Surfaces and Interfaces
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2024
·
IF 5.7
Ting Pan,Chuang Chen,Li Yu,Cong Yin,Mi Zhou,Huidong Qiu,Guoyuan Yuan,Wei Xiong,Xiaoqin Pu
In addressing the crucial need for separating cobalt ions from leachate solutions of spent ternary lithium batteries (TLBs), this study focuses on the development of an innovative molecular sieve (MS)-based MOFs material, MS-MIL-53(Al), synthesized by combining MS with 2,5-dihydroxyterephthalic acid. Since the powdered MS-MIL-53(Al) material presents a granular powdery form, which is difficult to recover during the adsorption process, electrospun nanofibers denoted as MS-MIL-53(Al)/PAN, were fabricated and functionalized with hydroxylamine hydrochloride to create MS-MIL-53(Al)/AOPAN. Static adsorption experiments conducted with MS-MIL-53(AL)/AOPAN as the adsorbent in cobalt-containing wastewater revealed a maximum adsorption content of 65.3 mg/g for Co(II). Moreover, the material exhibited a tensile strength at the breaking point of 0.077 kPa, indicating its excellent mechanical properties. The adsorption process followed pseudo-second-order kinetics and the Langmuir isotherm model, showcasing a spontaneous, endothermic monolayer chemical adsorption behavior. XPS analysis highlighted the influence of hydroxy and amidoxime functional groups on Co(II) adsorption. Notably, MS-MIL-53(Al)/AOPAN displayed exceptional stability, retaining over 90 % of its adsorption capacity after five cycles, demonstrating its potential for efficient Co(II) separation in wastewater treatment. This study is the first to synthesize MOFs material using MS as the base material, showing potential cost reduction and enhanced adsorption capabilities, with implications for advancing the innovative use of MOFs.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Journal of Environmental Sciences
·
2020
·
IF 4.302
Jingjing Zhao,Linqiong Xu,Yaozhuo Su,Hongwei Yu,Hui Liu,Shaoping Qian,Wenge Zheng,Yongqing Zhao
ABSTRACT Zirconium-based metal-organic frameworks (Zr-MOFs) have attracted widespread attention due to their high specific surface area, high porosity, abundant metal active sites and excellent hydrothermal stability. However, Zr-MOFs materials are mostly powdery in nature and thus difficult to separate from aqueous media, which limits their application in wastewater treatment . In this study, PDA/Zr-MOFs/PU foam was constructed by growing Zr-MOFs nanoparticles on a dopamine-modified polyurethane foam substrate by in-situ hydrothermal synthesis as an adsorbent for removing dyes from wastewater. The results demonstrated that the polydopamine coating improves the dispersion of the Zr-MOFs nanoparticles on the substrate and enhances the interaction between the Zr-MOFs nanoparticles and the PU foam substrate. As a result, compared with Zr-MOFs/PU foam, the prepared PDA/Zr-MOFs/PU foam exhibits higher adsorption capacity for crystal violet (CV) (63.38 mg/g) and rhodamine B (RB) (67.73 mg/g), with maximum adsorption efficiencies of CV and RB of 98.4% (pH=11) and 93.5% (pH=7), respectively, at a concentration of 10 mg/L. The PDA/Zr-MOFs/PU foam can simultaneously remove CV and RB from the mixed solution. Moreover, the PDA/Zr-MOFs/PU foam still exhibits high stability and reusability after five cycles.
