CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Min Zhang,Jieshu Zhou,Xiulan Guo,Xiangke Zeng,Lan Shi,Tingting Zhang,Yunfei He,Xintao Zhou,Shaoyun Shan,Kaili Yao
Mitigating the rise of atmospheric carbon dioxide (CO 2 ) levels presents one of humanity’s significant challenges. Metal-organic frameworks (MOFs) have emerged as promising materials for CO 2 capture, owing to their unique chemical structure and operability. Many researchers have demonstrated that amination treatment can further enhance CO 2 adsorption performance. However, the relatively low capture efficiency and limited cycling stability of these materials continue to impede their development. Alkali metal cations exhibit high CO 2 adsorption capacities and can be incorporated into the MOF structure to significantly enhance CO 2 capture capacity and cycling stability. Therefore, we synthesized novel alkali metal ion-doped M−NH 2 −MIL−101 (M = Li, Na, K) adsorbents using a post-modification method, successfully anchoring alkali metal cations to carboxylate group sites within the MOFs framework. The integration of microscopy, spectroscopy, and density functional theory (DFT) calculations has confirmed that the introduction of alkali-metal cations enhances the adsorption between MOFs and CO 2 , thereby providing stronger adsorption sites. Experimental studies have demonstrated that doping with 0.1 M K + (denoted as 0.1 K-NH 2 -MIL-101) exhibits a higher CO 2 adsorption capacity (8.2mmol g −1 ) at 298 K, approximately 3.2 times greater than that of NH 2 -MIL-101. Furthermore, it maintains an adsorption capacity of 7.4mmol g −1 after the sixth adsorption–desorption test, indicating excellent cyclic stability. Additionally, 0.1 K-NH 2 -MIL-101 was employed for in situ capture and electrocatalytic CO 2 reduction. By integrating 0.1 K-NH 2 -MIL-101 with a Bi-based catalyst to enhance the local CO 2 concentration, the Faraday efficiency for the formic acid product was effectively increased from 67 % to 85 %.
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Journal of Cleaner Production
·
2024
·
IF 9.7
Song Xiao,Menglei Jin,Junyi Chen,Peng Wu,Ju Tang,Yi Luo,Yi Li
Perfluoroisobutyronitrile (C 4 F 7 N) mixed with CO 2 has emerged as a promising eco-friendly alternative to sulfur hexafluoride (SF 6 ) in gas-insulated equipment (GIE). However, thermal or discharge faults in GIE inevitably lead to the generation of harmful decomposition by-products, necessitating their prompt removal to safeguard equipment operation and personnel safety. In this study, we propose a nanofiber composite material comprising polyacrylonitrile (PAN) as the base and multi-metal organic frameworks (MOFs) as the primary adsorbent material for removing typical decomposition components of C 4 F 7 N/CO 2 gas mixture. Utilizing grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations, we elucidate the selective adsorption mechanisms. Experimental results show that PAN@HKUST-1(Cu) exhibits superior adsorption efficiency for fluorocarbon gases compared to PAN@MIL-101(Cr), while the latter demonstrates better performance for nitrile gases. The PAN@HKUST-1(Cu)/MIL-101(Cr) composite adsorbent effectively removes eight typical harmful decomposition products while minimally affecting C 4 F 7 N. Our findings suggest that PAN@HKUST-1(Cu)/MIL-101(Cr) nanofiber film holds promise as an adsorbent for C 4 F 7 N/CO 2 based GIE.
