BIOCHEMICAL PHARMACOLOGY
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2026
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IF 6.5
Yu-Jing Wang,Shuai-Bing Ying,Lin Liu,Qiu-Dan Zhang,Yong Pan,Yu-Qi Hong,Hao-Yang Hu,Yi Liu,Jia-Ni Wei,Zhi-Juan Zhang,Yun-Qing Qiu,Yan Lou
Combretastatin A4 (CA4) is a potent microtubule inhibitor, but its phenolic hydroxyl group is prone to oxidation into toxic quinone products, leading to poor metabolic stability and dose-limiting toxicity that restricts its clinical application. To overcome this limitation, we propose a novel dimer prodrug strategy that covalently links two CA4 molecules via an enzyme-cleavable linker, achieving temporary masking of the phenolic hydroxyl group. The resulting CA4-dimer1 and CA4-dimer2 exhibited potent in vitro antiproliferative activity. Of the two dimers evaluated, CA4-dimer1 demonstrated superior in vitro potency. Crucially, CA4-dimer1 achieved significant tumor suppression rates in patient-derived xenograft (PDX) liver cancer models without notable toxicity. CA4-dimer2 releases active CA4 through gradual hydrolysis but showed slightly lower in vivo release efficiency compared to CA4-dimer1. Flow cytometry and Western blot analysis revealed that this prodrug exerts antitumor activity through the same mechanism as the parent compound CA4. Collectively, the reported CA4-dimer prodrug strategy offers a highly promising approach for treating liver cancer and enhancing the therapeutic index of phenolic drugs, while also providing a potential strategy for structural optimization of drugs containing phenolic hydroxyl groups
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Weichen Wang,Tian Sheng,Shanshuai Chen,Zhiyu Xiang,Fangyuan Zhou,Wanbin Zhu,Hongliang Wang
Designing highly active catalysts for selective hydrodeoxygenation (HDO) of lignin-derived oxygenates into well-defined compounds is of great importance for realizing high-value utilization of lignin. Defect engineering in metal–organic frameworks (MOFs) is an emerging concept for tailoring MOF properties, which might be a promising strategy in the synthesis of high-performance catalysts. Herein, we developed a facile synthetic strategy by adding trifluoroacetic acid as the modulator to prepare a bifunctional catalyst (Pd/NH 2 -MIL-53-d) consisting of Pd nanoparticles highly dispersed on defective NH 2 -MIL-53(Al). Characterizations, including TEM, XRD, IR, XPS and NH 3 -TPD, were employed to reveal the morphology and physicochemical properties of the catalysts. Results indicated that the introduction of defects leads to the generation of coordinatively unsaturated metal sites, which can act as anchor points for high-dispersion of Pd nanoparticles and as additional active acid sites for catalytic reactions. 100% conversion of vanillin and other 8 representative derivates of lignin into their decarbonyl products with yields over 99% has been achieved under mild conditions in the water. Density functional theory calculations revealed that the HDO of vanillin into 2-methoxy-4-methylphenol mainly underwent a cascade of hydrogenation-hydrogenolysis routes, and the synergistic interaction between Pd and defective NH 2 -MIL-53(Al) facilitated the novel bifunctional catalyst to exhibit outstanding catalytic performance. No apparent deactivation of the catalyst was noticed after it was reused 5 times. Therefore, engineering of defects in MOFs holds enormous potential in designing novel bifunctional catalysts for lignin valorization.
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Nano Research
·
2021
·Vol. 14
·期 11
·4347-4355
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IF 8.897
Lu Xiaowen,Guo Chunmu,Zhang Mingyang,Leng Leipeng,Horton J. Hugh,Wu Wei,Li Zhijun
Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added chemicals. Herein, we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31 (SAPO-31) as a highly active, chemoselective, and reusable catalyst for hydrodeoxygenation of vanillin. Characterizations by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, extended X-ray absorption fine structure measurement, and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed, without forming strong palladium-palladium metallic bonding, over the SAPO-31 support. This catalyst, with a full metal availability to the reactants, exhibits exceptional catalytic activity (TOF: 3,000 h −1 , Yield: > 99%) in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol (MMP) under mild conditions (1 atm, 80 °C, 30 min), along with excellent stability, scalability (up to 100-fold), and wide substrate scope. The superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters, as well as the strong metal-support interactions. This work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities.
