CATALYSIS TODAY
·
2020
·
IF 5.825
Yulong Gu,Wei Xu,Yinyong Sun
The development of active oxidative desulfurization (ODS) catalysts is of practical importance. Recently, MOF-808(Zr) has been attempted to use as ODS catalyst due to its various advantages. However, generally MOF-808(Zr) prepared by conventional method was less active in the oxidation reactions due to the lack of defect sites in the structure. In this contribution, we report that the catalytic oxidative performance of MOF-808(Zr) can be enhanced by acid treatment due to the formation of defect sites resulting from the partial removal of organic linkers in the structure. During the experiment, the effect of acid concentration, treatment time, the addition amount of oxidant and reaction parameters on the performance of MOF-808(Zr) was studied. The catalytic results show that MOF-808(Zr) treated with 0.4 M HCl for 1h can catalyze the oxidation of dibenzothiophene completely at 60°C in 15 min. The activity (mole number of converted DBT per hour per unit mass) is 70 mmol h −1 g −1 , which is much higher than that (45 mmol h −1 g −1 ) of parent MOF-808(Zr). In addition, the catalyst can be reused several times without obvious loss of catalytic performance.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 36
·期 3
·e6556
·
IF 4.105
Wen-Jing Qiu,Ming-Wu Gao,Qi Chen,Ao Zheng,Yi-Jia Shi,Xin Liu,Juan-Hong Li,Guo-Liang Dai,Yang Hu,Zi-Xia Lin
Under normal temperature and pressure, a novel improved Fenton system that was named MHACF-MOF-808(Zr) was constructed after the introduction of Pd/MOF-808(Zr) and H 2 to solve the inherent problem of the production of iron sludge in the classic Fenton system. Only trace amount of Fe II was required during the whole reaction because Fe III could be rapidly reduced by the active hydrogen derived from the adsorption and activation of H 2 on the surface of Pd/MOF-808(Zr) composite. The concentration of Fe II could be maintained more than 10 μM. The removal of target pollutant sulfamethazine in this system was mainly relied on the degradation of ·OH verified by both of the direct detection and indirect inhibition (using methanol). By using the calculation of Laplacian bond order, the degradation pathway of sulfamethazine followed by the cleavage of N S bond. This prediction was verified by the detection of intermediate products. Only 21% sulfamethazine could be degraded after 3-h reaction in the classic Fenton reaction system, while it could be thoroughly degraded in 1.5 h in the MHACF-MOF-808(Zr) system. The influence of main parameters on the degradation effect of sulfamethazine, such as initial pH, the flow of H 2 , dosage of Pd/MOF-808(Zr), concentration of sulfamethazine, ferrous, and hydrogen peroxide, were systematically studied. Based on the relative stability of Pd/MOF-808(Zr) confirmed by the morphological characterization, sulfamethazine could be efficiently degraded in the MHACF-MOF-808(Zr) system.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Jincheng Mu,Jianfang Liu,Zhenzhen Ran,Muhammad Arif,Min Gao,Chen Wang,Shengfu Ji
MOF-808(Zr) with the coordinated unsaturated (CUS) Zr4+ centers was synthesized by the thermal reflux method, and a series of Au/MOF-808(Zr) catalysts with different Au loading percentages have been prepared by the impregnation–reduction method. The related X-ray diffraction, Fourier transform infrared spectroscopy, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption, Inductively coupled plasma-mass spectrometry, and NH3 temperature-programmed desorption characterizations have been undertaken to understand the structure of catalysts. The catalytic activity in CO2 with aniline/H2 to N-methylation and N-formylation has been studied in a batch reactor. Results show that the MOF-808(Zr) structures in catalysts are of high quality and damage-free. The Au nanoparticles (NPs) are highly dispersed on the surface of the MOF-808(Zr) cage with a mean size of 2–20 nm. Also, the catalysts could catalyze the conversion of CO2 with aniline/H2 to N-methylation and N-formylation products with a high efficiency. With a 3.0 wt % Au/MOF-808(Zr) catalyst, the conversion of aniline is 18.4%, and the selectivity of N-methylaniline is 80.9% and that of N,N-dimethylaniline is 19.1%. The preliminary reaction mechanism and the critical role of CUS were also studied. It is determined that H2 is adsorbed and activated on Au NPs. CO2 is adsorbed on the CUS Zr4+ acidic sites and O2– basic sites. The primary and secondary amines are adsorbed on the CUS Zr4+ acidic sites, where they react with CO2 and H2 to form N-formamide. Subsequently, N-formamide reacts with activated H2 to yield N-methylamine.
