GREEN CHEMISTRY
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2023
·
IF 9.8
Guangxu Yang,Zhenggang Gong,Bei Zhou,Xiaolin Luo,Jing Liu,Guanben Du,Chengke Zhao,Li Shuai
Lignin is a phenolic polymer, making it a sustainable alternative to phenol for synthesizing lignin–phenol–formaldehyde (LPF) adhesives. However, technical lignins produced in pulping or biorefining processes are generally highly condensed and have low reactivity, limiting their uses in synthesizing phenolic-based adhesives. Herein, we report a two-step strategy to produce lignin-based wood adhesives with industrially available technical lignins through hydrodeoxygenation followed by acid-mediated methylolation of aromatic C2/6 positions to improve the flowability, water resistance, and crosslinking ability of lignins. We demonstrated that this biobased lignin–formaldehyde adhesive had a lighter color and far better adhesion performance compared to traditional LPF resins prepared from base-mediated methylolation of lignins. Mechanistic investigation suggests that the chemical crosslinking of methylolated lignin to form diarylmethane structures and the physical interlocking interaction at the interfaces of wood veneers contribute to the strength of plywood.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Yanjun Chen,Jie Dai,Xin Shen,Junqiang Shan,Yulian Cao,Tianpeng Chen,Hanjie Ying,Chenjie Zhu,Ming Li
PBAT composites with biomass fillers have gained considerable attention as alternatives to non-biodegradable plastics. This work employed xylan derivatives as fillers for PBAT composites. Xylan was modified by introducing cinnamoyl side groups which limit the hydrogen bonding and construct π-π stacking interactions with PBAT chains. The resultant xylan cinnamates (XCi) show degree of substitution (DS) of 0.55–1.89, glass-transition temperatures ( T g ) of 146.5–175.0 °C and increased hydrophobicity , which can be simply controlled by varying the molar ratio of reactants. NMR results demonstrate that the C3-OH of xylopyranosyl unit is more accessible to cinnamoylation. XCi fillers (30–50 wt%) were incorporated into PBAT through melt compounding. The filler with a DS of 0.97 exhibited the optimal reinforcing effect, showing superior tensile strength (19.4 MPa) and elongation at break (330.9 %) at a high filling content (40 wt%), which is even beyond the neat PBAT. SEM and molecular dynamics simulation suggest improved compatibility and strengthened molecular interaction between XCi and PBAT, which explains the suppressed melting/crystallization behavior, the substantial increase in T g (−34.5 → −1.8 °C) and the superior mechanical properties of the composites. This research provides valuable insights into the preparation of high-performance composites by designing the molecular architecture of xylan and optimizing the associated interactions.
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Frontiers of Optoelectronics
·
2023
·Vol. 16
·期 1
·1-10
·
IF 5.4
Zhao Xinzhao,Li Mingyu,Ma Tianjun,Yan Jun,Khalaf Gomaa Mohamed Gomaa,Chen Chao,Hsu Hsien-Yi,Song Haisheng,Tang Jiang
Infrared solar cells are more effective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region, thus also at broadening the absorption spectra and improving power conversion efficiency. PbS colloidal quantum dots (QDs) with tunable bandgap are ideal infrared photovoltaic materials. However, QD solar cell production suffers from small-area-based spin-coating fabrication methods and unstable QD ink. Herein, the QD ink stability mechanism was fully investigated according to Lewis acid–base theory and colloid stability theory. We further studied a mixed solvent system using dimethylformamide and butylamine, compatible with the scalable manufacture of method-blade coating. Based on the ink system, 100 cm 2 of uniform and dense near-infrared PbS QDs (~ 0.96 eV) film was successfully prepared by blade coating. The average efficiencies of above absorber-based devices reached 11.14% under AM1.5G illumination, and the 800 nm-filtered efficiency achieved 4.28%. Both were the top values among blade coating method based devices. The newly developed ink showed excellent stability, and the device performance based on the ink stored for 7 h was similar to that of fresh ink. The matched solvent system for stable PbS QD ink represents a crucial step toward large area blade coating photoelectric devices. Graphical Abstract
