EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
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2021
·
IF 6.514
Dongdong Luo,Zhikun Guo,Xuecui Zhao,Lijuan Wu,Xiaochun Liu,Yingzhi Zhang,Yuhang Zhang,Zirong Deng,Xianjun Qu,Shuxiang Cui,Shengbiao Wan
Sphingosine-1-phosphate receptor 2 (S1PR2) has been identified as a brand-new GPCR target for designing antagonists to reverse 5-FU resistance. We herein report the structural optimization and structure-activity relationship of JTE-013 derivatives as S1PR2 antagonists. Compound 9d was the most potent S1PR2 antagonist (K D = 34.8 nM) among developed compounds. Here, compound 9d could significantly inhibit the expression of dihydropyrimidine dehydrogenase (DPD) to reverse 5-FU-resistance in HCT116 DPD and SW620/5-FU cells. Further mechanism studies demonstrated that compound 9d not only inhibited S1PR2 but also affected the transcription of S1PR2. In addition, compound 9d also showed acceptable selectivity to normal cells (NCM460). Importantly, compound 9d with suitable pharmacokinetic properties could significantly reverse 5-FU-resistance in the HCT116 DPD and SW620/5-FU xenograft models without obvious toxicity, in which the inhibition rates of 5-FU were increased from 23.97% to 65.29% and 27.23% to 60.81%, respectively. Further immunohistochemistry and western blotting analysis also demonstrated that compound 9d significantly decreases the expression of DPD in tumor and liver tissues. These results indicated that compound 9d is a promising lead compound to reverse 5-FU-resistance for colorectal cancer therapy.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Ruokun Jia,Jiayuan Deng,Xiaohang Yang,Ruisong Xue,Pengpeng Wang,Xingbo Bian,Qiyao Wang
Graphitic carbon nitride (CN) hold great promise as a photocatalyst for generating hydrogen energy via water splitting, owing to its remarkable ability to respond to visible light and its strong reduction capacity. However, the photocatalytic water splitting for H 2 evolution performance of pure CN was impeded by its low surface area, inadequate hydrophilicity, and unsatisfactory photoelectric conversion efficiency. Here we tackled these challenges by synthesizing a series of CN/H-ZSM-5 composites with varying amount of H-ZSM-5 zeolite using a straightforward thermal copolymerization method. The contact angle and N 2 adsorption-desorption measurements confirmed that the incorporated hydrophilic and porous H-ZSM-5 zeolite contribute to increased surface area and improved hydrophilicity of the CN/H-ZSM-5 composites. Meanwhile the resulting CN/H-ZSM-5 composites exhibited significant separation and migration enhancement of photoexcited charge carriers. Consequently, the optimized CN/H-ZSM-5 composite, containing 50 mg of H-ZSM-5 zeolite, demonstrated 13 times increase in photocatalytic H 2 production rate than that of pure CN. This work not only provided a competitively universal approach on the design of high-efficiency CN based photocatalyst, but also clarified the role of H-ZSM-5 zeolite in the H 2 evolution enhancement.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Siyu Ma,Zhihao Wang,Bowen Liu,Xiaolei Wang,Shichao Du,Zichen Song,Xinxin Bian,Manchen Hao,Ju Huang,Zhimin Chen,Zhiyu Ren
Pairing the hydrogen evolution reaction (HER) with the thermodynamics-friendly electrooxidation reaction (EOR) is a powerful way to maximize the energy/economic effectiveness, but still a challenge. Herein, the symbiotic Ni/MoN heterojunction arrays were constructed on foam (Ni/MoN/NF) by the nitridation-induced in situ reduction/conversion strategy. The fascinating interfacial electronic structure and surface reconstruction of Ni/MoN/NF heterojunction are responsible for the enhanced HMF-H 2 O paired electrolysis. Ni/MoN/NF only requires a low overpotential of 53 mV to reach the HER current density of 10 mA cm −2 , as well as the good durability; and NiOOH derived on the anode are electronically activated by MoN to achieving high-efficiency conversion from HMF to FDCA (∼100 % conversion, 97.5 % yield and 97.4 % Faradaic efficiency). For the HMF-H 2 O paired electrolysis, the assembled Ni/MoN/NF||Ni/MoN/NF electrolyzer only requires a low potential of 1.391 V to yield the current density of 10 mA cm −2 , ranking at the forefront in the reported coupling catalysts. Theoretical calculations manifest that the upshift of d -band center of the NiOOH/MoN heterojunction contributes to HMF chemisorption and activation, thereby enhancing its catalytic activity towards HMFEOR. Our study sheds light on the significance of designing the paired electrolysis with low voltage input for renewable energy applications.
