SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiale Lu,Amin Jv,Hongyu Zhao,Guangbo Che,Bo Feng,Yufei Zhang,Chunbo Liu,Renquan Guan
MIL-101(Cr) is an ideal material for wastewater treatment due to its large specific surface area, excellent water stability, and chemical stability. However, its limited light absorption capacity hinders its application. We loaded ferrocene carboxylic acid (Fc-COOH) onto MIL-101(Cr) by a post-synthetic modification method, which resulted in the MOF possessing excellent optical properties while maintaining its original skeleton structure. The MIL-101(Cr)/Fc-COOH (1:2), (abbreviated as CFCC-2) exhibited the best performance, achieving a removal rate of 96% for tetracycline (TC) in just 30 min. This removal rate is significantly higher compared to MIL-101(Cr) and Fc-COOH, which achieved removal rates of only 15% and 21%, respectively. We propose a possible Z-type heterojunction mechanism between MIL-101(Cr) and Fc-COOH to explain the excellent photocatalytic performance of CFCC-2. The intermediates in TC were identified using LC-MS, and the toxicity of these intermediates was predicted and evaluated through the Toxicity Estimation Software Tool (T.E.S.T.). This study provides new insights into the design and fabrication of MIL-101(Cr)-based catalysts as photodegrading organic pollutants.
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Materials Today Communications
·
2025
·
IF 4.5
Lifeng Chi,Xiutong Wang,Siyao Guo,Meipeng Ren,Hua Guo,Mingchun Wang,Youbo Nan,Jinguo Wang
Photocathodic protection has obtained enormous attention in the field of metal corrosion control as an efficient and eco-friendly technology. Developing the photoelectrode with good photoelectrochemical properties is a prerequisite for achieving satisfactory photocathodic protection performance. Here, the NH 2 -MIL-101(Cr)/TiO 2 heterostructures are prepared. Meanwhile, the organic linkers and metal ions from NH 2 -MIL-101(Cr) are used to synthesize the N- and Cr-doped TiO 2 anodes, respectively. The UV–vis DRS, photoluminescence spectra and photoelectrochemical tests conducted under visible light demonstrate the enhanced light absorption, suppressed photoinduced charge carrier recombination, and accelerated separation and transfer rates of photoinduced electron-hole pairs in the TiO 2 composites. The 304 stainless steel connected with NH 2 -MIL-101(Cr)/TiO 2 heterostructures shows the most negative potential (about −0.72 V vs. SCE) and satisfied stability in a 3.5 wt% NaCl solution. The result can be explained by the significantly enhanced optical and photoelectrochemical properties and the strong electric field intensity in the composite heterojunctions. Besides, it has been observed that the NH 2 -MIL-101(Cr)/TiO 2 heterostructures exhibit the best photocathodic protection performance than Cr and N-doped TiO 2 anodes. This research broadens the application scope of MOFs in corrosion resistance and helps to assess the effect of heterostructure construction and element doping on TiO 2 .
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Materials Today Communications
·
2024
·
IF 3.7
Chunlong Qiu,Haiyang Sun,Yeyang Ni,Zhenjiang Dou,Ming Xia,Zhaoyang Fei,Zhuxiu Zhang,Mifen Cui,Qing Liu,Xu Qiao
The impressive water stability demonstrated by MIL-101(Cr) highlights its considerable potential for the effective elimination of organic contaminants from wastewater. Nevertheless, the limited availability of adsorption sites within MOFs leads to an unsatisfactory capacity for tetracycline (TC) adsorption. In this case, the lanthanum modified MIL-101(Cr) porous adsorbents, termed as nLa-MIL-101(Cr), were successfully synthesized using a post-synthetic modification method. Through various characterization analyses, it was confirmed that lanthanum exists in the form of La(OH) 3 within the adsorbents, and all adsorbents also preserved the original structure as MIL-101(Cr). The results of static adsorption experiments demonstrated that, compared to the original material, the adsorption capacity of 1La-MIL-101(Cr) for TC increased by 3.5 times. Further experiments demonstrated that the adsorbent exhibits remarkable ion interference resistance and cycle stability. Finally, based on X-ray photoelectron spectroscopy, the adsorption mechanism was primarily attributed to the coordination between TC molecules and metals active site, while electrostatic interactions also played a significant role in the process. This study has developed a highly efficient adsorbent for the treatment of TC-contaminated wastewater, which reflects promising practical application prospects.
