Journal of Environmental Chemical Engineering
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2025
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IF 7.2
YiRong Yao,Bing Xing,Jianbing Chen,YanLun Ren,YuJia Ma,Ying Zhang,Li Zhang
This study proposes an advanced method to tackle CO 2 emissions by enhancing solid acid catalysts, aiming to reduce the high energy consumption and low economic efficiency typically associated with chemical absorption processes. The research involves modifying commercial HZSM-5 zeolites through Cu ion exchange, with the optimal performance observed at a Cu ion content of 2.86 % and a Cu salt concentration of 0.2 M. This modification significantly minimizes the loss of copper ions—a common issue in the impregnation method—resulting in a 76.62 % reduction in the loss of active components. To further improve CO 2 gas-liquid mass transfer, mesoporous MCM-41 zeolites were introduced. Experimental results demonstrate that, at a regeneration temperature of 86°C and a mass ratio of 2:1 for HZSM-5 to MCM-41, the combined catalyst achieves a 61.28 % reduction in relative heat duty compared to the blank sample. Moreover, the energy consumption is 12.33 % and 16.45 % lower than that of HZSM-5 and MCM-41 used individually. Characterization analysis reveals that, under comparable acidic active site densities, catalysts with superior physical pore structures exhibit enhanced catalytic performance. The introduction of mesoporous structures notably improves the bidirectional mass transfer efficiency between carbamate macromolecules and CO 2 molecules. This work successfully demonstrates the synergistic effect of combining Cu ion-modified HZSM-5 zeolites with mesoporous MCM-41, leveraging the abundant active sites of HZSM-5 while harnessing the enhanced mass transfer properties of MCM-41.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Luxiao Zhou,Kun Gao,Huahua Yu,Ronge Xing,Song Liu,Weixiang Liu,Pengcheng Li,Yukun Qin
Chitin is a class of biomass second only to cellulose in abundance, and the preparation of platform compounds from chitin holds great promise. Herein, a pretreatment biphasic solvent system and a catalytic two-stage process are combined for the direct synthesis of 5-hydroxymethylfurfural (HMF) from chitin. The first step of the process, i.e., the pretreatment of chitin with a CH 3 OH/CaCl 2 solution, alters the structure of chitin, allowing it to be depolymerized more easily. In the second step of the process, a green and recyclable biphasic catalytic solvent system comprising a formic acid solution and n-butanol is prepared using pretreated chitin (Ca-PC) as the starting reactant, realizing an HMF yield of 47.65 % in 32 min. This HMF yield surpasses that reported in the literature (19.3 %–30 %). The synergistic interaction of Ca 2+ , introduced via formic acid pretreatment, is the key to the catalytic system of chitin, which disrupts the internal hydrogen bonding of chitin and simultaneously improves HMF selectivity. In summary, we have promoted the depolymerization of chitin using a simple and effective pretreatment process, designed a catalytic system with a green recyclable reaction, and effectively improved the yield of HMF directly prepared from chitin.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2024
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IF 5.3
Haofei Ji,Zhilin He,Ying Huang,Xiuen Cao,Qubo Zhu
5-Fluorouracil (5-FU) is a conventional nucleotide analogue used for cancer treatment. However, its clinical application faces challenges such as low stability and non-specific toxicity. With the remarkable advancements in DNA nanotechnology, DNA-based self-assembled nanocarriers have emerged as powerful tools for delivering nucleotide drugs. In this study, we have designed a non-linear hybrid chain reaction involving a fuel strand with AS1411 aptamer sequence to construct a dendritic structure capable of carrying 5-FU. This structure specifically targets cancer cells with overexpressed nucleolin on their surface, allowing the 5-FU to exert its anticancer effects and achieve therapeutic outcomes. Furthermore, we have also investigated the mechanistic action of this drug delivery system, aiming to establish a novel therapeutic platform for 5-FU treatment.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Cong Wang,Gang Li,Zheng Huang,Anfeng Peng
The cumbersome air isolation process is one of the main constraints in the development of linear α-olefins prepared by ethylene oligomerization. An effective way to solve this problem is to eliminate the use of an alkyl-aluminum cocatalyst. Herein, two forms of Versailles/Santa Barbara-5 (VSB-5) (VSB-5-H3PO4 and VSB-5-NaH2PO2) are prepared and used as heterogeneous catalysts in ethylene oligomerization in the presence of LiAlH4 as a cocatalyst. Compared to other Ni-MOFs and Ni silica–aluminate catalysts, VSB-5s maintain a wider distribution of Linear α-olefin (LAO) products at relatively high activity. In the reuse test of the catalyst, the Al species from LiAlH4 cover the surface of the catalyst and decrease its activity, which could be removed by acid treatment. In situ IR studies show that active centers for ethylene oligomerization may form in VSB-5 assisted by LiAlH4. In addition, a Cossee–Arlman-type mechanism is proposed.