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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DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2024
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IF 4.4
Yao Ning,Yuqi Yang,Dongming Shan,Shuxing Mei,Yibai Yan,Linjie Ding,Ying Zhang
Ethylene oligomerization plays an important role in industrial production. However, when taking the traditional non-metallocene catalysts and MOF catalysts for ethylene oligomerization, they typically require methylaluminoxane (MAO), aluminum alkyl, and other cocatalysts, which is neither environmentally friendly nor helpful in reducing production costs. Here, three sulfonic acid-modified MOFs (SA/MIL-101(Cr), UiO-66-NS and MIL-101(Cr)-NS) were prepared and used as catalysts for ethylene oligomerization at room temperature without using any cocatalysts. All of them exhibited excellent catalytic performances (e.g., 10SA/MIL-101(Cr), 21 953 g molCr−1 h−1, with C8 selectivity greater than 70.32%), and their oligomerization activity increased by almost tenfold compared to unmodified MOFs. The presence of Lewis acid (L acid) and Brønsted acid (B acid) sites in modified MOFs is the key to improved performances. In particular, the presence of B acid weakens the role of metal clusters and ligands in MOFs, making it easier for metal centers to bind to ethylene molecules for further oligomerization. This work first demonstrates that bifunctional MOF catalysts can catalyze ethylene tetramerization under mild conditions without cocatalysts.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Mengzhen Song,Jingru Han,Yingzhi Wang,Lungang Chen,YanYan Chen,Xiaoyuan Liao
Fe-based MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based MOF catalysts. In this work, we manipulated the structure of Fe-oxo nodes in MIL-88B(Fe) via a CuI species substitution method, affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved Fenton-like performance. It is found that the CuI serves as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results. A linear relationship was observed for the Fenton-like performance and the amount of CuI species for the catalysts. The corresponding value of the •OH formation is 2.17 eV for Cu-incorporated MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe) (2.69 eV). Meanwhile, the enriched CuI species suppress Fe species leaching during the catalytic reaction. The Fe-ion leakage of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly less than that of MIL-88B (2.00–3.02 mg/L). At the same time, H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%, which is almost 4.4 times that of pure MIL-88B(Fe). This work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for wastewater treatment.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 24
·5845
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IF 4.2
Yaling Wu,Zhaopeng Sun,Yingying Chen,Dan Liu,Yan Meng,Zheng Yan
Metal synergy can enhance the catalytic performance, and a prefabricated solid precursor can guide the ordered embedding, of secondary metal source ions for the rapid synthesis of bimetallic organic frameworks (MM’-MOFs) with a stoichiometric ratio of 1:1. In this paper, Co-MOF-1D containing well-defined binding sites was synthesized by mechanical ball milling, which was used as a template for the induced introduction of Fe ions to successfully assemble the ordered bimetallic Co 1 Fe 1 -MOF-74@2 (where @2 denotes template-directed synthesis of MOF-74). Its electrocatalytic performance is superior to that of the conventional one-step-synthesized Co 1 Fe 1 -MOF-74@1 (where @1 denotes one-step synthesis of MOF-74), and the ratio of the two metal sources, Co and Fe, is close to 1:1. Meanwhile, the iron valence states (Fe II and Fe III ) in Co 1 Fe 1 -MOF-74@2 were further regulated to obtain the electrocatalytic materials Co 1 Fe 1 (II)-MOF-74@2 and Co 1 Fe 1 (III)-MOF-74@2 . The electrochemical performance test results confirm that Co 1 Fe 1 (II)-MOF-74@2 regulated by valence state has a better catalytic performance than Co 1 Fe 1 (III)-MOF-74@2 in the oxygen evolution reaction (OER) process. This phenomenon is related to the gradual increase in the valence state of Fe ions in Co 1 Fe 1 (II)-MOF-74@2 , which promotes the continuous improvement in the performance of the MOF before reaching the optimal steady state and makes the OER performance reach the optimum when the Fe II /Fe III mixed-valence state reaches a certain proportion. This provides a new idea for the directed synthesis and optimization of highly efficient catalysts.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Wangchang Geng,Pengfei Song,Xinrou Cao,Libing Duan
Metal-organic frameworks (MOFs)-derived metal oxides are characterized by high porosity, large specific surface area, controllable composition, and tunable pore size, which make them have good potential as gas sensing materials. In this paper, Ni 3 V 2 O 8 @NiO hollow microspheres derived from bimetallic Ni/V-MOFs were synthesized using a three-step method (solvothermal method, cation-exchange method, and annealing process). XRD, Raman, SEM, TEM, XPS, and BET techniques were employed to investigate the structure, morphology, specific surface area, pore size distributions, elemental composition, and chemical state of Ni 3 V 2 O 8 @NiO composites. Gas sensing performance studies showed that the NV@NiO-2 sensor exhibited higher response (43.7) to 100 ppm triethylamine at a lower operating temperature (240℃), shorter response/recovery time (88 s/127 s), higher selectivity, lower detection limit (4.5 ppb), and better repeatability. In addition, the NV@NiO-2 sensor exhibited a strong linear relationship (R 2 = 0.996) between response and gas concentration across a range of 1–100 ppm. The present work serves as a valuable reference for the preparation of triethylamine sensing materials with high specific surface area, high porosity, high response and high selectivity.