研究领域:
材料科学
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环境工程
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化学工程
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纳米技术
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MICROCHIMICA ACTA
·
2024
·Vol. 191
·期 3
·1-10
·
IF 5.3
Miao Pandeng,Chen Jiaquan,Xu Guangfu,Yu Tao,Du Yingxiang
Chiral phenyl aromatic compounds (CPACs) are widely used in drug development, food/cosmetic production, and other organic synthesis processes, and their different enantiomers have distinct physiological activities and application differences. A double-layer metal–organic framework composite (MOF-on-MOF) was obtained by in situ synthesis of chiral metal–organic framework (CMOM-3S) on the surface of an iron-based metal–organic framework (NH 2 -MIL-101(Fe)). According to our investigation, MOF-on-MOF composite was for the first time applied to the stationary phase of capillary electrochromatography (CEC), and enantioseparations of eight CPACs were accomplished. Compared with single CMOM-3S, the enantioseparation performance of the coated capillary columns based on NH 2 -MIL-101(Fe)@CMOM-3S was improved by 34.07 ~ 720.0%. The R-/S-mandelic acid in actual sample (apricot leaves) was detected by the newly CEC system to be 0.0118 mg mL −1 and 0.0523 mg mL −1 , respectively. The spike recoveries were 96.60 ~ 104.7%, indicating its good stability and accuracy. In addition, the selective adsorption capacity of MOF-on-MOF composites was verified by adsorption experiments. Graphical Abstract
研究领域:
分析化学
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材料科学
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APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
Wentao Zhang,Kunrui Wei,Wenguang Huang,Jianghua Yang,Yonghai Gan,Shujuan Zhang
Post-synthetic modification with β -diketone has been proven as an effective strategy to improve the visible light response activities of metal-organic frameworks (MOFs). Nevertheless, the effects of the anchored-diketones on the excitonic behaviors and photocatalytic mechanisms of MOFs are still unclear. Herein, two MOFs (MIL-101 with Cr III and MIL-101 with Al III ) were employed as prototypical materials to further understand this post-synthetic modification strategy. Diketone anchoring could enhance the photocatalytic generation of singlet oxygen ( 1 O 2 ) by the two MOFs in a joint mechanism: exciton-mediated energy transfer and photosensitization. Diketone anchoring induced triplet exciton was found playing an important role in the photocatalytic generation of 1 O 2 . The photosensitization of the anchored-diketone also played a key role in the photocatalytic generation of 1 O 2 . The results here provide a useful guidance for the development of MOFs-based photocatalysts and are helpful to realize the regulation of excitonic behaviors and photocatalytic mechanisms of MOFs.
研究领域:
材料科学
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光化学
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环境科学
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Heliyon
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2022
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IF 3.776
Xuezhong Li,Yue Wang,Qi Guo
The porous iron-based metal organic frameworks (NH 2 -MIL-101(Fe)), which consists of 2-amino benzene dicarboxylic acid (H 2 BDC-NH 2 ) and ferrous ions were synthesized through one-step hydrothermal method. The surface area and pore volume of as-synthesized NH 2 -MIL-101(Fe) were 66.48 m 2 /g and 0.09 cm 3 /g, respectively. The excellent photocatalytic performance endows NH 2 -MIL-101(Fe) to generate hydroxyl radical ( OH), which then acting as efficiently active sites for azo dye degradation in wastewater. Meanwhile, the outstanding stability ability of NH 2 -MIL-101(Fe) indicates the potential candidate for wastewater treatment.