研究领域:
催化
·
材料科学
·
化学工程
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Yang Hu,Hai-Liang Yang,San-Jian Ma,Juan-Hong Li,Xin Liu,Yong-Jing Tian,Long Jin,Zi-Xia Lin
The promotion of Fenton process in organic wastewater treatment has been hindered by the disposal of large amounts of iron sludge derived from the excess addition of ferrous salt. The operation of the Fenton reaction could be maintained using trace level Fe II through the effective acceleration reaction of active hydrogen. However, the H 2 which is the precursor of active hydrogen is insoluble in water. Herein, the composite catalyst Pd/MOF-808(Zr) was introduced into the H 2 -Fenton system to enhance the adsorption and activation of this reducing gas. In this novel improved Fenton system called MHACF-MOF-808(Zr), the hydroxyl radical would be unceasingly produced based on the unceasingly recycling of FeII/FeIII at normal temperature and pressure. 15 mg L −1 sulfamethazine could be thoroughly degraded during 2 h reaction process in the initial condition of 60 mL min −1 H 2 , 20 μmol L −1 Fe II , pH 3, 20 mmol L −1 H 2 O 2 and 2 g L −1 Pd/MOF-808(Zr). And so did 10 mg L −1 2,4-Dichlorophenol. The activity and stability of Pd/MOF-808(Zr) could be maintained after at least 6 consecutive reaction cycles. It provides new insight for improving the inherent shortcoming of the Fenton reaction which will generate large amounts of iron sludge.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Guangqin Shi,Ting He,Haian Li,Zhao Yang,Wu Lei,Mingzhu Xia,Yu Tao
In a water solution and with a low reaction temperature of 85 °C, the green preparation of lanthanum-modulated MOF-808 (Zr) was realized, the obtained La-MOF-808 have smaller grain size, larger specific surface area, higher pore volume and larger average pore diameter. When the molar ratio of La: Zr=1:1, 1L-MOF-808 had the best fluoride ion removal performance, and its maximum adsorption capacity for F - reached 101.4 mg/g, which was higher than that of the unmodulated MOF-808 and some other reported fluorine adsorbents. Meanwhile, the regeneration experiment demonstrated that even after five cycles, 1L-MOF-808 retained 73.8 % of its initial adsorption capacity, highlighting its commendable reusability. In addition, when 1L-MOF-808 was applied to actual fluorine-containing wastewater, with the fluoride ion concentration of 25.3 mg/L and an adsorbent dosage of 0.6 g/L, 1L-MOF-808 exhibited excellent resistance to anionic interference (SO 4 2- , Cl - ), the concentration of fluoride ions in effluent was lower than 10 mg/L, meeting the stipulations of fluoride ion discharge outlined in GB39371–2020. Further adsorption mechanism investigation revealed that 1L-MOF-808's affinity for F - was attributed to electrostatic interaction and ligand exchange. Overall, the as-synthesized 1L-MOF-808 not only presents an environmentally friendly approach to producing MOF materials without organic solvents but also develops a new strategy for the design of high-performance adsorbent for effectively removing fluoride ions from wastewater.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Honghao Su,Jingwei Hou,Junyong Zhu,Yatao Zhang,Bart Van der Bruggen
