NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 5
·2189-2197
·
IF 3.591
Yangyang Xin,Dechao Wang,Dongdong Yao,Hailong Ning,Xiaoqian Li,Xiaoqian Ju,Yichi Zhang,Zhiyuan Yang,Yahong Xu,Yaping Zheng
Porous liquids (PLs), a new class of materials with permanent pores and macroscopic flowing behaviors, have attracted much attention for CO2 capture. However, the preparation of PLs is always complicated, which is not suitable for the scale-up. Herein, we propose a rather simple and feasible strategy based on post-synthetic modification of pore generators and the like-dissolves-like principle to synthesize UiO-66-PLs with low-viscosity. To be specific, the metal–organic framework (MOF) UiO-66 with hydroxyl groups (denoted UiO-66-OH) was modified by an organosilane (denoted KH550 or SID) via a post-synthetic modification method, obtaining the pore generator UiO-66-OS (denoted UiO-66-KH550 or UiO-66-SID). Then, the UiO-66-OS was dispersed into two different sterically hindered polydimethylsiloxane solvents (PDMS400 or PDMS6000). Thereby, a series of type 3 PLs (UiO-66-PLs) with superior fluidity at room temperature and accessible porosity were obtained. For instance, the viscosities of UiO-66-KH550-PDMS400 and UiO-66-SID-PDMS400 were 1.1 and 1.5 Pa S at 25 °C, respectively, which were far lower than those of values reported thus far. In addition, gas sorption–desorption measurements indicated that the UiO-66-PLs exhibit superior CO2 sorption performance and great potential for CO2/N2 separation. Moreover, molecular simulation was carried out to verify the retained accessible porosity. Notably, the strategy of constructing type 3 PLs based on the post-synthetic modification of MOFs with organosilane and the like-dissolves-like principle not only provides a new solution for the development of low-viscosity PLs, but also opens a new path for the construction of other types of advanced porous material (APM)-based (e.g., covalent organic frameworks (COFs), porous organic cages (POCs)) PLs, which have potential applications in the fields of gas trapping storage, and catalysis.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
Particuology
·
2024
·
IF 4.1
Jingchuan Wang,Junhong Luo,Yong Yao,Jiangfeng Song,Yan Shi
To improve room-temperature hydrogen storage, palladium (Pd) nanoparticles were innovatively decorated by carbon bridge onto the amino-group functioned Zr-terephthalate metal-organic framework (MOF) UiO-66 to reduce the diffusion energy barrier and then improve the hydrogen spillover effect. Powder X-ray diffraction shows broad Pd peak and retained UiO-66-NH 2 integrity after Pd decoration. The hydrogen uptake capacity show that UiO-66-NH 2 -Pd exhibits best hydrogen storage performance than UiO-66-NH 2 and pristine UiO-66. The hydrogen up taken in Pd decorated UiO-66 (UiO-66-NH 2 -1Pd) was close to 4 wt% under 20 MPa at room temperature. Density functional theory (DFT) calculations show that hydrogen adsorption energy of UiO-66-NH 2 -Pd was −0.5897 eV, which was much lower than that of UiO-66-NH 2 (−0.3716 eV) and UiO-66 (−0.2975 eV). Ultimately, Pd decorated NH 2 group functioned UiO-66 enable improve storage capacities through hydrogen spillover under ambient conditions which could satisfy the demand for sustainable energy, especially for the long-term storage energy media.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhijian Xiao,Wenda Yang,Jing Wang,Shuang Cao,Jingling Yang,Mingshan Zhu
Photocatalysis is a promising technology for removing low concentrations of nitric oxide (NO) from the atmosphere. However, the unsatisfactory photocatalytic NO removal efficiency and the high selectivity for NO 2 in catalysts limit the development of this technology. In this work, we used an in-situ synthesis method to incorporate Cs 3 Bi 2 Br 9 into UiO-66 for efficient and robust photocatalytic NO removal. The Cs 3 Bi 2 Br 9 /UiO-66 catalyst exhibits a 77.6 % NO removal efficiency and low NO 2 selectivity under visible light irradiation at a WHSV of 1,650,000 mL h −1 g −1 , exceeding the efficiencies of Cs 3 Bi 2 Br 9 (36.4 %) and UiO-66 (2.3 %), as well as those of most reported MOF-based photocatalysts. The synergy of weak Lewis acid sites from Cs 3 Bi 2 Br 9 in Cs 3 Bi 2 Br 9 /UiO-66 and the strong Lewis acid sites from UiO-66 promotes the enrichment of NO on the catalyst surface and act as electron traps to induce carrier separation, thereby promoting the generation of O 2 − to achieve high efficiency. This work provides a new idea for the development of catalysts in NO elimination.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 26