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CHEMICAL ENGINEERING SCIENCE
·
2014
·
IF 2.613
Shengnan Yu,Fusheng Pan,Sen Yang,He Ding,Zhongyi Jiang,Baoyi Wang,Zhuoxin Li,Xingzhong Cao
Hybrid membranes were fabricated with active layers composed of polydimethyl siloxane (PDMS) and metal organic framework MIL-101 (Cr), together with support layers composed of polyvinylidene fluoride (PVDF). Transmission electron microscopy (TEM), X-ray diffraction (XRD) and nitrogen adsorption were used to study the structure of MIL-101 (Cr) particles; scanning electron microscopy (SEM), infrared spectrum (IR), thermogravimetric analysis (TGA), thermomechanical analysis and positron anihilation lifetime spectroscopy (PALS) were employed to characterize the structural morphology, free volume property, thermal and mechanical features of the membranes. The effect of MIL-101 (Cr) incorporation on swelling and pervaporation performance of the hybrid membranes were evaluated with thiophene and n -octane mixture as model gasoline. The packing of PDMS chains was interrupted by MIL-101 (Cr), thus the fractional free volume was increased. Accordingly, the separation performance including permeation flux and selectivity was increased remarkably. The optimal performance was achieved when the weight fraction of MIL-101 to PDMS was 6% with a flux of 5.2 kg·m −2 h −1 (increased by 136% compared with the PDMS control membrane) and an enrichment factor of 5.6 (increased by 38% compared with the PDMS control membrane).
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2023
·Vol. 49
·期 9
·3825-3846
·
IF 3.3
Liu Suyan,Qi Xiaoran,Fan Zhanpeng,Song Jianzheng,Huo Quan
A series of NCDs-decorated hematite@MIL-101(Cr) (marked as HMC) hybrids were innovatively and successfully developed for the highly efficient removal of carbamazepine in this study, which were analyzed by X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, N 2 adsorption–desorption, X-ray photoelectron spectroscopy, etc. And, the successful preparation of the hybrid was directly proved by XRD, FT-IR, SEM, TEM and XPS. N 2 adsorption–desorption result revealed good textural properties of the hybrid. The evaluation results indicated that the as-prepared hybrids possessed markedly promoted removal performances for CBZ. Compared with other hybrids, 0.3HMC2 with introducing FeCl 3 ·6H 2 O (0.3 g) and NCDs (2 mL) presented an optimum adsorption–photocatalysis coupling effects. The photodegradation efficiency over the hybrid was able to reach 100% within 60 min under visible-light irradiation. The excellent performances should be ascribed to good textural properties, π – π interaction formation, fast electron separation nature of NCDs and internal Z-scheme construction between hematite and MIL-101(Cr) phases. Meanwhile, the hybrid 0.3HMC2 showed good stability and reusability for photocatalytic degradation of CBZ. Furthermore, a possible mechanism for the removal of CBZ was also proposed to illustrate the photodegradation process. It is thus clear that the hybrid HMC is a promising catalyst for the removal of CBZ in wastewater.
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Nanoscience and Nanotechnology Letters
·
2019
·Vol. 11
·期 2
·229-233
·
IF 0
Zhao Tian,Yu Jun,He Ziyu,He Nongyue,Dong Ming,Chen Zhu,Chen Hong
The well investigated chromium-benzenedicarboxylate metal-organic framework (MOF), nano-sized MIL-101(Cr), was synthesized in this study by using tetramethylammonium hydroxide (TMAOH) or acetic acid (HAc) as modulator. The addition of TMAOH/HAc played a crucial role on particle size
and morphology of MIL-101(Cr). The obtained MIL-101(Cr) had average diameter of about ∼90 nm in selected condition, and possessed relatively high porosity (the BET surface area can up to 3500 m2/g). Furthermore, compared to bulk phase MIL-101(Cr), the nano-MIL-101(Cr) presented
significant improvement of catalytic activity in oxidation of indene.