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Inorganic Chemistry Frontiers
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2024
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IF 6.1
Yifei Li,Senyao Meng,Ping Wang,Miao He,Jiasai Yao,Cheng Yang,Fangzhou Mo,Jiang Li,Zhenxing Li
The crystal facet of CeO2 is crucial in governing the catalytic performance of CeO2. However, studies on the relationship between the photocatalytic oxidation performance of CeO2 and its crystal facets are scarce. Herein, we synthesized a series of CeO2. Through loading Cu single atoms (Cu/CeO2), the facet effects of crystal facets on photocatalytic selective oxidation were systematically studied by employing the selective oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran as a model. Because the (110) facet's superior electron transfer efficiency is feasible for absorbing 5-hydroxymethylfurfural, eliminating α-H, and desorbing 2,5-diformylfuran, the selectivity of Cu/CeO2-nanorods (Cu/CeO2-R) with the (110) facet (93.34%) is much higher than that of Cu/CeO2-nanocubes (Cu/CeO2-C) with the (100) facet (32.22%) and Cu/CeO2-nanooctahedra (Cu/CeO2-O) with the (111) facet (15.20%). DFT calculation shows that Cu 3d exhibits orbital hybridization with Ce 5d and 4f, which provides a favorable pathway for electron transfer. This work delves into the facet-performance relationship during the photocatalytic process.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jiantao Su,Xiaohui Yang,Hui Shi,Shuangquan Yao,Minghao Zhou
Catalytic conversion of biomass-derived value-added chemicals was of great significance for the utilization of renewable biomass resources to instead of fossil chemicals. Biomass-derived lignin was regarded as an important support and 5-hydroxymethylfurfural (HMF) was a vital platform chemical derived from cellulose. Herein, a series of lignin-MOF hybrid catalysts were prepared and modified with different heteropolyacids (HPAs), which were then successfully introduced into the selective conversion of HMF to 5-hydroxymethylfurfuryl alcohol (MFA). The effect of different HPA, calcination temperature, etc. were all studied, and all catalysts were well characterized. It was confirmed that silicotungstic acid modified catalyst (Ni 3 Co-MOF-LS@HSiW) exhibited the best catalytic performance, while the highest conversion of HMF was up to 100%, with the best MFA yield of 86.5%. The finding in this study could provide novel insights for the utilization of lignin and preparation of value-added biomass-derived chemicals.
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AICHE JOURNAL
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2024
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IF 3.5
Xin Zhao,Linghan Xiao,Fengliang Wang,Zirong Shen,Ruiqi Fang,Yingwei Li
Herein, we report a controllable and versatile strategy for the synthesis of highly dispersed Co nanoparticles embedded in open-channel hierarchically porous N/O-doped carbon skeleton. Moreover, the pore sizes of the hierarchical structures can be easily tuned by adjusting the size of precursors. The as-obtained Co@NC-2ST exhibits unprecedented activity and selectivity in the oxidative esterification of 5-hydroxymethylfurfural (HMF) to dimethyl furan-2,5-dicarboxylate under base-free and atmospheric conditions. In particular, the achieved turnover frequency value is an order of magnitude higher than that of the state-of-art heterogeneous catalysts reported to date. A combination of experimental and density function theory studies reveals that the unique features of Co@NC-2ST enable a novel reaction route, that is, the CHO group of HMF is preferentially esterified instead of the OH group. This can be attributed to the nucleophilic addition reaction caused by the attack of methoxy anion on the CHO group of HMF.
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FOOD CHEMISTRY
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2024
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IF 8.5
Teng Liu,Yumin Niu,Kexin Cheng,Qichao Fei,Dengyong Liu
The present study aimed to elucidate the pathway of pigment formation and identify the source of antioxidant activity during sugar smoking. Building upon previous research, this investigation replicated the sucrose cleavage process involved in sugar-smoking through model reactions to obtain distinct model reaction products. The products were analyzed using various techniques such as ultraviolet–visible spectrometry, Fourier-transform infrared spectroscopy, high-performance liquid chromatography, and high-performance liquid chromatography-tandem mass spectrometry. The findings revealed that the pyrolysis of sucrose at 330 °C yielded glucose and fructose, with fructose pyrolysis producing significantly more 5-HMF than glucose. Moreover, the antioxidant capacity of 5-HMF was found to make a substantial contribution. The primary source of 5-HMF was identified as fructose resulting from the cleavage of sucrose at 330 °C, while the primary pathway for the formation of the sugar-smoking pigment 5-GGMF was attributed to the intermolecular dehydration of 5-HMF and glucose at 150 °C.
