JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Mengjiao Yu,Xiong-Fei Zhang,Siting Yang,Yunhua Bai,Zhongguo Wang,Jianfeng Yao
Developing functional catalysts with both Lewis and Brønsted acid sites is an essential task for achieving the direct conversion of glucose to 5-hydroxymethylfurfural (5-HMF), a process that is crucial for the sustainable production of renewable fuels and chemicals. In this work, a mixed-linker strategy is proposed to prepare defective MIL-53(Al)-NH 2 by introducing trifluoroacetic acid into the MIL-53(Al)-NH 2 synthesis process. The creation of defects facilitates the exposure and accessibility of Al 3+ centers, as well as changes the coordination environment within the MIL-53(Al)-NH 2 skeleton. Both the number of Lewis and Brønsted acid sites are boosted, which is beneficial for glucose activation and 5-HMF generation. Through optimizing the reaction conditions, a glucose conversion of 98.3 % with a 5-HMF yield of 59.3 % was achieved by using defective 6d-MIL-53(Al)-NH 2 in a biphasic tetrahydrofuran/H 2 O NaCl system. Moreover, the 6d-MIL-53(Al)-NH 2 catalyst showed excellent recyclability and reusability, with its catalytic efficiency maintained almost unchanged for consecutive 10 cycles. The catalytic mechanism was elucidated and the acidity of the Lewis and Brønsted acid was modulated by defect engineering to achieve exceptional performance.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lei Wang,Yilun Gao,Jianjun Luo,Wenyang Xu,Chi Zhang,Hua Yuan,Yaopeng Zhang,Yaokun Pang
Biodegradable or eco-friendly triboelectric materials from natural polymers are considered promising and viable alternative for the development of green triboelectric nanogenerators (TENGs). Yet, they are mostly struggling from poor mechanical properties and low triboelectric output performance. In this work, we developed a highly efficient NH 2 -MXene/TiO 2 @sodium alginate (NMTS) composite film with NH 2 -MXene/TiO 2 as a filler and sodium alginate (SA) as a matrix and a TENG based on this composite film (NMTS-TENG) was constructed. The tribo-positive characteristic of SA was enhanced by adding NH 2 -MXene and TiO 2 . Different loaded content of the NH 2 -MXene and TiO 2 were explored and optimized to improve mechanical properties of the composite film and the output performance of NMTS-TENG. The microstructure and dielectric constant of the composite films were well characterized to investigate the enhancement mechanism. Under optimal conditions, the tensile strength of the composite film reaches up to 175.0 MPa and surpass the pure SA film. The NMTS-TENG shows the output performance with an open-circuit voltage of 357.6 V and short-circuit current of 55.1 µA, and the output peak power increases by 9.3 times compared with pure SA-based TENG. In addition, we developed a TENG device to harvest ocean wave energy for self-powered cathodic protection. The electrochemical test results reveal that the open circuit potential of the protected Q235 carbon steel can decrease by 74 mV and the corrosion potential decrease by 146.5 mV, indicating the good anti-corrosion properties. This study provides a promising method to develop high-performance biomaterials based TENG and expands the practical application of SA in the field of the electrochemical cathodic protection.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Yongbo He,Mengqi Liu,Linzhi Zhai,Hongshuang Li,Peng Song,Xiufang Zhu,Yubin Tang
The metal organic framework (MOF) polycrystalline membranes on stainless steel mesh (SSM) are urgently required for effective oil-water separation, but the affordable preparation still remains a challenge. Herein, we report a series of UiO-66-NH 2 /SSM films, which are developed by a rational ‘seeding-assisted secondary growth’ method. Results depict that the proposed method greatly shortens the synthesis time, and helps to achieve a continuous and uniform modification of UiO-66-NH 2 on SSM, and hence contributes to a superior hydrophilicity and superoleophobicity for UiO-66-NH 2 /SSM with minimum water contact angle of 32° and maximum underwater oil contact angle of 150°, respectively. Specifically, the UiO-66-NH 2 /SSM-600–2 has total permeation fluxes and separation efficiencies of ca. 8.4×10 4 L·m −2 ·h −1 and 100% for the n-hexane-, petroleum ether- and chloroform-water emulsions (1% volume ratio), which exceed numerous polycrystalline membranes reported so far. It also exhibits a great durability with only 0.1% loss of separation efficiency after 8 cycles. Furthermore, outstanding acid-resistivity and salt-tolerance are also presented. Our work supplies a new strategy to construct UiO-66-NH 2 /SSM, and the decent properties confirm a huge potential for practical use in oil-water separation.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yating Xie,Nicui Yuan,Hongyang Liu,Lukai Luo,Jun Gong,Xiping Yin,Tengfei Li,Yonghua Zhou