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高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Haifeng Tian,Zhiyu Chen,Xing Yang,Peng Gao,Chunxue Jiao,Fei Zha,Yue Chang,Hongshan Chen
A method for the direct synthesis of hierarchical zeolites was developed by converting precursors of zeolites and mesoporous copolymers into homogeneous gels using conventional block copolymers as scaffolds. In this method, hydrothermal synthesis is accomplished on a steam-assisted basis, and the dry gel leaves the system free of the liquid water phase, which successfully avoids phase separation between the soft stencil and the solid silica phase. The catalytic performance of hierarchical zeolites was evaluated on a fixed-bed reactor for the methanol-to-aromatics reaction. The hierarchical structure greatly enhances the catalytic activity of the probe reaction due to the increased outer surface, decreased coke formation, and diffusion resistance in the microporous network. The selectivity of BTX reached 65.8%, and there was no significant deactivation after a reaction of 107 h. The transition state and energy barrier for methanol to aromatics were obtained by the minimum energy search of the LST/QST transition state.
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Advanced Composites and Hybrid Materials
·
2023
·Vol. 6
·期 5
·1-10
·
IF 20.1
Guo Sijia,Ma Min,Ge Ruixiang,Algadi Hassan,Shao Qian
Developing efficient electrocatalysts for biomass electro-oxidation in alkaline seawater is of great significance but remains less explored. Herein, we reported a hierarchical structure consisting of nickel-cobalt layered double hydroxide nanosheets and copper oxide nanowires (CuO@NiCo-LDH), which was favorable for increasing active sites and facilitating electron transfer during 5-hydroxymethylfurfural oxidation (HMFOR). As-designed CuO@NiCo-LDH catalyst achieved a high yield of 2,5-furandicarboxylic acid (FDCA, 89%) and 82% faradaic efficiency (F.E.). It also showed a large current density of 133.4 mA cm −2 at 1.4 V vs. RHE, outperforming most of the previously reported Ni/Co-based HMFOR electrocatalysts. More importantly, it also showed an outstanding HMFOR performance in alkaline seawater, suggesting great promise in practical electrolysis.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
·
IF 5.541
Yang Li,Bin Hu,Salman Raza Naqvi,Zhen-xi Zhang,Kai Li,Qiang Lu
5-Hydroxymethylfurfural (5-HMF) is a value-added platform chemical, which can be obtained from pyrolysis of biomass materials, whereas related investigation on its selective production via catalytic fast pyrolysis (CFP) process is still insufficient. In this work, a zirconium-tin mixed metal oxide (ZrO 2 -SnO 2 ) catalyst was developed for the selective production of 5-HMF from the in-situ CFP of cellulose. According to pyrolysis-chromatography/mass spectrometry (Py-GC/MS) tests, the ZrO 2 -SnO 2 catalyst has better performance on the selective preparation of 5-HMF than single nano oxide ZrO 2 , SnO 2 , or their physical mixture. 5-HMF was sensitive to the reaction conditions, and its yield and selectivity always exhibited the tide of first increasing followed by decreasing along with the increase of Zr loading and catalyst-to-cellulose (CA-to-CL) ratio. At the optimum conditions with ZrO 2 -SnO 2 of 15 wt% Zr loading (ZrO 2 -SnO 2 -15), pyrolysis temperature of 350 °C and CA-to-CL ratio of 2:1, the 5-HMF yield was 6.49 wt%, which was 4 times more than that of the non-catalytic process (1.35 wt%). Correspondingly, the selectivity of 5-HMF was up to 23.50 %. The catalyst characterization combined with the pyrolysis texts of several typical saccharides, including cellobiose, maltose, glucose, and mannose indicated that the ZrO 2 -SnO 2 -15 could promote the breakage of glycosidic bonds with the formation of reducing ends and the selective conversion of the reducing end to 5-HMF due to its mild acidity. Overall, the ZrO 2 -SnO 2 is expected a promising catalyst for the CFP of cellulose to prepare 5-HMF.
