FUEL
·
2018
·
IF 4.908
Xiong-Fei Zhang,Zhongguo Wang,Yi Feng,Yuxia Zhong,Jiaqiang Liao,Yaquan Wang,Jianfeng Yao
Metal organic frameworks (MOFs) have recently emerged as promising candidates for efficient removal of sulfur-containing compounds (SCCs) from liquid fuels. In this study, adsorptive desulfurization (ADS) is performed by adsorbing thiophene (TP) and benzothiophene (BT) from model fuels over pristine and functionalized UiO-66 (Zr). The introduction of amino ( NH 2 ) and carboxylic ( COOH) groups reduces the porosity of UiO-66. However, the adsorption capacities of functionalized UiO-66 improved remarkably. Especially for the adsorbent functionalized with amino moieties (UiO-66-NH 2 ), its maximum adsorption capacities for TP (29.5 mg S/g) and BT (35.7 mg S/g) are 1.7 and 1.8 times to that of bare UiO-66. The superior performance of UiO-66-NH 2 is ascribed to the higher availability of hydrogen-bond donor sites in the surface and the favorable interactions between H atoms of NH 2 and sulfur species. UiO-66-COOH is beneficial for the adsorption of SCCs than that of pristine UiO-66 because of the existence of acid-base interactions. Moreover, the reusability of UiO-66-NH 2 is confirmed by regenerating it via a simple solvent washing.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Ji Wang,Shuqing Zhang,Yiming Han,Lilei Zhang,Qingyin Wang,Gongying Wang,Xiaoming Zhang
PET (poly(ethylene terephthalate)) is one of the most important type of thermoplastic polyesters and widely used in various fields. Titanium-based catalysts are environmentally friendly and have higher catalytic activity than antimony-based catalysts when used in industry. However, titanium-based catalysts are prone to hydrolysis and result in discolored products. UiO-66 (Zr/Ti) with different Ti 4+ contents were successfully synthesized via one-step method. The material was characterized by XRD, SEM, FT-IR, XPS, BET and TG techniques. The results demonstrates that Ti 4+ was integrated into the UiO-66 framework. NH 3 - in situ DRIFTS, pyridine-IR, and NH 3 -TPD were used to explore the acidic properties of the samples, which proved that stable Lewis acidic sites are present in the samples even at 300 °C. The catalytic performance of UiO-66 (Zr/Ti) containing different Ti 4+ was explored under different conditions. At the same time, the scale-up experiment was carried out in a 5 L reactor, and the PET chips obtained had a lower b value. The catalytic reaction mechanism of UiO-66(Zr/Ti) was demonstrated by DFT calculations and the catalytic performance was close to Sb-based catalysts.
研究领域:
材料科学
·
化学工程
·
催化
✓ 已验证
DOI
高影响因子
FUEL
·
2017
·
IF 4.601
Xiaotian Zhang,Pengcheng Huang,Aili Liu,Mingyuan Zhu
Owing to the high prices and other shortcomings associated with the existing methods of complex catalyst preparation, we used the UIO-66(Zr) metal–organic frameworks to directly catalyze the oxidative desulfurization (ODS) reaction. The synthesized UIO-66(Zr) was characterized using nitrogen adsorption–desorption isotherm analysis, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Under optimal reaction conditions, the ODS conversion of dibenzothiophene (DBT) reached 100%. This excellent catalytic activity was attributed to the unsaturated coordination of Zr, which may produce beneficial Lewis acid sites.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 65
·37733-37738
·
IF 3.049
Yanghe Fu,Jieyu Wu,Rongfei Du,Ke Guo,Rui Ma,Fumin Zhang,Weidong Zhu,Maohong Fan