研究领域:
环境科学
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材料科学
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化学工程
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CATALYSIS LETTERS
·
2026
·Vol. 156
·期 9
·245
·
IF 2.5
Xia Ruixin,Song Jiahe,Guo Bao,Sun Daolai,Lv Jianhua
An ionic liquid-grafted catalyst, denoted as IL@MIL-101-NH 2 , was synthesized by introducing a novel functionalized bis-imidazolium ionic liquid containing carboxyl groups into the MIL-101-NH 2 (Cr) using a simple one-step method. The structural features of the catalyst were characterized by FT-IR, XRD, XPS, BET, SEM and so on, and its catalytic performance in the cycloaddition reaction of carbon dioxide (CO 2 ) with propylene oxide (PO) to propylene carbonate (PC) was investigated. The results demonstrated that IL@MIL-101-NH 2 exhibited excellent catalytic activity. Under the conditions of 110 °C, 2 MPa, 3 h, and a catalyst loading of 3.0 wt%, a PO conversion of 95.1% and a PC selectivity of 98.7% were achieved. The superior catalytic performance of IL@MIL-101-NH 2 was attributed to the synergistic effect among the Cr 3+ metal active centers, nucleophilic Br − species and hydrogen-bond-donating –COOH groups. In addition, the catalyst maintains good catalytic performance after four consecutive cycles, indicating its favorable stability and promising application potential. Graphical
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122400
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IF 7.5
Longjie Lai,Jie Tao,Yutao Xue,Xusheng Suo,Juan Liu,Qi Liu,Aihua Yuan
Interfacial engineering in heterostructure photocatalysts is crucial for efficient charge migration, yet achieving rational and controllable interface design remains a major challenge. In this work, SnIn 4 S 8 nanosheets were in situ grown on the octahedral surface of MIL-101(Cr) to leverage the Lewis acid-base properties of Cr and S, thereby enabling the controlled construction of an ion-coordinated interface. The resulting MIL-101(Cr)@SnIn 4 S 8 heterojunction enabled efficient capture and conversion of CO 2 and H 2 O. Furthermore, the Lewis acid-base coordination induces interfacial electron density redistribution, generating a built-in electric field that drives the formation of an S-scheme heterojunction between MIL-101(Cr) and SnIn 4 S 8 , while simultaneously preserving high‑energy photogenerated electron-hole pairs. Consequently, MIL-101(Cr)@SnIn 4 S 8 exhibited superior CO 2 photoreduction performance with H 2 O in the gas-solid phase, delivering a CO evolution rate of 26.9 μmol·g −1 ·h −1 . This work provides a viable strategy for interfacial engineering and demonstrates the application potential of S-scheme heterojunctions in photocatalytic reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Yi Hao,Kaili Wang,Cheng Chen,Xingyu Chen,Rongrong Jia,Ping Cheng,Liyi Shi,Lei Huang
Waste PET-derived MIL-101(Cr) enables polyethylene oxidation. • Photogenerated holes directly participate in PE C–H activation. • A thermally assisted photoinduced oxidation pathway is established. • Polyethylene is converted into recoverable dicarboxylic acids. • Cross-polymer valorization integrates PET and PE waste streams. Heterogeneous catalytic oxidation of polyethylene (PE) into dicarboxylic acids remains challenging because of the difficulty in activating chemically inert C–H bonds. Here, we report a waste polyethylene terephthalate (PET)-derived MIL-101(Cr) photothermal catalyst that enables photogenerated hole ( h + )-driven activation of PE during oxidation. Under 130 °C, 1.0 MPa O 2 , and 370 mW cm −2 light irradiation, complete conversion of PE is achieved, affording aliphatic dicarboxylic acids (C4-C22) with a carbon yield of up to 63.7 wt%. Experimental and theoretical investigations reveal that photogenerated h + directly activate C–H bonds of surface-adsorbed PE through hydrogen abstraction, thereby initiating the oxidation process. The carboxylate ligands on the MIL-101(Cr) surface promote favorable interfacial interactions with PE chains, facilitating effective catalyst-polymer contact for interfacial C–H bond activation. This work provides new mechanistic insights into heterogeneous photothermal PE oxidation and offers new guidance for catalyst design based on photogenerated h + oxidation. Download: Download high-res image (246KB) Download: Download full-size image
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JOURNAL OF MOLECULAR STRUCTURE
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2026
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IF 4.9
Hongbin He,Xi Zhu,Ziping Huo,Bolong Liang,Shu-Xuan Liang