·11164-11171
·
IF 3.288
Zhuo Wang,Jin Liu,Zhen Li,Xianbiao Wang,Ping Wang,Di Wang,Fengjun Zhang
A crosslinkable UIO-66 type MOF material denoted UIO-66-DETA composed of Zr(IV) metal ions and 2,5-diallyl ether terephthalic acid (DETA) was synthesized, and then by initiating double bond crosslinking, a new crosslinking MOF material denoted UIO-66-DETA-CL was obtained. UIO-66-DETA and UIO-66-DETA-CL were characterized by FTIR spectroscopy, PXRD, 1H solid-state NMR spectroscopy, SEM, nitrogen sorption, thermogravimetric analysis and hydrogen storage tests to analyze their structure and properties. The results showed that a crosslinked structure has been formed, and UIO-66-DETA-CL can maintain its structure below 340 °C, compared with UIO-66-DETA; its carbon residual rate is improved, which shows that the crosslinking modification enhances the thermal stability. Meanwhile, the hydrogen uptake capacity of UIO-66-DETA-CL reaches 5.36 wt% at 77 K and 4 MPa. Furthermore, the hydrogen adsorption enthalpy of UIO-66-DETA-CL (ΔHUIO-66-DETA-CL) calculated using the Arrhenius equation reaches −0.889 kJ mol−1, which is significantly improved by crosslinking modification. The crosslinked structure changes the pore size and increases the active adsorption sites in organic ligands. The framework of UIO-66-DETA-CL can provide more polar charges to cause some hydrogen molecules to be negatively charged because of a small HOMO–LUMO gap, and a lower LUMO energy level of UIO-66-DETA-CL enables stronger negative charge acceptability. Therefore, crosslinking modification enhances the material's hydrogen storage capacity. This result provides a new idea for the crosslinking modification of MOFs.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Yanan Ding,Feng Wei,Changchang Dong,Jiadong Li,Chang Zhang,Xiaojun Han
Heavy metal ion pollution has been a potential threat to human health. Herein, a sensitive electrochemical sensor for simultaneously detection of Cd(II) and Pb(II) was developed using a metal–organic framework material UiO-66. UiO-66 before and after carbonization was used to modify the GCE electrodes, respectively. The carbonized UiO-66 modified GCE electrode (CUiO-66/Bi/GCE) showed good detection ability with the linear detection range of 10–50 μg/L and detection limit of 1.16 and 1.14 μg/L for Cd(II) and Pb(II), respectively. Compared with UiO-66, carbonized UiO-66 provided more active sites for Bi ions and heavy metal ions to co-deposit and facilitated the electron transfer, leading to better detection performance. The decoration strategy was applied to disposable screen-printed carbon electrodes (SPCEs) to obtain the linear detection range of 20–120 μg/L and detection limit of 4.67 and 1.24 μg/L for Cd(II) and Pb(II) respectively. The prepared electrochemical sensors hold great potential in real water sample detections.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
高影响因子
ECS Journal of Solid State Science and Technology
·
2024
·Vol. 13
·期 5
·057004
·
IF 1.8
Yu Ding,Yaru Li,Soufian Chakir,Jun Mei,Xianbiao Wang
Phosphate pollution leads to deterioration in water quality, posing a serious threat to human health. Therefore, it is important to develop a highly selective and sensitive fluorescent probe for phosphate detection. Here, we report a novel ratiometric fluorescent probe, Fluorescein@NH2-UiO-66 (denoted as Flu@NH2-UiO-66), for the trace detection of phosphate in water. Specifically, during the in situ solvothermal synthesis of Flu@NH2-UiO-66, fluorescein molecules were encapsulated into the cavities of the metal-organic framework. Furthermore, the encapsulation amount of fluorescein was controlled by adjusting the acidity of the system. The Flu@NH2-UiO-66 (60 H+) sample, prepared with a 60:1 molar ratio of acetic acid to the metal center exhibited distinct dual fluorescence signal peaks. The probe showed a highly selective fluorescence response to phosphate. Within a range of 0–20 μM phosphate concentration, the probe demonstrated excellent linear detection capability with a detection limit of 0.37 μM. Moreover, the mechanism of fluorescence enhancement can be attributed to the addition of phosphate, which greatly increases the UV absorbance of the probe. This study developed a novel ratiometric fluorescent probe capable of rapid, sensitive, and stable detection of trace phosphate, which is of great significance for environmental management.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2024