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DOI
Inorganics
·
2022
·Vol. 10
·期 3
·33
·
IF 3.149
Tian Zhao,Hexin Zhu,Ming Dong,Minmin Zou,Songfan Tang,Mingliang Luo,Xianggang Li
The chromium-benzenedicarboxylate metal–organic framework (MOF), MIL-101(Cr), is one of the most well-investigated and widely used prototypical MOFs. Regarding its synthesis, the use of a toxic modulator (usually HF) and high reaction temperature (220 °C) are the main factors hindering its further expansion of production and utilization. In fact, high quality MIL-101(Cr) crystals can be prepared at a much lower temperature (160 °C) with spherical morphology via an additive-free approach. Compared to traditional octahedral MIL-101(Cr), the spherical MIL-101(Cr) possesses higher adsorption performance toward dye molecules, including methyl orange (MO) and rhodamine B (RB). The results suggest that toxic additives and high reaction temperatures are not essential in the synthesis of MIL-101(Cr), and the fabrication of spherical MIL-101(Cr) may offer a facile and effective pathway for the large-scale industrial application of MIL-101(Cr).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Senda Su,Xiaoman Li,Xu Zhang,Jingting Zhu,Guodong Liu,Mengyao Tan,Yingying Wang,Min Luo
The incorporation of polyoxometalates (POMs) in metal-organic frameworks (MOFs) with host-guest structure have proven to be effective strategy to rational design of heterogeneous catalysis. In this study, the Keggin-type POM@MIL-101(Cr) composite catalysts (PMo 12 , PW 12 and SiW 12 ) are synthesized for nitrogen fixation reaction without sacrificial agents at room temperature in the first time. The SiW 12 molecules are encapsulated in smaller cavities of MIL-101(Cr) by solvothermal method and in larger cavities by impregnation method, respectively. Solvothermal synthesized catalyst has a performance of 75.56 μmol·h −1 ·g -1 cat and TOF value of 1.95 h −1 , which are about 10 and 88 times than that of Na 4 SiW 12 O 40 . The excellent performance is ascribed to the synergistic effect of SiW 12 and MIL-101(Cr). The MIL-101(Cr) adsorbs a large amount of N 2 and generates sufficiently photogenerated electrons under sunlight irradiation, and electrons quickly transfer to the SiW 12 through hydrogen bonds. Moreover, the agglomeration effect of the homogeneous catalyst SiW 12 is weakened due to encapsulation with more exposed active sites. This work provides a feasible route to design and synthesize nanocomposite materials with exceptional performance for photocatalytic nitrogen fixation.
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PubMed
高影响因子
ChemPlusChem
·
2026
·Vol. 91
·期 8
·e70223
·
IF 3.1
Huan V Doan,Huong T T Tran,Duyen T Le,Xuan N Pham
In this study, a novel Ni–MoO 3 @MIL‐101(Cr) composite catalyst was synthesized via a one‐step hydrothermal method for the oxidative desulfurization (ODS) of dibenzothiophene (DBT). The catalyst combines the high specific surface area of MIL‐101(Cr) with the redox properties of Ni–MoO 3 , providing an effective synergy between adsorption and catalytic oxidation. The incorporation of Ni as a promoter significantly enhances catalytic activity, enabling complete sulfur removal (∼100%) under mild conditions (50 °C) within 60 min. Structural characterizations (scanning electron microscopy, X‐ray diffraction, and SAED) reveal that the catalyst retains its nanosheet–nanorod morphology and crystalline MoO 3 phase after repeated use, with only a slight decrease in the crystallinity of the MIL‐101(Cr) framework. Mechanistic analyses using X‐ray photoelectron spectroscopy, Raman, and temperature‐programmed reduction demonstrate that surface oxygen vacancies and Lewis acid sites promote ODS activity, while highly dispersed Ni–MoO 3 species facilitate H 2 O 2 activation and Mo 6+ /Mo 5+ redox cycling, leading to efficient generation of reactive oxygen species. The catalyst also exhibits excellent stability, maintaining 98.7% DBT conversion after five cycles. These results demonstrate that the strong Ni–Mo synergistic effect and efficient oxygen activation make Ni–MoO 3 @MIL‐101(Cr) a robust and highly efficient catalyst for deep fuel desulfurization. This study presents a significant advancement in the field of oxidative desulfurization by developing a synergistic Ni–MoO 3 redox catalytic system confined within the porous MIL‐101(Cr) framework. Unlike conventional catalysts, the designed material effectively enhances H 2 O 2 activation through cooperative interactions between Ni and Mo species, enabling rapid and ultra‐deep removal of refractory sulfur compounds under mild conditions. The integration of redox‐active sites with a high‐surface‐area MOF support not only improves catalytic efficiency but also ensures excellent stability and recyclability. This work provides new insights into the rational design of bimetallic catalysts for green fuel purification and offers a promising strategy for achieving sustainable and energy‐efficient desulfurization processes.