AgI@MIL-101(Fe) photocatalyst was fabricated via in-situ precipitation method. • The photocatalyst achieved 95.25% degradation efficiency of OTC within 180 min. • The photocatalyst exhibited excellent practical applicability in real water samples. • Z-scheme heterojunction mechanism and degradation pathway were elucidated. Owing to their extensive and long-term application as well as poor degradability, antibiotics are inevitably persistent in aquatic environments due to their extensive and long-term use as well as heir difficulty in degradation. The development of efficient photocatalysts is therefore of crucial significance in environmental purification. In this study, a Z-scheme MIL-101(Fe) heterojunction photocatalyst was rationally designed and fabricated via a combined solvothermal and in-situ precipitation methods for the efficient removal of oxytetracycline hydrochloride (OTC), where MIL-101(Fe) is a typical member of the metal-organic framework (MOF) family. A series of characterization methods were employed to systematically observe the morphology and microstructure, optical properties, and photocatalytic performance of the as-prepared photocatalyst. The AgI@MIL-101(Fe) nanocomposites achieved an OTC degradation efficiency of 95.25% within 180 min under visible-light irradiation, demonstrating superior photocatalytic activity compared to a single-component counterparts. Structural characterizations results indicated that AgI formed a tight interface contact with MIL-101(Fe), which provided an effective structural foundation for theheterojunction construction. AgI particles were well dispersed on MIL-101(Fe), effectively mitigating their aggregation and thus creating abundant light absorption and reaction sites for photocatalytic reactions. Photoelectrochemical measurements further demonstrated that the nanocomposite possessed strong light absorption ability and high separation efficiency for photogenerated carriers. The as-prepared photocatalyst also exhibited excellent practical applicability in the treatment of actual water samples from Baiyangdian Lake. Five cycles of experiments indicated that its outstanding structural and catalytic stability. Mechanistic investigations identified superoxide radicals (•O 2 − ) as the primary active factors responsible for OTC degradation. Finally, the typical Z-scheme heterojunction mechanism and degradation pathway of OTC were finally proposed. This work provides a new design strategy and practical reference for the development of high-performance photocatalysts targeting the efficient removal of OTC and other antibiotics from aquatic environments. Download: Download high-res image (211KB) Download: Download full-size image
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Materials
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2026
·Vol. 19
·期 4
·753
·
IF 3.7
Ziyang Yang,Xicheng Sun,Wenhui Yuan,Li Li
Highlights What are the main findings? A green acid-free route produces MIL-101/GO-0.1, enabling superior C 3 F 8 capture. The content of graphene oxide affects the adsorption properties of the composite material. MIL-101/GO-0.1 achieved a record-breaking IAST separation selectivity of 17,069 for C 3 F 8 /N 2 . What are the implications of the main findings? Overcome the current technical bottleneck of low C 3 F 8 adsorption capacity. Green synthesis coupled with high adsorption capacity opens up possibilities for industrial applications. This provides insights for future research into the adsorption and separation of C 3 F 8 . As a perfluorinated compound with a high global warming potential, octafluoropropane (C 3 F 8 ) needs to be efficiently separated from industrial waste gas, but separating it from nitrogen at low concentrations is highly challenging. To address the common drawback of using corrosive acids in conventional MIL-101(Cr) synthesis, this study developed a green, acid-free solvothermal method for preparing graphene oxide (GO)-modified MIL-101(Cr) composites (MIL-101/GO). By systematically varying the GO doping, the optimal composite (MIL-101/GO-0.1) exhibited breakthrough adsorption performance: its equilibrium adsorption capacity for C 3 F 8 reached 210 mg/g in fixed-bed breakthrough experiments. The predicted C 3 F 8 adsorption selectivity relative to N 2 reached 17,069, ranking among the highest values reported for adsorbents, indicating a significant performance enhancement over the pristine MIL-101(Cr). Mechanistic analysis reveals that graphene oxide not only increases specific surface area and micropore volume but also enhances dispersion forces, substantially boosting affinity for C 3 F 8 . Additionally, the composite exhibits outstanding cycling stability and thermal stability. This study provides a novel eco-friendly synthetic strategy for high-performance metal–organic frameworks and offers a highly promising candidate material for industrial-scale fluorocarbon recovery.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Xiaojing Tian,Zhiqi Qu,Jiaoyang Wang,Ying Zhang,Zhiping Li,Dandan Peng