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STRUCTURE
·
2023
·
IF 5.7
Jin Dong,Han Xiao,Jia-Nan Chen,Bai-Feng Zheng,Yu-Ling Xu,Meng-Xi Chen,Wen-Chao Yang,Hong-Yan Lin,Guang-Fu Yang
4-Hydroxyphenylpyruvate dioxygenase (HPPD) has attracted increasing attention as a target for treating type I tyrosinemia and other diseases with defects in tyrosine catabolism. Only one commercial drug, 2-(2-nitro-4-trifluoromethylbenzoyl)-1, 3-cyclohexanedione (NTBC), clinically treat type I tyrosinemia, but show some severe side effects in clinical application. Here, we determined the structure of human HPPD-NTBC complex, and developed new pyrazole-benzothiadiazole 2,2-dioxide hybrids from the binding of NTBC. These compounds showed improved inhibition against human HPPD, among which compound a10 was the most active candidate. The Absorption Distribution Metabolism Excretion Toxicity (ADMET) predicted properties suggested that a10 had good druggability, and was with lower toxicity than NTBC. The structure comparison between inhibitor-bound and ligand-free form human HPPD showed a large conformational change of the C-terminal helix. Furthermore, the loop 1 and α7 helix were found adopting different conformations to assist the gating of the cavity, which explains the gating mechanism of human HPPD.
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FUEL
·
2023
·
IF 7.4
Meiyu Liu,Xinyu Sun,Yiming Zhang,Ye Yang,Yucai Qin,Binbin He,Yi Mei,Yun Zu
Propane dehydrogenation (PDH) is one of the most effective methods for intentional (“on-purpose”) propylene production. Isolated Sn sites on open supports exhibit considerable PDH performance comparable to that of industrial Pt- and Cr-based catalysts, but the loss of Sn is inevitable. Herein, highly dispersed and stable NiSn subnanoclusters encapsulated within the channels of silicalite-1 zeolite are fabricated through a one-step hydrothermal synthesis in this work. The as-prepared Ni 1 Sn 1 @S-1 zeolite catalyst exhibits outstanding PDH performance with considerable propylene formation rate (ca. 12.3 mmol∙g cat -1 ∙h −1 ) and high propylene selectivity (>88 %). Most significantly, no Sn loss is detected after three regeneration cycles. Structural elucidation of NiSn sites on catalysts, by HRTEM, H 2 -TPR, FTIR and XPS characterizations confirms that the Ni sites embedded in the geminal silanols of zeolitic framework play a vital role in anchoring Sn species and preventing the active sites from losing and sintering. The cooperative action of robust NiSn subnanoclusters is conducive to the selective C–H activation and the propylene desorption. A plausible dehydrogenation mechanism is revealed by in situ infrared spectroscopy. This study on siliceous zeolite confined NiSn catalysts delivers an insight into the nature of selective and stable NiSn sites involved in the PDH reaction.
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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2023
·
IF 3.4
Taixiang Gao,Hongxiong Zhang,Qinqing Li,Feng Zhao,Nan Wang,Wenbin He,Junlong Zhang,Rui Wang
Fuzi decoction (FZD) is clinically used to treat chronic heart failure (CHF) in China, but the mechanism underlying FZD treatment in CHF remains unclear. Here, we investigated the potential mechanism underlying FZD treatment of CHF in rats. First, the compounds in FZD-containing serum of rats were identified, and 16 S rRNA sequencing and GC–MS-based untargeted metabolomics analysis were then performed. The levels of fecal short-chain fatty acids (SCFAs) were determined and compared, and fecal microbiota transplantation (FMT) was used to verify the role of the gut microbiota . Our results identified 27 in FD-containing serum. FZD increased the Firmicutes -to- Bacteroidetes ratio and the Lactobacillus abundance and affected the β diversity of the gut microbiota in rats with CHF. Differential species analysis showed that Lactobacillus and Prevotella were biomarkers of FZD treatment of CHF. Untargeted metabolomics analysis revealed that FZD affected valine , leucine and isoleucine biosynthesis; galactose metabolism; and aminoacyl-tRNA biosynthesis in rats with CHF. Furthermore, FZD significantly increased the acetic acid, propionic acid , butyric acid and isopentanoic acid levels in the feces of rats with CHF. Correlation analysis showed that the butyric acid and Lactobacillus levels had the strongest correlation in the control, sham and high-dose FZD (HFZD) groups, and many microbiota components were closely related to differentially abundant metabolites. FMT revealed that the fecal microbiota obtained from the HFZD group changed the heart rate; the brain natriuretic peptide (BNP), acetic acid, propionic acid, butyric acid, and metabolite levels; and the gut microbiota in rats with CHF. In summary, our study revealed that the mechanism of action of FZD in CHF treatment may be related to improvements in the gut microbiota, elevations in the SCFA content and the regulation of valine, leucine, and isoleucine biosynthesis; galactose metabolism; and other metabolic pathways.