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PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2026
·
IF 4.5
Yan Jin,Hui Zhang,Tengfei Li,Shaojie Lei,Meier Jiaerheng,Dezhang Ren,Zhibao Huo
Biodiesel has emerged as a promising alternative to conventional diesel due to its renewability and environmental friendliness. In this study, a MIL-101(Cr) featuring synergistic acid sites was developed through a combined defect engineering and post-sulfonation strategy, enabling efficient esterification of oleic acid under mild conditions. Defects were introduced in the MIL-101(Cr) through a mixed-ligand approach. The existence of abundant oxygen vacancies in the defect-engineered MIL-101(Cr) was confirmed by electron paramagnetic resonance (EPR), which could provide adequate grafting sites for the subsequent sulfonation. The sulfonic acid-functionalized MIL-101(Cr) catalyst (MRBSX) was then synthesized by post-sulfonation with chlorosulfonic acid as the sulfonation agent. The chemical structure and sulfonic acid density of MRBSX were systematically investigated by X-ray diffraction (XRD), scanning electron microscope (SEM), brunauer-emmett-teller (BET), and Fourier-transform infrared spectra (FT-IR), and other characterization techniques. Acid-base titration combined with elemental analysis (EA) demonstrated the successful loading of sulfonic acid groups in MRBSX, highlighting the promotional role of oxygen vacancies in enhancing acid site density and catalytic efficiency. Under optimized reaction conditions (100 °C, 6 wt%, 3 h, and M/O = 8:1), the MRBSX with 10 mol% benzoic acid achieved a high oleic acid conversion of 96.7 % and a corresponding biodiesel yield of 91.5 %. Therefore, the proposed synergistic strategy of defect engineering and post-sulfonation is effective in constructing high-performance solid acid catalysts, demonstrating promising potential in green energy conversion applications.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zejun Cao,Ruixi Xiao,Yuxia Chen,Jiangtao Dong,Xuezhong Du
The widespread global use of paraquat (PQ) is attributed to its high herbicidal efficacy and low cost, however, the unresolved issue of its fatal toxicity to humans after ingestion remains a major challenge. The nanocarriers MIL-101(Cr)@MoS 2 @Fe 3 O 4 (MMF) are synthesized to load PQ through the strong π–p electron coupling between the delocalized π electrons of PQ and the localized p electrons of S atoms of MoS 2 at the interface, and then encapsulated with chitosan to construct magnetically recyclable PQ nanoherbicides with excellent stability and biosafety. The release of PQ from the nanoherbicides in simulated human gastrointestinal environments is inhibited (“PASS0” logic gate) from the source, thereby enhancing user safety. Under natural sunlight conditions, the near-infrared photothermal effect of MMF weakens the strong interfacial π–p electron coupling between PQ and MMF, resulting in the release of PQ (“YES” logic gate). The PQ nanoherbicides maintain the herbicidal efficacy of bare PQ in practical applications. The residual nanoherbicides can be easily recovered using magnets, with the collection ratios of 97.8 % and 91.1 % in water and soil, respectively, at a magnetic field strength of 0.5 T. Seed dressing, cytotoxicity, and mouse models demonstrate that the nanoherbicides have excellent biosafety for both plant growth and PQ-ingesting users. The creative PQ nanoherbicides simultaneously address the challenging issues of user safety, herbicidal efficacy, and environmental friendliness from the source.
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高影响因子
CHEMICAL ENGINEERING COMMUNICATIONS
·
2025
·
IF 2
Fan Pan,Lijiang Tian,Fulong Chen,Jie Zhang
The photocatalytic efficiency of titanium dioxide(TiO2) is easy to restrict by rapid recombination of carriers, narrow spectrum response range, and low specific surface area. Constructing heterojunctions has been widely acknowledged as a viable strategy to enhance the photocatalytic performance of TiO2. Here, TiO2@MIL-101(Cr) heterojunction was synthesized via the in-situ method and applied to adsorbing and photocatalytic degrading of gaseous benzene. The findings demonstrate 40TM exhibited the best adsorption(1157.03 μgC6H6/(g·h)) and photocatalytic(817.80 μgC6H6/(g·h)) performance, which were 2.05 and 5.21 times of TiO2, respectively. The enhancement of adsorption performance probably resulted from the higher specific surface area(637.33 m2/g) and the micro-mesoporous structure. The excellent photocatalytic performance might stem from the extended wavelength response range(400–700 nm) and the Z-scheme heterojunction formation. The possible mechanism is that electrons in MIL-101(Cr) and holes in TiO2 could participate in redox reactions to generate radicals, with superoxide radicals(∙O2−) and hydroxyl radicals(∙OH) being identified as the primary active species for benzene degradation. Overall, this investigation offers a valuable reference for the application of heterojunction catalysts in the field of adsorption-photocatalytic degradation of volatile organic compounds (VOCs).
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