Defect engineering can be a promising approach to improve the photocatalytic performance of metal–organic frameworks (MOFs). Herein, a series of defective NH2-UiO-66(Zr) materials were synthesized via simply controlling the synthesis temperature, with concentrated HCl as the modulator and then these as-prepared samples were used to systematically investigate the effects of their structural defects on photocatalytic CO2 reduction. Remarkably, these MOFs with defects exhibit significantly enhanced activities in photocatalytic CO2 reduction, compared with the material without defects. The defect engineering creates active binding sites and more open frameworks in the MOF, and thus facilitates the photo-induced charge transfer and restrains the recombination of photo-generated charges efficiently. The current work provides an instructive approach to improve the photocatalytic efficiency by taking advantage of the structural defects in MOFs, and could also inspire more work on the design of advanced defective MOFs.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yan Yin,Yueyang Xu,Konglu Guo,Peng Zhang,Yongping Zeng
Adsorptive desulfurization is one of the alternative technologies for the effective removal of sulfides from fuels. Functionalization of metal-organic frameworks (MOFs) with Cu + is extremely desirable for adsorption separation via π-complexation interaction with adsorbed molecules. Here we report that Cu + cation is significant and highly effective for adsorption desulfurization in a new type of Cu + - modified UiO-66(Zr). First, Cu 2+ was introduced via ion-exchange with H + of UiO-66-SO 3 H. Then, Cu + cation was obtained from the reduction of Cu 2+ by using vapor-induced reduction, in which vapors of reducing agents diffuse into the pores of MOFs at a lower temperature. The resulted UiO-66-SO 3 Cu(I)− 0.15 has a better adsorption capacity for thiophene compared to pure UiO-66. In the presence of toluene, the UiO-66-SO 3 Cu(I)− 0.15 also exhibits high adsorption capacity for thiophene. After recycling four times, UiO-66-SO 3 Cu(I)− 0.15 still remains a high adsorption capacity.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Konglu Guo,Yueyang Xu,Yan Yin,Yongping Zeng
Adsorption desulfurization can effectively remove thiophene-containing compounds in fuels. UiO-66 is a potential candidate for adsorption desulfurization due to the excellent chemical stability and resistances to acids and alkali. However, the adsorption capacity is relatively low for the big molecules of sulfide (such as thiophenes) because of the pore size in the microporous structure. We used Zn 4 O(BC) 6 as a template to synthesize a new π-complexation adsorbent (H-UiO-66-SO 3 Cu(I)) via ion-exchange and steam-induced reduction, with hierarchical porous (microporous and mesoporous) structure. The adsorbent was characterized by FT-IR, XRD , SEM , TEM and N 2 adsorption-desorption isotherms. The results show that H-UiO-66-SO 3 Cu(I) has the stable structural properties with the new mesopores . H-UiO-66-SO 3 Cu(I) has a good adsorption performance for thiophene and benzothiophene in the model fuel. The regeneration results show that H-UiO-66-SO 3 Cu(I) can be recycled four times and still has good adsorption performance.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Qingqing Wang,Wei Zhou,Claudia Li,Sibudjing Kawi,Yinhui Li
The application of photocatalysts in environmental field has emerged as a prominent research topic. Nevertheless, the efficiency of photocatalysts is reduced as the recombination of photogenerated chargers significantly, restricting their extensive use in this domain. In the present study, photocatalysts composed of bismuth molybdate/NH 2 -UiO-66(Zr) (Bi 2 MoO 6 /NH 2 -UiO-66(Zr)) featuring Z-scheme heterojunctions were effectively synthesized using a two-step hydrothermal technique. These photocatalysts exhibit remarkable photocatalytic degradation under visible light conditions. Notably, the broad planar configuration of Bi 2 MoO 6 sheets improves the separation of the photogenerated charge carriers. NH 2 -UiO-66(Zr) layered atop Bi 2 MoO 6 sheets enhances the availability of catalytically active sites, reduces charge recombination, and promotes charge transfer through the interface. The kinetic rate constant for Bi 2 MoO 6 /NH 2 -UiO-66(Zr) is around 0.00329 L mg −1 min −1 , indicating the increase of 3.78 and 41.13 times compared with pure Bi 2 MoO 6 and NH 2 -UiO-66(Zr), respectively. The efficiency for photocatalytic degradation of tetracycline using Bi 2 MoO 6 /NH 2 -UiO-66(Zr) reaches 81.72 % under visible