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Youfang Huang,Yueyue Zhang,Yilin Yu,Xiaochong Song,Xiaojia Huang
Specific capture is a beneficial tactic in simultaneous monitoring of sulfonamides (SAs) and quinolones (QLs). For this purpose, a new magnetic molecularly imprinted adsorbent based on double-template molecules (DT-MIP@MNA) was facilely prepared by “one-pot” hydrothermal technique and utilized as the adsorbent of magnetic solid-phase extraction (MSPE). Molecular simulation technique was employed to quickly screen functional monomer. The recognition factors of prepared adsorbent towards templates sulfamethazine and nalidixic acid were 5.89 and 2.90, respectively, and the corresponding adsorption capacities were as high as 8.85 mg/g and 8.97 mg/g, respectively. Under the optimized parameters, the proposed DT-MIP@MNA/MSPE was combined with HPLC to simultaneously and selectively monitor trace SAs and QLs residuals in water and milk samples. The achieved limits of detection were 0.012–0.028 μg/L and 0.015–0.032 μg/kg for water and milk samples, respectively. The current supplied a sensitive, reliable and anti-interference method for simultaneously monitoring trace SAs and QLs in food.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 18
·13695
·
IF 5.6
Jia Sun,Zuying Zhou,Yang Zhou,Ting Liu,Yueting Li,Zipeng Gong,Yang Jin,Lin Zheng,Yong Huang
The purpose of this study was to elucidate the metabolic action patterns ofP. forrestiiagainst rheumatoid arthritis (RA) using metabolomics, and to obtain its potential effective substances for treating RA. First, the therapeutic effects ofP. forrestiiagainst RA were confirmed; second, the chemical composition ofP. forrestiiwas analyzed, and 17 prototypes were absorbed into blood; subsequently, plasma metabolomics studies using UPLC-Triple-TOF-MS/MS and GC-MS were performed to disclose the metabolomics alterations in groups, which revealed 38 altered metabolites after drug intervention. These metabolites were all associated with the arthritis pathophysiology process (−log(p) > 1.6). Among them, sorted by variable important in projection (VIP), the metabolites affected (VIP ≥ 1.72) belonged to lipid metabolites. Finally, Pearson’s analysis between endogenous metabolites and exogenous compounds was conducted to obtain potential pharmacological substances for theP. forrestiitreatment of RA, which showed a high correlation between five blood-absorbed components andP. forrestii-regulated metabolites. This information provides a basis for the selection of metabolic action modes forP. forrestiiclinical application dosage, and potential pharmacological substances that exerted anti-RA effects ofP. forrestiiwere discovered. The study provided an experimental basis for further research on pharmacoequivalence, molecular mechanism validation, and even the development of new dosage forms in the future.Keywords:Periploca forrestiiSchltr.;rheumatoid arthritis;network pharmacology;metabolomics;pharmacodynamic substances
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Hua Huang,Jinqiang Yan,Huaxue Yan,Biao Jiang
Surface wax crystals play important roles in protecting plants from pest and disease invasions, and UV irradiation. The wax crystals are less probed individually from the fruit surfaces. Herein the morphologies, chemicals and an efficient method to sample the wax blooms of white wax gourd were addressed. Various crystalloids such as rodlets, platelets, fragments, and granules were observed, which stacked as fine wax film covering on wax gourd fruit surface. The wax blooms were effectively removed by cryo-adhesive after consecutive manipulating set by a high-end device with cylinders. Wax crystals were dominated by triterpenols and triterpenol acetates over 61 % of total crystals, followed by vey-long-chain aliphatics. Accordingly, the high-end device with cryo-adhesive provides an efficient approach to selectively probe the wax crystals from those fruits covering wax blooms. The elucidation of morphologies and chemical compositions of wax crystals may help to better understand their regulations on fruit quality traits.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Ziwei Guo,Huan He,Kunqian Liu,Shicheng Yang,Zihui Li,Chaochao Lai,Zhicheng Liao,Xiaomin Ren,Bin Huang,Xuejun Pan