Construct TiO 2 @MIL-101-Fe S-scheme via impregnation in situ hydrolysis. • Hierarchically distributed TiO 2 maximizes interfacial contact. • Achieves 13.91% cyclohexane conversion and retains high activity after five cycles. • Interfacial fields drive spatial charge separation and preserve redox potentials. • Hierarchical confinement and pore-mouth anchoring enable selective C H activation. The selective photocatalytic oxidation of cyclohexane is a sustainable and environmentally friendly route for KA-oil production, yet it remains limited by low conversion, moderate selectivity, and inefficient charge utilization. This study employed an in-situ TBOT hydrolysis strategy to synthesize a TiO 2 @MIL-101-Fe S-scheme heterojunction with hierarchically distributed TiO 2 nanodomains within the MOF pores, at pore mouths, and on the external surface. This spatially engineered heterostructure enhances photogenerated carrier separation, stabilizes the interface, and improves cyclohexane oxidation efficiency and KA-oil selectivity. The optimized 50 wt% composite material achieved a cyclohexane conversion rate of 14.3%, which was 2.17 times that of the original MIL-101-Fe material. Meanwhile, it still maintained a cyclohexane conversion rate of up to 13.9% and excellent catalytic activity after five cycles. Steady-state and time-resolved photoluminescence, electrochemical impedance, and transient photocurrent measurements reveal accelerated charge separation and prolonged carrier lifetime, enabled by an S-scheme heterojunction with a built-in interfacial electric field. Radical trapping and ESR studies indicate that photogenerated holes and electrons dominate C H activation, with reactive oxygen species contributing synergistically. DFT calculations confirm directional electron transfer and preserved high redox potentials. This work highlights spatially confined S-scheme heterojunctions as a general strategy to enhance photocatalytic efficiency, selectivity, and stability, offering a promising avenue for solar-driven hydrocarbon oxidation. Graphical abstract Download: Download high-res image (215KB) Download: Download full-size image
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Coatings
·
2025
·Vol. 15
·期 12
·1449
·
IF 2.8
Asen Dimov,George R. Ivanov,Leonard Keil,Andreas Terfort,Jinxuan Liu,Velichka Strijkova
HighlightsWhat are the main findings?A metal–organic Framework (MOF) MIL-101(Cr) with crystal sizes around 20 nm was synthesized and the results were compared to a 300 nm crystal-sized commercially available material.What are the implications of the main findings?Smaller-sized MIL-101(Cr) crystals form a stable insoluble monolayer at the air–water interface with denser, more homogeneous water coverage and packing upon compression, and no visible micrometer-sized aggregates.Langmuir-Blodgett monolayers from the 20 nm MOF show six times lower surface roughness.Metal–Organic Frameworks (MOFs) have diverse applications due to their tunable porosity, large surface area, and diverse chemical functionalities. Among them, one of the most researched MOFs is MIL-101(Cr), which, in addition, is very stable in water. We have used a commercially available substance with approximately 300 nm large crystals for the preparation of a sensing nano-thin layer for the emerging water contaminant PFOS, due to its high selectivity towards this compound. Here, we have synthesized 20 nm sized crystals of MIL-101(Cr), which are among the smallest reported, and compared them to the same material with 300 nm sized crystals. The material was characterized by TEM and XPS. It was possible to prepare insoluble monolayers at the air–water interface (Langmuir films), which were characterized with film compression isotherms, Brewster angle microscopy, and surface potential measurements. The Langmuir–Blodgett (LB) method was used to deposit monolayers on Si wafers and 434 MHz Surface Acoustic Wave resonator simultaneously. The LB layers were very stable over time. The smaller-sized MIL-101 (Cr) crystals exhibit denser, more homogeneous water coverage and packing upon compression, with no observable 10–100 µm aggregates. LB monolayers from the 20 nm particles have approximately six times lower surface roughness. The LB monolayer is far from being smooth, but this will allow excellent access to the MOF pores by the tested analyte in a chemical sensing application. The lack of research on depositing presynthesized MOFs using probably the best method for nanoarchitectonics—the LB method—is addressed. The 20 nm sized MOF crystals are the smallest deposited by this method so far.
研究领域:
材料科学
·
纳米技术
·
表面化学
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分析化学
·
传感器与传感材料
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