研究领域:
材料科学
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化学传感器
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DOI
高影响因子
RSC Advances
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2015
·Vol. 5
·期 41
·32714-32719
·
IF 3.84
Gui-lin Zhuang,Jia-qi Bai,Li Tan,Hong-liang Huang,Yi-fen Gao,Xing Zhong,Chong-li Zhong,Jian-guo Wang
Zr-based MOFs usually feature exceptionally high thermal and chemical stability, which suggests that composites of noble metals and Zr-based MOFs could have wide industrial applications. In this work, we report the synthesis and characterization of Pd nanoparticles (of three different loadings: 0.3%, 0.5% and 1.0%) supported on micro-crystal DUT-67 MOFs. Via SEM, TEM and XPS characterization methods, it was found that the Pd nanoparticles were well dispersed on the interface of the MOF micro-crystals, with a diameter of 3.5 nm, and both the dangling organic groups and the cavities of the MOFs play important roles. Furthermore, PXRD, IR, TGA and N2 adsorption measurements confirmed that the composites are very robust. Studies on the catalytic properties indicated that they have good catalytic performance with a conversion of 99% and selectivity of 89% in the Suzuki coupling reaction. By a series of explorations, we found the best catalytic conditions are an ethanol–water mixed solvent as the medium, K2CO3 as the base and a temperature of 70 °C. Moreover, good catalytic properties were also shown for the hydrogenation of nitrobenzene, where the optimum temperature was 60 °C, and a conversion of 99% and selectivity of 99% were achieved.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Shuang Liang,Guanzhihui Wang,Likun Dong,Xiaobo Yang,Bao Zhou,Zhuoqi Duan,Zaixin Xie,Yongmao Hu
Metal-organic frameworks (MOFs) are great precursors and templates for preparing adsorbents, catalysts and electrodes due to the porous structure and high specific surface area. We report a promising approach to prepare nanocrystalline Co, Ni sulfides (CNS) embedded and N self-doped porous carbon (NPC) matrix composites derived from NiCo-MOFs. The CNS@NPC composite was investigated as electrodes for hybrid supercapacitors (HSCs). The prepared electrode achieved specific capacitance of 2789 F g −1 at 1 A/g, and high capacitance retention of 88.93% after 6000 galvanostatic charge–discharge (GCD) cycles under 10 A/g. The HSC structured with CNS@NPC//AC achieved an energy density of 46.79 Wh kg −1 at power density of 800 W kg −1 . Meanwhile, specific capacitance of 131.56 F g −1 at 1 A/g and capacitance retention of 99.17% over 6000 GCD cycles under 3 A/g were obtained. Space confinement by the carbon skeleton effectively prevents the aggregation of the redox active nanocrystalline and improves the durability of the electrode. Meanwhile, the carbon skeleton provides abundant charge transfer channels to enhance the redox reaction. In other words, synergistic effect of the carbon skeleton and the active redox nanocrystalline significantly improves the electrochemical properties of the composite.
研究领域:
材料科学
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能源存储与转换
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Menghan Qin,Yumiao Shi,Dingkun Lu,Jingjing Deng,Guoyue Shi,Tianshu Zhou
Due to the excessive use, cephalosporin antibiotics have been detected in various aquatic environments, which may result in environmental and health concern. In this study, bimetallic metal–organic frameworks (MOFs), Hf-UiO-66 and Ti-UiO-66, were successfully designed and obtained via post-synthetic method from UiO-66 for the adsorption of cefoperazone. A serious of adsorption experiments were investigated. The adsorption kinetics and isotherms demonstrated that the adsorption process followed pseudo-second-order kinetic model and Langmuir isotherm model. Hf/Ti-UiO-66 exhibited much better adsorption performance than the undoped UiO-66. Particularly, Hf-UiO-66 had the highest adsorption capacity (346.0 mg g −1 ). With the introduction of Hf or Ti, the chemical coordination environment changed, which resulted in defective structures of MOFs. Such defective structures increased the adsorption active sites, changed the surface charges and enlarged pores. Based on the characterization by FT-IR, XPS, and zeta potential, it was identified that the electrostatic attraction, π-π stacking, hydrogen bonding and metal complexation were the driving force for the high adsorption capacity of the bimetallic MOFs. The as-prepared MOFs displayed good stability and reusability. This work provides a great prospect for the design and application of bimetallic defective MOFs in cephalosporins removal in environmental water.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Chang Ping Yang,Cong Yi Hu,Zhong Wei Jiang,Si Yu Xiao,Xiao Yan Wang,Cheng Zhi Huang,Yuan Fang Li,Shu Jun Zhen