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JOURNAL OF SOLID STATE CHEMISTRY
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2024
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IF 3.2
Feng Ye,Shuanshi Fan,Xuemei Lang,Yanhong Wang,Yihui Lv,Gang Li
Developing hierarchical zeolites is highly important for catalytic applications. In this study, micro- and submicron-sized hierarchical ZSM-5 zeolites, composed of aggregated nanosized ZSM-5 crystals, were facilely synthesized without any mesoporogen. The effects of the gel composition in a mesoporogen-free system on the formation of ZSM-5 aggregates were studied. The results revealed that the Na 2 O/SiO 2 molar ratio and the aluminum source exerted significant impacts. Furthermore, we demonstrated that the morphology and size of the ZSM-5 aggregate could be easily adjusted by varying the gel composition. Mechanistic insights indicated that the formation of hierarchical ZSM-5 aggregates in the mesoporogen-free system likely followed a space-confined growth mechanism.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Yan Chen,Ming-Kun Yang,Shan-Xin Li,Suo-Luan Zhou,Cheng-Nuo Hu,Yun-Han Yang,Li-Juan Yang
Developing efficient and recyclable iodine adsorbents is crucial for addressing radioactive iodine pollution. An imidazole cation-bridged pillar[5]arene polymer (P5–P5I) was synthesized via a salt formation reaction. P5–P5I exhibited a high iodine vapor capture capacity of 2130.0 mg/g and a maximum adsorption capacity of 1935.3 and 942.4 mg/g for I2 and I3– in solution, respectively. The adsorption kinetics of I2 and I3– on P5–P5I in aqueous solution followed a pseudo-second-order kinetic model, reaching adsorption equilibrium within a few minutes. P5–P5I demonstrated the ability to selectively capture I2 and I3– in the presence of competing anions (10–1000-fold), removing over 97.1% of iodine from various environments. Meanwhile, under extreme conditions (strong acids, strong bases, and high temperature), P5–P5I still has a superior adsorption performance and cycling ability for I2 and I3–. Molecular modeling revealed that P5–P5I could synergistically enhance iodine capture through multiple weak interactions, including host–guest, C–H···I hydrogen bond, and electrostatic interactions. This study indicates that P5–P5I has promising applications for rapid and efficient iodine uptake from vapor and various aqueous media.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Kanglu chang,Xiaowen kong,Yining Zhang,Xumei Tao,Liang Huang
Photo-assisted thermo-catalytic conversion of glucose to 5-hydroxymethylfurfural (HMF) is one of the most promising ways for channeling solar energy. Photo-assisted thermo-catalytic conversion of glucose and HMF yield were improved with SnO 2 /Cr-MOFs/Cr(OH) 3 catalysts under visible light irradiation at 135 ℃-165 ℃ nitrogen atmosphere. SnO 2 /Cr-MOFs/Cr(OH) 3 afforded relatively high Lewis acidity and Brønsted acidity, which was beneficial for thermo-catalytic conversion of glucose. The light and the interface between SnO 2 and Cr-MOFs/Cr(OH) 3 assistantly promoted the HMF formation. The photo-generated holes (h + ) under light irradiation was the driving force for the formation of “free” protons from water and carboxylic acid in Cr-MOFs, which acted as Brønsted acid sites to promote HMF formation. With 576 mg glucose as the substrate and DMSO as the solvent, 92 % glucose conversion with 43.2 % HMF yield was achieved at 150 ℃ for 2 h under nitrogen atmosphere and 500 W Xe lamp irradiation. The results demonstrate the promise of photo-assisted thermo-catalytic conversion of glucose in the future.
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ChemNanoMat
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2024
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IF 2.6
Delong Yang,Ziting Du,Jinhang Dai,Qingya Cao,Zhaobao Xiang,Gang Chen,Fukun Li
Here, a series of nitrogen-doped carbon (NC) supported transition metal oxide catalysts were prepared by pyrolysis of chitosan-metal salt mixtures for the efficient synthesis 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) and fructose. Among them, supported molybdenum-based species on nitrogen-doped carbon (Mo/NC) exhibited excellent activity and selectivity for selective oxidation of HMF to DFF. The presence of nitrogen species reduces the electron cloud density around the Mo species, thereby improving the catalytic activity. Moreover, the interaction between active MoO2 species on the catalyst surface and NC ensured the stability of the catalyst, resulting in no significant loss of activity after four catalytic cycles. 99.5% and 55.1% yields of DFF with full conversion were obtained from HMF and fructose respectively over Mo/NC-chitosan-600 in DMSO under ambient air. In order to enhance DFF yield from fructose, sulfonate groups were introduced into Mo/NC-chitosan-600 catalyst, leading to the highest DFF yield of 70.2%. In addition, this catalyst also allowed 10.0%, 22.9% and 33.3% DFF yields from glucose, sucrose and inulin, respectively.
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