Applications in Energy and Combustion Science
·
2021
·
IF 0
Huiyan Zhang,Bingbing Luo,Kai Wu,Han Wu,Jiajun Yu,Siyu Wang
Catalytic fast pyrolysis of lignin is easy to cause agglomeration and coking, resulting in low-yield aromatic hydrocarbons. Catalytic pyrolysis of modified lignin combined with metal-modified HZSM-5 was proposed to enhance the aromatic yield. The experiment results showed that chemical modification with Ca(OH) 2 not only inhibited the agglomeration behavior of lignin but also increased the yield of light phenolic compounds. Moreover, Ca 2+ -loaded lignin combined with metal-modified HZSM-5 was conducive to the formation of aromatics. The total yield of aromatics from the catalytic fast pyrolysis of Ca 2+ -loaded lignin over Zn/HZSM-5 was improved from 31.1 to 46.1 mg/g. The mechanism insight showed that Ca 2+ modification realized the chemical combination between Ca 2+ and the functional groups which are responsible for the agglomeration of lignin, and then the introduction of the Zn species suppressed the hydrogen transfer reaction and enhanced the dehydrogenation pathway, resulting in the increase of aromatic yield.
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DOI
Sensors & Diagnostics
·
2023
·Vol. 2
·期 2
·427-437
·
IF 0
Xiangfei Zheng,Dongmiao Qin,Shenglan Hu,Weiming Mo,Biyang Deng
Tin oxide nanoflowers (SnO2NFs) are used as both an electrochemiluminescent (ECL) signal generator and a carrier of nanomaterials due to the advantages of excellent electrical conductivity, large specific surface area, and good optical properties. AuNPs/PEI-SnO2NFs provide a larger binding site for the immobilization of secondary antibodies (CA12-5-Ab2). The synthesized Ag@ZnONS composite with a large specific surface area and good biocompatibility was applied to immobilize more primary antibodies (CA12-5-Ab1), which further enhanced the ECL signal and obviously improved the sensitivity and selectivity of the immunosensor. A novel signal amplification ECL immunosensor for detecting carbohydrate antigen 12-5 (CA12-5) was fabricated with AuNPs/PEI-SnO2NFs as a signal probe and Ag@ZnONSs as the sensing matrix. The ECL intensity was linearly related to the logarithm of the CA12-5 concentration in the range from 1 × 10−5 to 50 ng mL−1 under optimized conditions. The limit of detection was 2.6 fg mL−1 (S/N = 3). The assay had good operational stability, specificity, and high sensitivity. The study was applied to analyze the CA12-5 level in human serum with satisfactory results, which could be applied in clinical immunoassays.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 9
·2487-2495
·
IF 3.709
Yutong Li,Bajin Chen,Shengpeng Wang,Meichao Li,Chunmei Li,Zhenlu Shen
BACKGROUND On the way to convert biomass-derived products as a renewable and environment-friendly source to high-value added chemicals, one great challenge is the effective control of selectivity in the reaction. Here, we contribute a heterogeneous catalysis method for selective transformation of biomass-based 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) via multicomponent bismuth molybdate catalyst. The influence of the different pH value on the catalytic activity of the catalyst were investigated. In addition, to evaluate the catalytic performance of the catalyst in the selective oxidation of HMF, a variety of important reaction parameters such as the reaction temperature, catalyst amount, atmosphere, and solvent were examined. RESULTS The catalyst prepared with pH value in the range of 1–2 exhibits the optimal catalytic activity in the selective aerobic oxidation of the hydroxy group of HMF. As a result, the target compound of DFF could be obtained with excellent yield (99%) and high selectivity (> 99%) in the presence of 0.25 mg Co 9 Fe 3 BiMo 12 O 51 (pH = 1–2) in DMSO at 130 °C under O 2 atmosphere. In addition, the catalyst Co 9 Fe 3 BiMo 12 O 51 could be reused several times without a significant loss of its catalytic activity. CONCLUSION In this work, a heterogeneous catalytic approach to oxidizing HMF to DFF using Co 9 Fe 3 BiMo 12 O 51 as catalyst and molecular oxygen as oxidant was established. The O 2 temperature-programmed desorption (O 2 -TPD) characterization indicated that the pH value of co-precipitation obviously affected the oxygen mobility and storage capacities in the catalysts, which is related to the catalytic performance in the selective aerobic oxidation. © 2022 Society of Chemical Industry (SCI).