·
IF 4.1
Mingtao Wang,Shijie Wang,Zhenzi Li,Xuepeng Wang,Liping Guo,Haixia Liu,Lijun Liao,Wei Zhou
Photocatalysis is an alternative for antibiotics removal from wastewater for the sustainable development of human society. However, applying photocatalysts for antibiotics (e.g., tetracycline) degradation under practical conditions is highly restricted by the low reaction efficiency due to the prompt charge recombination. Constructing porous heterojunctions is an efficient way to regulate the electron transfer path and accelerate charge migration efficiency. Herein, TiO 2 /defective UiO-66 porous octahedral S-scheme heterojunctions are successfully fabricated through an in-situ growth strategy. The strong interaction and charge migration behavior between TiO 2 and defective UiO-66 have been studied using X-ray photoelectron spectroscopy and electron paramagnetic resonance measurements. The photocatalytic removal efficiency of tetracycline is notably improved by forming TiO 2 /defective UiO-66 porous heterojunctions. The promoted photocatalytic performance can be ascribed to the strong interaction between TiO 2 and defective UiO-66, and the accelerated charge separation and transfer efficiency due to the formation of S-scheme heterojunctions, thus generating abundant reactive oxygen species, including O 2 − and OH. The optimized 38-TiO 2 /UiO-66-300 can eliminate 97.9 % of tetracycline in 60 min with a reaction constant rate of 0.0425 min −1 , which is approximately 4 and 10 times that of pristine TiO 2 and UiO-66-300, respectively. This work provides an alternate strategy for preparing highly active heterojunction photocatalysts for environmental applications.
研究领域:
环境科学
·
材料科学
·
光催化技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Lichuan Tan,Peng Wang,Ruowei Lu,Siwen Feng,Guangsong Yuan,Cuijuan Wang
Hollow MOFs nanoreactors with controlled shape, size, pore volume , and shell thickness have been considered as emerging materials for a variety of applications. Selecting environmentally friendly and cheap colloidal carbon (CNs) as the template, bimetallic hollow Ce/Zr-UiO-66 nanoreactors were synthesized. The PXRD , TEM , EDS and other characterization analysis proved that hollow structure was formed, accompanied with incorporating of Ce(III) in UiO-66 and the crystal morphology was good. Furthermore, bimetallic hollow Ce/Zr-UiO-66 was studied as a catalyst to catalyze the conversion of furfural (FF) to furfuryl alcohol (FAL) without exogenous hydrogen. The results showed that the hollow structure and bimetallic UiO-66 was beneficial to the catalytic reaction by modulating the ratio of Ce(III) and Zr(IV). Among then, the 1:4 ratio of Ce(III) and Zr(IV) displayed good catalytic activity, the conversion rate of FF was 95% and selectivity of FAL was 94%. This study opens a new avenue for further rational design and construction of well-performing MOFs nanoreactors.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Songjian Zhao,Dongyao chen,Haomiao Xu,Jian mei,Zan Qu,Ping Liu,Yong Cui,Naiqiang Yan
The zirconium metal-organic framework material UiO-66 was doped with Ag nanoparticles and investigated for the removal of elemental mercury (Hg 0 ) in flue gas . Physical and chemical characterization of the adsorbents showed that adding Ag did not change the crystal structure and morphology of the UiO-66. Ag doping can improve the redox activity of UiO-66, and the adsorbent exhibited high thermal stability and surface area. Hg 0 removal experiments indicated that UiO-66 exhibited the higher performance compared with P25 and activated carbon, and the addition of Ag exhibited a significant synergistic effect with the UiO-66, which had highest Hg 0 adsorption capacity (3.7 mg/g) at 50 °C. Furthermore, the Hg 0 removal mechanism was investigated, revealing that Hg 0 is removed by the formation of an Ag amalgam and channel adsorption at low temperature, and through Ag-activated oxygen oxidation and channel capture at high temperature.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 36