Defect engineering by creating oxygen vacancies (OVs) and heterogeneous frustrated Lewis acid-base pairs (FLPs) emerged as an efficient strategy to enhance the selective conversion CO 2 to CH 4 . Considering the intrinsic FLPs contained in UiO-66-NH 2 (UNH for abbreviation), in this paper, the OVs was introduced therein by fabricating the Ce-doped UNH (denoted as UNH(Ce/Zr)) via one-step solvothermal route. The as-prepared UNH(Ce/Zr) catalyst exhibited the CH 4 yield of 31.02 μmol·g −1 ·h −1 accompanied with the CH 4 selectivity of 93 % and satisfying recycling stability. The XRD, SEM, FT-IR, XPS, TG, TPD and NH 3 in situ DRIFTS and in situ FT-IR characterization results justified that the UNH(Ce/Zr) possess the obviously increased OVs sites and enhanced Lewis acidic and basic properties. Additionally, the photoelectrochemical characterization results showed that UNH(Ce/Zr)−0.014 efficiently improved photogenerated electron-hole separation efficiency and charge transfer rate. It could be concluded that it was the cooperative action of OVs and FLPs that led to the high CH 4 selectivity and CH 4 yield.
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INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Wenfan Yu,Zhenxuan Liang,Shaoyu Luo,Qian Yan,Yi Sun,Yisheng Zhu,Shifeng Zhang
Metal-organic frameworks (MOFs) are highly advantageous due to their tunable pore size, exceptional thermal and chemical stability, and high specific surface area, making them ideal for applications in formaldehyde adsorption. However, the practical use of powdered MOFs is significantly hindered by their recycling challenges. In this research, wood-based composite aerogels (WAZN-X) were successfully prepared through loading Zeolitic Imidazolate Framework-8-NH 2 (ZIF-8-NH 2 ) inside wood aerogels. Ascribing to the elimination of lignin and hemicellulose, the enlarged pore structures of wood aerogels and the potential interactions (e.g., hydrogen bonding and electrostatic attractions) between components promoted the uniformly depositing of ZIF-8-NH 2 nanocrystals. The WAZN-X aerogels displayed excellent mechanical strength (e.g., the longitudinal Young’s modulus of 68.57 MPa) and promising formaldehyde adsorption performance (e.g., a stable formaldehyde removal rate of 98.11 %), and kept commendable reusability (95.98 % after 5 cycles). This research provides a new insight for developing high-value functional composite adsorbents for efficient formaldehyde purification.
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COMPOSITES COMMUNICATIONS
·
2024
·
IF 6.5
Xinyue Yang,Yong Li,Deyun Yue,Rui Li,Haojie Song
The construction of ternary heterojunction photocatalysts can achieve multi-gradient transfer of charges and accurate control the position of photogenerated electrons which has received increasing attention. In this paper, NH 2 -MIL-53(Al)@BiOBr@CQDs-10 % (ABCQDs-10 %) was prepared via a facile hydrothermal and chemical synthesis processes. Three-dimensional serration of NH 2 -MIL-53(Al) as a platform for irregular BiOBr nanosheets, CQDs promote interfacial contact and act as electron transport channels between BiOBr and NH 2 -MIL-53(Al) and constitute Z-type heterojunctions with high redox properties. ABCQDs-10 % shows the best photocatalytic removal efficiency (94.24 %) of CIP, the reaction rate constants (0.045 min −1 ) were 1.2 and 64 times higher than BiOBr and NH 2 -MIL-53(Al), respectively. The excellent degradation performance is attributed to the construction of Z-type heterojunction of NH 2 -MIL-53(Al)@BiOBr@CQDs which improve electron-hole separation and transfer efficiency. The main active species was •O 2 - . The photocatalytic activity of ABCQDs-10 % had not obvious loss after cycle experiments and the crystal structure had no significant changes, means high stable photocatalytic activity.