The slow conversion of Fe(Ⅱ)/Fe(III) cycle was largely limited the degradation efficiency of many photo-Fenton systems. Herein, four Fe-MOFs nanorods (namely Fe-TCPP-1, Fe-TCPP-2, Fe-TCPP-3, Fe-TCPP-4) with decreasing length-diameter ratios were synthesized in a household microwave oven, using photosensitizer porphyrin and iron ions with Fenton activity as building blocks. Among them, the Fe-TCPP-3 exhibited high photogenerated electron-hole ( e − - h + ) separation efficiency and largest pore structure , endowing Fe-TCPP-3 with superior photo-Fenton property. In addition, Fe-TCPP-3 based photo-Fenton system was applied to efficiently degrade antibiotic ciprofloxacin (CIP) under neutral condition, due to the continuously generated reactive species ( h + , e − , OH · , O 2 ·– , 1 O 2 ) in Fe-TCPP-3 under visible-light irradiation. With irradiation for 30 min, the degradation efficiency of the system could reach about 73 %, which was about 26-fold towards the system without light irradiation . This study paved a way to modulating the photo-Fenton activity of MOF-based catalysts.
研究领域:
材料科学
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环境化学
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光化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yi Wang,Liang Li,Fangli Zhang,Huajiang Wang,Zhaoliang Cui,Zhaohui Wang,Xiaozu Wang
Mixed matrix membranes (MMMs) can significantly improve gas separation performance, but the type and state of the filler in the membrane matrix are key indicators for the development of MMMs. Therefore, in this work, 6FDA-DAM/ODA (1:1), metal–organic frameworks (MOFs) with different particle sizes (UiO-66 and UiO-66-NH2) were synthesized, and then MOFs were doped into 6FDA-DAM/ODA to prepare MMMs. The effects of the dopant materials and their particle sizes on the gas separation performance of the membranes were investigated by testing the permeability of the MMMs to H2, CO2, CH4, and N2. When the dopant material was UIO-66, the permeability and selectivity of MMMs for each gas were significantly improved compared with that of the original membrane; when the dopant material was 300 nm UIO-66-NH2 with a loading of 10 wt %, the permeability performance and the CO2/CH4 selectivity increased from 44.1 to 57.2 compared with that of the original membrane. The permeation performance for CO2, N2, and H2 and the selectivity for CO2/N2, H2/N2, and H2/CH4 were also significantly improved. In terms of comprehensive separation performance, doping 300 nm UiO-66-NH2 was better than doping 70 and 400 nm UiO-66-NH2 and also showed excellent performance in 50:50 (vol/vol) CO2/CH4 binary mixed gas separation. This work provides an idea for the fabrication of MMMs for high-performance gas separation.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Xialin Ji,Xiaoke Tian,Mengqing Zhou,Changzhou Chen,Jianchun Jiang
In this study, different kinds of lignin, including enzymatic hydrolysis of lignin (EHL), alkaline lignin (AL), kraft lignin (KL) and sodium lignosulfonate (LS) were investigated as precursor to prepare Ni@BTC@X (X= EHL, AL, KL, LS) catalysts using a traditional hydrothermal method with Ni-MOF for HDO upgrading of lignin derivative vanillin (VAN) to generate high value chemical 2-methoxy-4-methylphenol (MMP). The catalytic performance of these catalysts was investigated under different reaction conditions, and it was explored that the conversion of VAN was close to 100 % and the MMP yield was close to 90 % under the optimal conditions (Ni@BTC@LS catalyst, 220 ℃, 4 h, isopropanol, 2 MPa N 2 ). Various physical-chemical characterization results verified that the effects of active sites Ni, porous structure of lignin biochar support and electronic properties of the catalysts played a significiant role in HDO of lignin derived VAN. Additionally, synergistic effect of the highly homogeneously dispersed oxygen vacancies and acidic sites also promoted the VAN conversion efficiency. This work developed a strategy combing the advantages of MOFs and biomass derived substrates for manufacturing novel lignin/MOFs materials in the catalytic field.
研究领域:
化学工程
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环境科学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）