light. Importantly, this efficiency exhibits a reduction of 10 % after five recycling cycles, demonstrating notable stability. The photocatalytic mechanism involved in tetracycline degradation was uncovered through trapping experiments and EPR, indicating that it is predominantly facilitated by the active oxidation of ·O 2 - and ·OH. The intermediates of the photocatalytic process as well as the possible degradation pathways were discussed. The creation of Bi 2 MoO 6 sheets/NH 2 -UiO-66(Zr) heterojunction photocatalysts provides a fresh approach to the development of novel catalysts, which may lead to significant advancements in environmental remediation efforts.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiajun Yu,Xiao Wang,Yan Wang,Xiaofeng Xie,Haijiao Xie,Nat Vorayos,Jing Sun
The removal of indoor/outdoor toluene by photocatalysis has drawn much attention due to its low energy consumption and easy availability. However, light inevitably generates heat, and pollutants desorb from catalysts as the temperature rises, which is not beneficial to degradation. Contrast to the frequently occurred phenomena, we firstly found that the adsorption capacity of UiO-66 (Zr) on toluene increased with increasing temperature as adsorption isotherms and in-situ Fourier transform infrared spectra (in-situ FTIR) showed. The optimum temperature was 30 °C. This stage in which adsorption capacity was positively correlated with temperature was called heating-induced adsorption, which achieved a toluene removal efficiency of 69.6 %. By density functional theory (DFT) calculations and changing the metal centers and organic ligands of UiO-66 (Zr) respectively, we disclosed that the heating-induced adsorption was mainly related to the π-π stacking interaction of MOF ligands and toluene. The analysis of samples before and after adsorption showed that the interaction between UiO-66 (Zr) and adsorbed toluene facilitated the charge transfer and prolonged the carrier lifetime, leading to the increase of hydroxyl radicals (•OH) in photocatalysis. Therefore, a synergistic effect between heating-induced adsorption and photocatalysis was proposed by analyzing the adsorption of toluene on UiO-66 (Zr) in detail. This work provided new viewpoint to understand the role of concomitant heat contributed to the adsorption and degradation of toluene during photocatalysis.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jie Yin,Wendi Fu,Jinrui Zhang,Xinyu Liu,Xinmiao Zhang,Chao Wang,Jing He,Wei Jiang,Hongping Li,Huaming Li
Porous ionic liquids are a novel category media that possesses the catalytic activity of porous solids and the extraction property of ionic liquids. Herein, a new type of porous ionic liquids (denoted as UiO-66-T3PILs) was fabricated by employing UiO-66(Zr) as the pore generator and the ionic liquid ([P 6,6,6,14 ][NTF 2 ]) as the size-excluded solvent for extraction coupled catalytic oxidative desulfurization (ECODS) using hydrogen peroxide (H 2 O 2 , 30 wt%) as an oxidant. Furthermore, several significant reaction parameters such as UiO-66 loading in porous ionic liquids, reaction temperatures, molar ratio of H 2 O 2 /DBT and sulfide species as well as recyclability were investigated in detail. As UiO-66-T3PILs exhibited higher efficiency (95.3%) than the summarized efficiency of UiO-66 and [P 6,6,6,14 ][NTF 2 ], there did exist a synergistic effect between the UiO-66(Zr) moiety and the ionic liquid moiety in UiO-66-T3PILs. With the assistance of density functional theory calculations, a possible mechanism was proposed that aromatic sulfur compounds in the oil phase were first extracted into ionic liquids moiety phase via C-H···π interactions and then rapidly oxidized by OH radicals in the presence of the UiO-66 moiety. This work will pave the way for the rational design of novel porous ionic liquids towards catalysis.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2022
·
IF 5.477
Yong Pan,Feng Liu,Yong Zhou,Chen Zhu,Haixia Pang,Baoming Xu
