSS membranes show strong promise in water remediation and CO 2 capture, respectively.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Fukun Bi,Xiaodong Zhang,Shang Xiang,Yunyun Wang
The effect of Pd loading (0.25, 0.5 and 1.0 wt%) and ZrO 2 support calcined at diverse temperatures (600, 700 and 800 °C) by pyrolysis of UiO-66 was investigated for CO oxidation in this work, respectively. The physicochemical properties of the samples were characterized by various characterization methods. The XRD results exhibited that all ZrO 2 support possessed mixed crystalline phase, the monoclinic ZrO 2 and tetragonal ZrO 2 . And the calcination temperature had a big impact on the composition of ZrO 2 supports. Pyrolysis of UiO-66 at high temperature was favorable for the formation of monoclinic ZrO 2 . Additionally, the introduction of Pd was induced the phase conversion from tetragonal to monoclinic of ZrO 2 . The order of catalytic efficiency was as follows: 0.5Pd/Zr-700 > 0.5Pd/Zr-600 > 0.5Pd/Zr-800. Moreover, 0.5Pd/Zr-700 presented high stability and great reusability. The good catalytic performance of 0.5Pd/Zr-700 was ascribed to the better reduction ability at low temperature and high O ads /O lat and Pd 0 /Pd 2+ on the surface. Importantly, the reaction pathway of CO oxidation over the 0.5Pd/Zr-700 was exposed.
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2019
·Vol. 319
·期 3
·737-748
·
IF 1.186
Feng Sheng,Ni Ziqiu,Feng Shanshan,Zhang Zhihui,Liu Shuguang,Wang Runbai,Hu Jiawei
In this study, the UiO-66/Fe 3 O 4 /GO composite was prepared by one step method for removal of cesium ions (Cs + ) in water and exhibited excellent adsorption capacity for Cs + (62.07 mg g −1 ), which can be attributed to the size compatibility of nanosized cavities and the addition of GO. As supporting matrix, GO decreased particle aggregation and increased the surface area of the adsorbent. The composite had good acid and alkali resistance, thermal stability, rapid adsorption rate and can be separated from water by magnetic separation rapidly.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
MOLECULES
·
2021
·Vol. 26
·期 19
·5736
·
IF 4.412
Chunhua Wang,Zhiquan Yu,Yuhao Yang,Zhichao Sun,Yao Wang,Chuan Shi,Ying-Ya Liu,Anjie Wang,Karen Leus,Pascal Van Der Voort
Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2reduction. The obtained Pd/UiO-66-NO2catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.Keywords:Pd/UiO-66-NO2;furfural;hydrogenative ring-rearrangement;cyclopentanone;double-solvent method
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Membranes
·
2023
·Vol. 13
·期 9
·781
·
IF 4.2
Jiaming Gao,Yongchao Sun,Feifei Kang,Fei Guo,Gaohong He,Hanli Wang,Zhendong Yang,Canghai Ma,Xiaobin Jiang,Wu Xiao
Mixed matrix membranes (MMMs) generally have some fatal defects, such as poor compatibility between the two phases leading to non-selective pores. In this work, PIM-1 was chosen as the polymer matrix, and UiO-66 modified with amidoxime (UiO-66-AO) was used as the filler to prepare the MMMs. In the MMMs, the amino and hydroxyl groups on UO-66-AO form a rich hydrogen bond network with the N and O atoms in the polymer PIM-1 chain to improve the compatibility between the polymer matrix and the filler. In addition, the selective adsorption of CO2by the amidoxime group can promote the transport of CO2in the membrane, which enhances the gas selectivity. The CO2permeability and CO2/N2selectivity of UiO-66-AO@PIM-1 MMMs are increased by 35.2% and 45.2% compared to pure PIM-1 membranes, reaching 7535.5 Barrer and 26.9, surpassing the Robeson Upper Bound (2008) and close to the 2019 Upper Bound. After 38 days of the aging experiment, the CO2permeability is approximately 74% of the original. The results show that the addition of UiO-66-AO has an obvious effect on improving the aging properties of the membrane. The UiO-66-AO@PIM-1 MMMs have a bright prospect for CO2separation in the future.Keywords:amidoxime;UiO-66-AO;mixed matrix membrane;PIM-1;CO2/N2separation
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子