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高影响因子
SOLID STATE SCIENCES
·
2016
·
IF 2.041
Haoliang Xue,Zhuangzhang He,Yun Zhao,Qingze Jiao,Qin Wu,Hansheng Li
ZSM-5/KIT-1 composites were synthesized using an ionic liquid as a template. The structures and morphologies of as-obtained products were characterized using an infrared spectroscopy, X-ray diffractometer, N 2 adsorption/desorption, scanning electron microscopy and transmission electron microscopy . The resultant zeolites show a fully crystalline microporous MFI zeolite framework and a three-dimensional network of short worm-like channels. Mesopores and microspores of 4.2 and 0.8 nm in diameter coexist in the zeolite composites. Moreover, the ratio of ZSM-5 and KIT-1 could be simply adjusted by controlling the pre-crystalline time. We believe that the strategy for fabricating ZSM-5/KIT-1 through a simple method could potentially promote the large-scale production of zeolite composites.
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高影响因子
ENERGY & FUELS
·
2016
·
IF 2.835
Fan Wang,Liang Jiang,Junmei Wang,Zehui Zhang
In this study, the mesporous SBA-15 was prepared and used to graft biimidazole groups, which were used to anchor Ru3+ to give rise to a new ruthenium catalyst (SBA-15-Biimidazole-Ru). The structure of the SBA-15-Biimidazole-Ru catalyst was well characterized and used for the aerobic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF). Several important parameters were studied and found that the reaction solvent and oxygen pressure showed a crucial role in the activity of the as-prepared SBA-15-Biimidazole-Ru catalyst. HMF conversion of 96.9% and DFF yield of 88.7% were achieved after 11 h at 110 °C under 15 bar oxygen pressure. One important characteristic of the SBA-15-Biimidazole-Ru catalyst is that it was very stable without loss of its catalytic activity during the recycling experiments, which was due to the strong interaction between the Ru3+ and the Biimidazole groups on the surface of SBA-15. Finally, the direct conversion of fructose into DFF was also performed by the use of Amberlyst 15 and SBA-15-Biimidazole-Ru as two binary catalysts. The dehydration of fructose over Amberlyst 15 catalyst and the subsequent oxidation of HMF over SBA-15-Biimidazole-Ru catalyst afforded DFF with an overall yield of 72.4%.
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高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 6
·1743-1755
·
IF 2.936
Zhou Yi,Yao Tiantian,Tan Yawen,Chen Yongbo,Chen Zhiyue,Zhang Jin
In this study, a novel composite DUT-5/Bi 2 MoO 6 (DUT-5/BMO) photocatalytic material was prepared by two-step hydrothermal method for the first time. The materials were characterized by SEM, XPS, etc. Studies have shown that material with a new n–n heterojunction structure can quickly degrade tetracycline. DUT-5 was embedded between the Bi 2 MoO 6 nanosheets, which promotes the photogenerated electrons from DUT-5 flows to Bi 2 MoO 6 , thereby reducing the recombination rate of photo-generated electron–hole pairs. The BET results show that the composite material has a larger specific surface area than the monomer Bi 2 MoO 6 . It can provide more active sites. After 60 min of visible light irradiation, the photocatalytic degradation efficiency of TC with 15% DUT-5/BMO reached 84.22%, which is 5.37 and 2.12 times higher than that of pure DUT-5 and Bi 2 MoO 6 , ·O 2 − and h + were the main active substances in the photocatalysis process. In addition, DUT-5/BMO composites show excellent stability and recyclability in 5 times cyclic experiments. In conclusion, DUT-5/BMO has good stability in the environment, and can be used for environmental remediation without pollution. Graphical
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高影响因子
Research
·
2021
·
IF 0
Zhuanghe Ren,Xin Zhang,Hai-Wen Li,Zhenguo Huang,Jianjiang Hu,Mingxia Gao,Hongge Pan,Yongfeng Liu
Sodium alanate (NaAlH 4 ) with 5.6 wt% of hydrogen capacity suffers seriously from the sluggish kinetics for reversible hydrogen storage. Ti-based dopants such as TiCl 4 , TiCl 3 , TiF 3 , and TiO 2 are prominent in enhancing the dehydrogenation kinetics and hence reducing the operation temperature. The tradeoff, however, is a considerable decrease of the reversible hydrogen capacity, which largely lowers the practical value of NaAlH 4 . Here, we successfully synthesized a new Ti-dopant, i.e., TiH 2 as nanoplates with ~50 nm in lateral size and ~15 nm in thickness by an ultrasound-driven metathesis reaction between TiCl 4 and LiH in THF with graphene as supports (denoted as NP-TiH 2 @G). Doping of 7 wt% NP-TiH 2 @G enables a full dehydrogenation of NaAlH 4 at 80°C and rehydrogenation at 30°C under 100 atm H 2 with a reversible hydrogen capacity of 5 wt%, superior to all literature results reported so far. This indicates that nanostructured TiH 2 is much more effective than Ti-dopants in improving the hydrogen storage performance of NaAlH 4 . Our finding not only pushes the practical application of NaAlH 4 forward greatly but also opens up new opportunities to tailor the kinetics with the minimal capacity loss.