Insights into COVID-19 antivirals’ environmental fate and ecological risk are urgently required due to their increasing concentrations in aquatic environments, which have rarely been studied. Herein, we first investigated the photochemical transformation and the resulting alterations in toxicity of arbidol, an antiviral drug with relatively higher toxicity. The photolysis of arbidol was rapid with a rate constant of 0.106 min −1 due to its superior ultraviolet light absorption , in which the direct photolysis was predominated with a contribution of 91.5%. Despite its substantial photolysis, only 14.45% of arbidol was mineralized after 100 min, implying that arbidol and its products might have a long-term impact on aquatic environment. It was inferred that arbidol was photolyzed mainly via the loss of thiophenol, bromine, and alkylamine, based on twelve photolytic products identified. Notably, the experimental results demonstrated that the photolysis process increased the acute toxicity of arbidol, and the toxicity prediction indicated that the ecotoxicity of two photolytic products was very high with LC 50 values below 0.1 mg/L. Due to the co-effect of multiple constituents, the photolytic rate observed in wastewater treatment plant effluent and in river water was comparable to that in ultra-pure water, while it was slightly enhanced in lake water. The presence of dissolved organic matter suppressed arbidol photolysis, while NO 3 − exhibited a promotion effect. These results would be of great significance to assess the fate and risk of COVID-19 antivirals in natural aquatic environments.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Weiting Yu,Dezheng Yang,Rendan Zhu,Luzhen Liu,Yan Yu,Juntao Tang,Zhiqiao He,Jiexu Ye,Shuang Song
The photoassisted electrochemical CO2 reduction reaction (CO2RR) toward CO is considered one of the most promising routes of CO2 utilization. In this work, 2,6-diaminopyridine (2,6-DAP) with both the pyridine ring and the –NH2 functional group is utilized for the first time to functionalize the surface of the electrode. The p-Si/Ag/2,6-DAP electrode has been identified as a good catalyst with relatively high activity and CO selectivity at a low overpotential as well as good stability. The Faradaic efficiency of CO is 84.56% at an optimized potential of −0.9 V vs reversible hydrogen electrode (RHE). A synergistic mechanism has been proposed for the enhanced catalytic performance of p-Si/Ag/2,6-DAP in the CO2RR. Ag facilitates the reduction of CO2 to produce CO. 2,6-DAP helps CO2 adsorption and inhibits the competitive hydrogen evolution reaction accompanying the CO2RR under low potentials.
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JOURNAL OF POLYMER SCIENCE
·
2023
·Vol. 61
·期 24
·3276-3287
·
IF 3.4
Jinglei Xing,Ge Zhu,Xingzhong Fang,Guofei Chen
To meet the needs of high heat-resistant and colorless polyimide (CPI) films, a series of poly(amide-imide) (PAI) films were synthesized by copolymerization of 1,2,3,4-cyclobutanetetracarboxylic dianhydride (CBDA), terephthaloyl chloride (TPC), 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) and 2,2′-bis(trifluoromethyl)benzidine (TFDB) with the addition of lithium chloride (LiCl) for ionic coordination. The coordination of Li cations with carbonyl groups significantly reduced the coefficient of thermal expansion (CTE) and improved the mechanical properties. Moreover, by adjusting the ratio of CBDA and TPC, all PAI films exhibited high glass transition temperature ( T g ), low CTE and high transparency. Among these PAI films, PAI-6-2Li exhibited excellent comprehensive performance with a high T g of 363 °C, low CTE of 6.4 ppm/K, high transmittance of 84% at 400 nm and tensile modulus of 7.2 GPa, which was expected to be used in the field of flexible displays. Graphical
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