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Materials Today Communications
·
2025
·
IF 4.5
Jiahua Cheng,Linya Fei,Xiaoqing Zhou,Beibei Lu,Zhihui Zhang,Le Chen,Guojian Ji
UiO-66 and its functionalized derivatives (UiO-66-X, X = -OH, -NO 2 , -NH 2 ) were successfully synthesized via a solvothermal method, and their structural integrity and functionalization were confirmed. Hydrogen adsorption experiments and Grand Canonical Monte Carlo (GCMC) simulations demonstrated that UiO-66-OH exhibited the highest hydrogen adsorption capacity. At 300 K and 1 bar, its experimental adsorption capacity reached 0.0301 wt%, representing increases of 29.18 %, 3.44 %, and 19.92 % compared to UiO-66, UiO-66-NH 2 , and UiO-66-NO 2 , respectively. At 77 K and 20 bar, its simulated adsorption capacity reached 2.352 wt%, surpassing UiO-66-NH 2 (2.229 wt%) and UiO-66-NO 2 (1.927 wt%). This superior performance is attributed to optimized pore structure and enhanced functional group interactions, providing new insights for optimizing hydrogen storage in UiO-66 materials.
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LANGMUIR
·
2024
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IF 3.7
Yinyin Peng,Ting Pan,Chuang Chen,Yuchen Zhang,Guoyuan Yuan,Derong Liu,Xiaoqin Pu,Wei Xiong
In this study, researchers developed a novel composite material called NH2-MIL-53-Al/PAN, which consists of metal–organic frameworks (MOFs) grown on electrospun PAN nanofibers (NFs). The successful formation of the composite was confirmed by X-ray diffraction (XRD) and Fourier transform infrared (FTIR), and the hydrophilicity of NH2-MIL-53-Al/PAN was demonstrated by the water contact angle (WCA). Batch experiments were conducted to investigate the adsorption performance of Co(II) under different conditions. The maximum adsorption capacity reached 58.72 mg/g, and almost 95% of the adsorption was achieved within the first 6 h. The adsorption process was found to be spontaneous and endothermic and followed the pseudo-second-order kinetics and Langmuir models. Chemisorption and molecular layer adsorption are the main mechanisms of adsorption, and X-ray photoelectron spectroscopy (XPS) analysis further reveals that the interaction between the adsorbent and cobalt is a coordination interaction. In this study, NH2-MIL-53-Al was grown in situ on PAN to ensure effective loading of MOFs and prevent agglomeration during the NF mixing process. This approach successfully addressed the challenge of exposing active sites within the embedded MOF crystals. Additionally, it overcame the difficulty of recycling traditional MOF adsorbents. As a result, the exceptional performance of MOF NFs offers a promising solution for the efficient removal of cobalt-containing wastewater.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Hongfei Jia,Yangchen Wang,Lizi Yang,Ran Fang
Lithium metal, a pivotal element in modern electric vehicles and electronics, necessitates secure and sustainable supply chains. Extracting lithium from brines presents significant challenges, particularly when dealing with high magnesium-to-lithium ratios, due to the nearly identical ionic radii of lithium and magnesium ions. Herein, we propose an innovative strategy for the selective separation of Li + /Mg 2+ by integrating ZIF-8-NH 2 into polyamide membranes through the interfacial polymerization (IP) of polyethyleneimine (PEI) and trimesoyl chloride (TMC). The synthesized PEI@ZIF-8-NH 2 + TMC membranes exhibit an impressive permeation rate for Li + of 0.863 mol m -2 h -1 , alongside a Li + /Mg 2+ selectivity ratio of 33.06. The unique pore structure of ZIF-8-NH 2 and surface chemistry facilitate efficient Li + /Mg 2+ separation, driven by synergistic interactions such as elevated positive surface charges, subnanometer channels, and strong π-π stacking with polyamide layers. These developments are anticipated to augment both the selectivity and durability of MOF-based membranes, providing new directions for research and practical implementations in ion separation technology.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Wei Liu,Ming Yang,Shuang Wang,Yan-Sai Bao,Yong-He Cui,Ling-Xu Meng,Liang-Cheng Li,Yang Wu,Yu-Yang Zhang