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MOLECULES
·
2025
·Vol. 30
·期 7
·1643
·
IF 4.6
Dongmei Gao,Lele Shi,Yuhang Huang,Yingmei Lv,Xuan Yang,Zhenting Du
The thiazole heterocycle is one of the most common moieties found in various drugs. Using 2-aminothiazole as the core structure, the amino group was functionalized with an amide. As a result, 30 trisubstituted 2-amino-4, 5-diarylthiazole derivatives were synthesized, with different substitutions introduced at the C2, C4, and C5 positions. The anti-Candida albicansbiological activities of these synthetic compounds on five kinds ofCandida albicansat different concentrations were detected by the microdilution method. In the first round, four derivatives of 2-amino-4, 5-diarylthiazole exhibited moderate anti-Candida albicansactivity. Among them,4a8was chosen to be subjected to a demethylation process. Thus,5a8was synthesized successfully, giving anti-Candida albicansactivity (MIC80= 9 μM) similar to that of a typical antifungal drug, fluconazole. To understand the mechanism of anti-Candida albicans, molecular docking of the most active5a8against four target proteins of anti-Candida albicans,such as glutamine-fructose-6-phosphoamidamitransferase (GFAT), protein kinase (Yck2), heat-shock protein 90 (Hsp90), and lanosterol 14a-demethylase (CYP51) was carried out. Our research will provide an experimental basis and theoretical guidance for the further design of a new aminothiazole-leading pharmaceutical molecule.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yixuan Wang,Shijia Fu,Yao Zeng,Siwen Jiao,Guihong Chai,Yuehong Xu
5-aminolevulinic acid photodynamic therapy (ALA-PDT) is an emerging therapeutic strategy for skin cancer due to its noninvasiveness and high spatiotemporal selectivity. However, poor skin penetration, poor intratumoral delivery, the instability of aqueous ALA, and the tumor’s inherent hypoxia microenvironment are major hurdles hindering the efficacy of ALA-PDT. Herein, we aim to address these challenges by using microneedles (MNs) to assist in delivering nanoparticles based on natural polymeric tea polyphenols (TP NPs) to self-assemble and load ALA (ALA@TP NPs). The TP NPs specifically increase cellular uptake of ALA by A375 and A431 cells and reduce mitochondrial membrane potential. Subsequently, the photosensitizer protoporphyrin IX derived from ALA accumulates in the tumor cells in a dose-dependent manner with TP NPs, generating reactive oxygen species to promote apoptosis and necrosis of A375 and A431 cells. Interestingly, TP NPs can ameliorate the tumor’s inherent hypoxia microenvironment and rapid oxygen consumption during PDT by inhibiting hypoxia inducible factor-1α, thereby boosting reactive oxygen species (ROS) generation and enhancing ALA-PDT efficacy through a positive feedback loop. After ALA@TP NPs are loaded into MNs to fabricate ALA@TP NPs@MNs, the MNs enhance skin penetration and storage stability of ALA. Importantly, they exhibit remarkable antitumor efficacy in A375-induced melanoma and A431-induced squamous cell carcinoma with a reduced dose of ALA and reverse hypoxia in vivo . This study provides a facile and novel strategy that integrates MNs and green NPs of TP for addressing the bottlenecks of ALA-PDT and enhancing the ALA-PDT efficacy against skin cancers for future clinical translation.
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DOI
PubMed
高影响因子
Microbial Cell Factories
·
2025
·Vol. 24
·期 1
·1-11
·
IF 4.9
Liu Wen,Guo Jing,Lu Wei,Cheng Tao,Li Yiting,Xian Mo,Zhang Rubing
Background L -5-Methyltetrahydrofolate (5-MTHF) is the sole biologically active form of folate present in human blood and serves as an essential nutritional supplement. While microbial biosynthesis of 5-MTHF offers a sustainable alternative to chemical synthesis, its low yield limits industrial potential. Results In this study, strategies for improving the methyl supply combined with engineering the tetrahydrofolate (THF) synthetic pathway were employed in E. coli to increase 5-MTHF production. First, a new exogenous C1 pathway was introduced to improve the intracellular methyl supply through acetyl-CoA breakdown. High expression of key rate-limiting genes folE , folP and purU enhanced metabolic flux of THF pathway, resulting in a 5-MTHF titer of 1.075 mg/L during shake-flask fermentation. A subsequent increase in 5-MTHF production was achieved by knocking out the metE gene, which is involved in the consumption of 5-MTHF. The best engineered strain, M3012, produced 8.2 mg/L 5-MTHF in a 5 L bioreactor via fed-batch fermentation, which presented the highest 5-MTHF titer to date. Conclusion We successfully engineered E. coli by introducing a novel exogenous C1 metabolic pathway to augment the methyl donor pool essential for the biosynthesis of 5-MTHF. Further metabolic optimizations, including the enhancement of the THF precursor flux and the elimination of competing degradation pathways, developed a recombinant strain with significantly increased yield, which paves the way for industrial production of 5-MTHF.