Zr IV -based metal–organic frameworks (MOFs) featuring distinguished water stability, large surface area, and intriguing functionalities have immense potential for practical usage. However, conventional MOF synthesis approaches generally require high reaction temperatures and organic solvents to initiate and template the nucleation and growth, hindering sustainable and cost-effective manufacturing and application of Zr-based MOFs. In this study, a scalable, room-temperature and aqueous synthesis of MOF-808—a Zr-MOF extensively explored as an adsorbent in both academic and industrial sectors—was reported. A rational use of water/formic acid (FA) as a green co-solvent enabled the formation of Zr 6 -cluster in an aqueous phase, thereby facilitating subsequent coordination with H 3 BTC to yield well-crystallized MOF-808. The effects of the water/FA volume ratio, the total solvent volume, and reaction time on the physicochemical properties of MOF-808 were studied. The optimized synthesis conditions (FA/water = 2.7:8.1, and reaction time = 24 h) resulted in the synthesis of MOF-808 with good hydrophilicity, excellent stability, high surface area, and weak positive charges. Moreover, this synthesis approach was successfully upscaled, yielding 11.5 g of MOF-808 at a magnification factor of 48. Notably, MOF-808-V 10.8 exhibited an impressive adsorption capacity for Congo Red (ca. 1500 mg/g) and demonstrated selective fractionation of dye mixtures, suggesting their potential application in dye wastewater treatment. This methodology is expected to provide guidance for aqueous and scalable fabrication of Zr-MOFs towards water-related environmental applications.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 32
·15405-15413
·
IF 3.925
Yuzhu Zhai,Yijing Li,Qin Hou,Yuanhong Zhang,Enlong Zhou,Houshen Li,Shiyun Ai
A phosphate ion (Pi) is usually considered as an important index of eutrophication in water and can cause great harm to the water ecological environment. In this work, MOF-808(Zr/Ce) was synthesized simply for phosphate detection and removal. MOF-808(Zr/Ce) with oxidase-like activity can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB). The colorimetric sensing of phosphate was performed based on the enhancement of the oxidase-like activity of MOF-808(Zr/Ce). The linear detection range for phosphate detection was 11–581 μM, and the detection limit (LOD) was 3.7 μM. The MOF-808(Zr/Ce)/CNF (cellulose nanofibers) flexible film synthesized by the filtration method also enables the rapid identification of phosphate. Besides, the phosphate adsorption performance of MOF-808(Zr/Ce) was also investigated. The adsorption capacities are 54.9, 65.1, and 68.5 mg g−1 at 298, 308, and 318 K, respectively. The results show that MOF-808(Zr/Ce) has great potential for phosphate detection and removal.
✓ 已验证
DOI
高影响因子
npj Science of Food
·
2025
·Vol. 9
·期 1
·1-8
·
IF 7.8
Pan Hui,Zhang Wei,Jin Meng,Zhang Fang,Chen Xuelei,Meng Xiao,Shao Hua,Song Liqun,Zhang Zhihu,Wang Cuijuan
Concerns over health risks associated with mixed pesticide residues have led to a demand for rapid analytical methods. We present a portable surface-enhanced Raman spectroscopy (SERS) device specifically designed for real-time monitoring of indoxacarb (INDX) and chlorfenapyr (CFP) in vegetable juice. This point-of-use sensor integrates silver nanoparticles with a metal-organic framework (Ag/MOF-808(Zr)) and employs a 19-well quartz plate alongside a portable Raman spectroscopy instrument, facilitating simultaneous adsorption, separation, and detection. Detection limits for INDX and CFP in ginger and spinach juices were 0.26–0.76 ppb. Notably, results closely matched those from liquid chromatography, and in-situ detection was achieved within 2 min without pre-treatment, significantly enhancing efficiency over conventional chromatographic methods. This innovative approach demonstrates substantial potential for detecting pesticide mixtures in non-laboratory settings, presenting a valuable option for point-of-use applications.
研究领域:
分析化学
·
食品安全
·
环境监测
·
纳米技术
·
光谱学
✓ 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）