Solid-phase microextraction (SPME) has been widely used for the analyzing trace organic pollutants in environmental samples. The properties of coatings have a significant effect on the application range, selectivity and sensitivity of existing analytical methods. Therefore, the development of SPME technology depends on fibers with a stable, efficient, and selective coating. In this study, metal-organic frameworks (MOFs) were used to fabricate porous carbon membranes in situ for SPME. The composite material (UIO66-NH 2 @PAC) was directly carbonized to prepare a derivative porous carbon material (C-UIO66-NH 2 @PAC), which was applied to the extraction of off-odour organic pollutants for the first time. The Zr-N co-doping in the material was not only beneficial to the formation of derivatized porous carbon, but also endowed it with a certain hydrophilicity, which was highly advantageous for capturing weakly polar compounds. By optimizing the extraction and desorption conditions, a highly selective and sensitive analytical method was developed, which exhibited a detection limit of 0.61 and 0.78 ng L −1 for 2-methylisoborneol (2-MIB) and geosmin (GSM), respectively, along with a linear range from 10 to 3000 ng L −1 . Both intra-fiber repeatability (RSD 5.5 % and 3.7 %) and inter-fiber repeatability (RSD 9.7 % and 8.8 %) were satisfactory. The fiber coated with C-UIO66-NH 2 @PAC exhibited high extraction efficiency (the extraction efficiency of the analytes was 4.6–8.3 times higher than that of commercial fibers), and had excellent thermal and chemical stability. Finally, the C-UIO66-NH 2 @PAC-coated fibers were successfully applied to the SPME analysis of off-odour organic pollutants in real water samples, and these results highlighted the broad prospect for the detection of natural/drinking water.
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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.
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Processes
·
2024
·Vol. 12
·期 9
·1879
·
IF 2.8
Huiying Yang,Xiangchao Meng
The conversion of nitrogen (N2) and water (H2O) into NH3by photocatalysis under ambient conditions has been considered an environmentally friendly strategy. However, developing effective catalysts for N2fixation is still challenging. Herein, we report a bimetallic JH Fe, Co/TiO2derived from NH2-MIL-125(Ti) by the fast Joule heating (FJH) method for visible–light–driven catalytic N2fixation. It was found that the photocatalytic N2reduction efficiency of bimetallic FC@TiO2-JH was improved, enabling an NH3yield rate of 110.14 µmol g−1h−1without any sacrificial agents. Furthermore, the rate was higher than those of Fe@TiO2-JH and Co@TiO2-JH, suggesting that the synergistic effect between Fe and Co broke the electronic equilibrium and increased the center of its d-band, enhancing electronic feedback to the antibonding π* orbitals of N2while weakening the bonding energy of N≡N. Meanwhile, the rate was about 2.75 times higher than that of FC@TiO2-TF, which was calcined in a tube furnace. It is assumed that FJH might lead to the formation of lattice defects, leading to localized charge deficiency, enhanced carrier separation, and transport. Thus, doping of Fe and Co synergistically interacted with the defects produced from FJH, facilitating the photocatalytic reduction process. As detected, it had a greater ability to separate hole–electron pairs and transferred electrons to adsorbed N2at faster rates. Our work demonstrates a prospective strategy for designing bimetallic catalysts derived from NH2-MIL-125(Ti) for N2fixation.
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