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Bioactive Materials
·
2021
·
IF 14.593
Beibei Yang,Yating Dong,Yifeng Shen,Ailin Hou,Guilan Quan,Xin Pan,Chuanbin Wu
Hypertrophic scar (HS) is an undesirable skin abnormality following deep burns or operations. Although intralesional multi-injection with the suspension of triamcinolone acetonide (TA) and 5-fluorouracil (5-Fu) has exhibited great promise to HS treatment in clinical, the difference of metabolic behavior between TA and 5-Fu remarkably compromised the treatment efficacy. Besides, the traditional injection with great pain is highly dependent on the skill of the experts, which results in poor compliance. Herein, a bilayer dissolving microneedle (BMN) containing TA and 5-Fu (TA-5-Fu-BMN) with biphasic release profile was designed for HS therapy. Equipped with several micro-scale needle tips, the BMN could be self-pressed into the HS with uniform drug distribution and less pain. Both in vitro permeation and in vivo HS retention tests revealed that TA and 5-Fu could coexist in the scar tissue for a sufficient time period due to the well-designed biphasic release property. Subsequently, the rabbit ear HS model was established to assess therapeutic efficacy. The histological analysis showed that TA-5-Fu-BMN could significantly reduce abnormal fibroblast proliferation and collagen fiber deposition. It was also found that the value of scar elevation index was ameliorated to a basal level, together with the downregulation of mRNA and protein expression of Collagen I (Col I) and transforming growth factor-β1 (TGF-β1) after application of TA-5-Fu-BMN. In conclusion, the BMN with biphasic release profiles could serve as a potential strategy for HS treatment providing both convenient administrations as well as controlled drug release behavior.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 9
·4236-4245
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IF 3.591
Jia Zhang,Jian Yang,Junying Tian,Hailong Liu,Xuemei Li,Weiguo Fang,Xun Hu,Chungu Xia,Jing Chen,Zhiwei Huang
The synthesis of useful amines from bio-based carbonyl compounds is highly desired owing to their mild reaction conditions and green sustainability. The reductive amination of bio-furfural-derived 2-hydroxytetrahydropyran (2-HTHP) to high-value-added 5-Amino-1-pentanol (5-AP) was carried out over efficient Ni–Al2O3 catalysts prepared by a co-precipitation method. Among the Ni–Al2O3 catalysts with different Ni loadings (0–100 wt%) tested, the 50Ni–Al2O3 catalyst exhibited the highest 5-AP yield of 91.3% under mild conditions of 60 °C and 2 MPa H2. This catalyst also presented good stability during a 150 h time-on-stream without appreciable deactivation. Characterization results showed that the 50Ni–Al2O3 catalyst exhibited small Ni0 nanoparticles (5.5 nm), a high reduction degree (up to 95%), and a large amount of strong Lewis acid sites. The cooperative catalysis of the strong Lewis acid sites and highly dispersed metallic Ni sites is suggested to play an important role in achieving high efficiency in 2-HTHP reductive amination.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zenan Ni,Yuming Li,Yaoyuan Zhang,Yajun Wang,Guoqing Cui,Guiyuan Jiang,Zhen Zhao,Chunming Xu
Ga species with high dehydrogenation capability were prepared by H 2 -O 2 atmosphere treatment, and efficient balance of bifunctionality (dehydrogenation/cracking) was realized between Ga species and ZSM-5 over Ga/ZSM-5 based catalysts. Compared with parent Ga/ZSM-5, the conversion rate of n -butane was increased from 0.53 to 2.59 mmol·g −1 ·min −1 on Ga/ZSM-5 with H 2 -O 2 treatment. Kinetic analysis revealed that the apparent activation energy of n -butane catalytic cracking decreased largely from 141 to 47 kJ·mol −1 , which is attributed to the formation of new interaction between Ga species and ZSM-5 upon such an atmosphere treatment. It was also found Butane-O 2 treatment acted as a similar role with H 2 -O 2 treatment in enhancing the catalytic performance. On this basis, different Ga species were correlated with activity and kinetic data, and the effect of practical reaction atmosphere on Ga species was also investigated.