Background Phosphorus in wastewater is a major environmental concern. Very small phosphorus inputs in the environment can cause algal blooms that can deplete the dissolved oxygen and decrease the water quality, leading to eutrophication. Furthermore, some algal blooms produce toxins and bacterial growth that can cause human illness through exposure to contaminated water. Therefore, It is necessary to remove phosphorus before it is discharged to the environment. Methods adsorbent enhanced adsorptive ultrafiltration (UF) has recently emerged as an advanced ion recovery technology with membrane filtration function and adsorption function, and is very effective in removing cationic bisphosphate and anionic phosphate. Significant findings Herein, a novel defect-rich and covalently-crosslinked octanoic acid (OA)-UiO-66(Zr)-NH 2 /PVC adsorption ultrafiltration membrane are designed for removal of phosphate ions in water. The OA-UiO-66-NH 2 /PVC-33 membrane achieved the adsorption capacity (∼30 mgg −1 ) and higher removal efficiency (∼90%). The OA-UiO-66(Zr)-NH 2 /PVC ultrafiltration membrane exhibited a higher water flux of 266.9 L/(m 2 ·h·bar) compared to those of pristine PVC and UiO-66-NH 2 /PVC. Filtration and cyclic stability experiments reveal that OA-UiO-66(Zr)-NH 2 /PVC membrane can maintain a high retention capacity and exhibit excellent regeneration performance after 5 cycles.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 6
·2653-2661
·
IF 3.925
Long Jin,Feng Liu,Jian-hua Wu,San-Jian Ma,Juan-Hong Li,Yong-Jing Tian,Xin Liu,Zi-Xia Lin
A novel improved Fenton system named MHACF-UiO-66(Zr) was constructed under normal temperature and pressure based on the reduction of FeIII accelerated by hydrogen. The regeneration of FeII was enhanced by Pd/UiO-66(Zr). The hydroxyl radical could be continuously generated using only trace level FeII. 10 mg L−1 4-chlorophenol could be thoroughly degraded in the initial conditions of 75 mL min−1 H2, pH 3, 20 mM H2O2, 2 g L−1 Pd/UiO-66(Zr) and 20 μM FeII. Moreover, the removal efficiency of 15 mg L−1 sulfamethazine could be maintained at least more than 94% under the same conditions. The activity of the solid catalyst could be maintained after 6 consecutive reaction cycles. This provides new insight for improving the inherent shortcomings of the Fenton reaction, which generates large amounts of iron sludge.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2013
·Vol. 19
·期 42
·14279-14285
·
IF 5.831
Dengrong Sun,Yanghe Fu,Wenjun Liu,Lin Ye,Dengke Wang,Lin Yang,Xianzhi Fu,Zhaohui Li
Graphical Higher CO 2 photoreduction activity than previously studied metal–organic framework (MOF) NH 2 -MIL-125(Ti) in the presence of triethanolamine (TEOA) as the sacrificial agent under visible light is exhibited by the amino-functionalized MOF NH 2 -Uio-66(Zr). The photoinduced electron transfer from 2-aminoterephthalate linkers to Zr oxo clusters was revealed for the first time by photoluminescence studies, and the generated Zr III was detected by ESR analysis (see figure). Metal–organic framework (MOF) NH 2 -Uio-66(Zr) exhibits photocatalytic activity for CO 2 reduction in the presence of triethanolamine as sacrificial agent under visible-light irradiation. Photoinduced electron transfer from the excited 2-aminoterephthalate (ATA) to Zr oxo clusters in NH 2 -Uio-66(Zr) was for the first time revealed by photoluminescence studies. Generation of Zr III and its involvement in photocatalytic CO 2 reduction was confirmed by ESR analysis. Moreover, NH 2 -Uio-66(Zr) with mixed ATA and 2,5-diaminoterephthalate (DTA) ligands was prepared and shown to exhibit higher performance for photocatalytic CO 2 reduction due to its enhanced light adsorption and increased adsorption of CO 2 . This study provides a better understanding of photocatalytic CO 2 reduction over MOF-based photocatalysts and also demonstrates the great potential of using MOFs as highly stable, molecularly tunable, and recyclable photocatalysts in CO 2 reduction.
研究领域:
材料科学
·
环境科学
✓ 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）