·期 3
·e6559
·
IF 4.105
Liang Chu,Junzhen Guo,Liyan Wang,Huiyang Liu,Jiamin Yan,Lingmei Wu,Mu Yang,Ge Wang
Due to environmental and health concerns, it is very important to develop high activity oxidative desulfurization (ODS) catalyst for petroleum purification. Recently, defect engineering of metal organic frameworks (MOFs) to generate a large number of unsaturated catalytic active sites is a very promising approach. Defective MOF has good research value as ODS catalyst. Here, UIO-66 with lots of defects can be prepared by rapid crystallization using concentrated hydrochloric acid as a modulator. The prepared UIO-66 material has good industrial applicability due to its low synthesis temperature (100°C), short synthesis time (20–30 min), large-scale preparation, and excellent catalytic performance (dibenzothiophene can be entirely removed in 6 min under the optimal catalytic conditions [25-mg catalyst, 60°C, O/S 7.5]). The obtained material exhibits not only extraordinary ODS activity of 37.6 mmol h −1 g −1 but also good cycle stability for the removal of DBT (in 7 cycles without significant loss of activity, greater than 90.2%). And for large space volume 4,6-DMDBT, it also shows excellent catalytic performance. The ODS mechanism of defect UIO-66 for DBT is explored, and it proves that hydroxyl radicals and superoxide radicals are generated and play a critical role in ODS reaction. The excellent catalytic performance of defect UIO-66 gives mainly the credit to the abundant defect sites, large specific surface area, and pore volume.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 7
·1487
·
IF 4.6
Senliang Xi,Dawei Xu,Renzeng Chen,Wenhao Yao,Wenying Wu,Teng Zhang,Liang Yu
Ammonia borane (AB) has attracted much attention in the field of solid-state hydrogen storage due to its high hydrogen storage capacity. Nanoconfinement in UiO-66 can reduce the hydrogen release temperature. In particular, terephthalic acid was used as a linker to further improve the dehydrogenation properties through the modification of -NH2, -OH, -NO2, -Br, and -F groups. The hydrogen release content of 0.5AB/UiO-66 was 1.98 wt.%, whereas the hydrogen release content of UiO-66-2OH modified by -OH groups increased to 3.85 wt.%. The non-covalent interaction results show that -NH2and -OH preferred adsorption with -BH3, and the H in -NH2and -OH were able to interact directly with the H in AB to modify the dehydrogenation process of AB, whereas -NO2, -Br, and -F indirectly affected the charge density of hydrogen atoms in AB to alter the dehydrogenation property of AB. The modification of functional groups provides a theoretical basis for the design of high-performance MOF nanoconfinement AB composite hydrogen storage materials.
研究领域:
材料科学
·
氢能存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2024
·
IF 3.5
Zhengyan Wang,Chenhao Yuan,Dong Yang,Mifen Cui,Jihai Tang,Zhuxiu Zhang,Xu Qiao
It is of great significance to develop catalysts for the degradation of hexachlorobenzene from the industrial thermal process. In this paper, formic acid was used as a modulator to generate defect sites in Ce/Zr-UiO-66 with intrinsic Brønsted acidity. The defective formate ligands were removed through methanol–water vapor treatment to expose additional open metal sites with Lewis acidity. The intrinsic Brønsted acid sites of the resulting Ce/Zr-UiO-66-FA-P achieved a hexachlorobenzene degradation efficiency of 99.5% at 250 °C. The generated Lewis acid sites facilitated the C–C cleavage of degradation intermediates. More than 95.0% of the final products were CO2/CO, coupled with chlorinated alkanes/alkenes, which outperformed other benchmark metal oxide catalysts. The Ce/Zr-UiO-66-FA-P catalyst maintained its catalytic activity in the model industrial flue gas and humid environment. The degradation pathway of hexachlorobenzene was tracked using in situ FT-IR spectra.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）