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Green Energy & Environment
·
2021
·
IF 8.207
Weiyao Yang,Mengchen Fu,Chenyu Yang,Yiwen Zhang,Chun Shen
Despite wide applications of noble metal-based catalysts in 5-hydroxymethylfurfural (HMF) oxidation, promoting the catalytic performance at low loading amounts still remains a significant challenge. Herein, a series of metal oxide modified MO x -Au/TiO 2 (M = Fe, Co, Ni) catalysts with low Au loading amount of 0.5 wt% were synthesized. Addition of transition metal oxides promotes electron transfer and generation of the Au δ − –O v –Ti 3+ interface. A combination study reveals that the dual-active site (Au δ − -O v -Ti 3+ ) governs the catalytic performance of the rate-determining step, namely hydroxyl group oxidation. Au δ − site facilitates chemisorption and activation of O 2 molecules. At the same time, O v -Ti 3+ site acts as the role of “killing two birds with one stone”: enhancing adsorption of both reactants, accelerating the activation and dissociation of H 2 O, and facilitating activation of the adsorbed O 2 . Besides, superoxide radicals instead of base is the active oxygen species during the rate-determining step. On this basis, a FDCA yield of 71.2% was achieved under base-free conditions, complying with the “green chemistry” principle. This work provides a new strategy for the transition metal oxides modification of Au-based catalysts, which would be constructive for the rational design of other heterogeneous catalysts.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7326-7330
·
IF 6.119
Wei Wang,Min Wang
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising and green process, which urgently demands high-performance catalysts. In this work, a nitrogen-modulated NiMoO4 growth on Ni foam (N-NiMoO4/NF) is prepared via the treatment of NiMoO4 in 1% NH3 at 500 °C. Compared with NiMoO4, the nitrogen-modulated NiMoO4 promotes electro-oxidation of HMF to FDCA and exhibits almost 100% HMF conversion, 97% FDCA yield, and 91% faradaic efficiency. N-NiMoO4 has a higher electrochemical surface area and lower charge transfer resistance than NiMoO4, which enhances the activity of the catalyst for electrocatalytic oxidation of HMF to FDCA. This work gives enlightenment on the nitrogen modulation method to tune the activity of electrocatalysts for biomass refineries.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
·
IF 3.171
Yao Zhong,Cuiying Huang,Lijie Li,Qiang Deng,Jun Wang,Zheling Zeng,Shuguang Deng
Developing an efficient and selective catalyst for the dehydration of fructose to 5-hydroxymethylfurfural (HMF) is significant for biomass conversion. Herein, a metal-organic framework (MOF) with acidity and strong hydrophobicity is first reported by the condensation of amino-tagged MOFs with mercapto carboxylic acids and subsequent oxidation. The hydrophobic acidic MOFs possess acid densities ranging from 0.2−1.0 mmol·g −1 , H 2 O contact angles of 114°−125°, and specific surface areas above 260 m 2 ·g −1 . Compared to the methyl sulfo-functionalized MOF, the benzene sulfo-functionalized MOF with a strong hydrophobicity shows much higher activity and selectivity for the conversion of fructose to 5-hydroxymethylfurfural. In particular, 2.99% (mass) UiO-PhSO 3 H shows the best catalytic performance with a 90.4% HMF yield due to its suitable hydrophobicity and abundant acidic sites. Moreover, the catalyst shows great stability after recycling for 5 runs. This work provides an interesting design strategy for the preparation of hydrophobic acidic MOFs and shows the powerful synergistic effect of acidity and hydrophobicity.
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