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DOI
PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Yiheng Wu,Yangping Lv,Ruipu Wang,Lixia Bao,Zhongdong Zhang,Dejun Shi,Anlv Zhang,Yaoyuan Zhang,Qi Liu,Qin Wu,Daxin Shi,Kangcheng Chen,Guiyuan Jiang,Hansheng Li
The aromatization of light alkane is an important process for increasing the aromatic production and utilization efficiency of light alkane resources simultaneously. Herein, Ga-modified HZSM-5 catalysts were prepared and investigated by a series of characterization techniques such as X-ray diffraction, nuclear magnetic resonance spectroscopy, transmission electron microscopy, N2 adsorption–desorption, and NH3 temperature-programmed desorption to study their physicochemical properties. The catalytic performance in propane aromatization was also tested. Importantly, the structure–activity relationship, reaction pathway, and coke formation mechanism in propane aromatization were systematically explored. It was found that different Ga introduction methods would affect the amounts of Brønsted and Lewis acid sites, and Ga-HZSM-5 prepared by the hydrothermal method exhibited higher amounts of Brønsted and Lewis acid sites but a lower B/L ratio. As a result, Ga-HZSM-5 showed higher propane conversion and benzene, toluene, and xylene yield compared with that of Ga2O3/HZSM-5. The propane aromatization reaction pathway indicated that propane dehydrogenation to propene was a crucial step for aromatic formation. The increase of the Lewis acid density in Ga-HZSM-5 can effectively improve the dehydrogenation rate and promote the aromatization reaction. Furthermore, the formation of coke species was studied by thermogravimetry–mass spectrometry and Raman approaches, the results of which indicated that the graphitization degree of coke formed over spent Ga-HZSM-5 is lower, resulting in enhanced anticoking stability.
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PubMed
高影响因子
WATER RESEARCH
·
2020
·
IF 9.13
Chen Zhong,He Zhao,Qingzhen Han,Hongbin Cao,Feng Duan,Junyi Shen,Yongbing Xie,Wanqian Guo,Shanshan Sun
As an important raw material and intermediate of widely used antibiotics cefazolin and cefazedone, 2-mecapto-5-methyl-1,3,4-thiadizaole (MMTD) in antibiotic wastewater is hardly decyclized during wastewater treatment, posing great risk to the environment. This work proposed a green “coupling-oxidation” process to enhance ring-opening of MMTD during antibiotic wastewater treatment. In particular, the significant role of humic substances (HS) as pre-coupling reagent was emphasized. Real HS and different model HS, especially quinones, not only efficiently pre-coupled MMTD (>95%) but also promoted the MMTD removal by MnO 2 (from 72.4% to 92.4%). Mass spectrometric analysis indicated that MMTD pre-coupled to HS would be oxidized with ring opening to environmental-friendly sulfonated HS, while direct oxidation of MMTD produced MMTD dimers or sulfonated MMTD that would not undergo ring opening. Theoretical calculations indicated that pre-coupling to HS enabled the ring-opening oxidation by increasing the nucleophilicity and decreasing ring-opening barrier of thiadiazole. Based on the density function theory (DFT), the global nucleophilicity index (Nu) followed the trend of HS-MMTD > MMTD dimer > sulfonated MMTD, while the ring-opening barrier followed the trend of HS-MMTD (274 kJ/mol) < first ring of MMTD dimers (286 kJ/mol) < MMTD (338 kJ/mol). Theoretical calculations further confirmed that the cross-coupled HS-MMTD intermediate was more likely to be decyclized than intermediates from direct oxidation. Moreover, nitrogen, acetaldehyde group, sulfate and CO 2 were the products of thiadiazole ring degradation. Pre-coupling of MMTD with HS provides a new idea and strategy in developing a green and sustainable scheme for wastewater treatment.
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PubMed
高影响因子
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