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ANALYST
·
2021
·Vol. 146
·期 21
·6643-6649
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IF 4.616
Qiaoyan Li,Zhentao Li,Yuanyuan Fu,Igor Clarot,Ariane Boudier,Zilin Chen
Covalent organic frameworks (COFs) are a class of porous materials with high surface area, high porosity, good stability and tunable structure that have been widely used in the separation area. In this work, we have proposed the in situ synthesis of a novel COF composed of 4,4′,4′′-(1,3,5-triazine-2,4,6-triyl)trianiline (Tz) and 1,4-dihydroxyterephthalaldehyde (Da) onto the capillary inner surface for electrochromatographic separation. Fourier transform infrared (FT-IR) spectroscopy, elemental analysis (EA) and scanning electron microscopy (SEM) have facilitated the characterization of the prepared capillary columns. The COF (TzDa) modified OT-CEC column exhibited satisfactory separation selectivity towards neutral compounds (such as chlorobenzenes and alkylbenzenes), acidic and basic compounds (such as phenols and anilines), food additives (vanillin and its analogues) and small biomolecules (such as amino acids and polypeptides). Furthermore, the TzDa modified capillary was quite stable and reproducible. The relative standard deviations for retention times of the test analytes (alkylbenzenes) were as follows: for intra-day (n = 3) runs (≤1.74%), inter-day (n = 3) runs (≤2.25%) and between columns (n = 3) (≤4.83%). This new type of COF-based stationary phase has tremendous potential in separation science.
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Dongdong Wang,Wanbing Gong,Jifang Zhang,Miaomiao Han,Chun Chen,Yunxia Zhang,Guozhong Wang,Haimin Zhang,Huijun Zhao
Catalytic hydrodeoxygenation (HDO) is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels, but highly challenging due to the lack of highly efficient nonprecious metal catalysts. Herein, we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst. The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100% conversion efficiency and selectivity under mild reaction conditions, surpassing the reported high performance nonprecious HDO catalysts. Impressively, our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100% conversion efficiency and over 90% selectivity. Importantly, our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O, and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs . The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Zhijun Li,Xiaowen Lu,Weiwei Sun,Leipeng Leng,Mingyang Zhang,Honghong Li,Lu Bai,Dundong Yuan,J. Hugh Horton,Qian Xu,Jun Wang
The pathway for efficient catalytic hydrodeoxygenation of biomass represents a powerful, yet challenging route for production of value-added liquid fuels. Herein, we describe a one-step synthetic approach to fabricate WO 2.72 decorated with atomically dispersed palladium atoms that bond covalently to the nearby oxygen atoms. The presence of isolated palladium atoms is confirmed by spherical aberration correction electron microscopy, extended X-ray absorption fine structure measurement, and diffuse reflectance infrared Fourier transform spectroscopy. This catalyst manifests outstanding catalytic performance in hydrodeoxygenation of vanillin to yield 2-methoxy-4-methylphenol (MMP) efficiently and selectively, along with exceptional stability and scalability. Density functional theory (DFT) calculations indicate that this high activity results from the unique electronic structure of isolated palladium atoms confined in defective WO 2.72 . These findings may pave the way for the facile creation of single atom catalysts in a coordination-engineered strategy for the advance of single atom catalysis.
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POLYMER TESTING
·
2019
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IF 2.943
Ju Bai,Yaxin Zhang,Liyan Dong,Yanjun Hou,HaiJun Niu,Shuhong Wang,Cheng Wang
Here, we synthesized two kinds of novel conjugated block copolymers P1 and P2 by reacting squaric acid and three kinds of homemade diamine monomers . The polymers P1 and P2 can be dissolved in many normal organic solvents and form films by solution-cast method with high mechanical properties . In addition, when the 10% weight loss is selected as a reference point, the polymers P1 and P2 showed the thermal decomposition temperatures at around 309 and 312 °C, respectively. The polymer films exhibit high coloration efficiencies (CE) (262–282 cm 2 C −1 ) and good cyclic stabilities. In addition, the ITO/polymer/Al sandwich memory devices exhibited non-volatile resistive switching behaviors with low write, erase voltages (more than −0.6 V and less than 3.1 V, respectively), good ON/OFF ratio (843 and 1435) and reliable cycling endurance (more than 30,000 cycles). These properties illustrate that the polymers could be considered as potential electrode materials for both electrochromic and resistive memory devices.
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CRYSTAL GROWTH & DESIGN
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2022
·
IF 4.01
Haozhou Huang,Jun Li,An Du,Yinggang Jia,Yuehua Cong,Baoyan Zhang
A new series of bent-structure liquid crystalline dimers containing a cholesteryl group were synthesized. The molecular structure and mesophase properties of the dimers were characterized by FTIR, 1H-NMR, DSC, XRD, POM, and UV–vis. The BPmem was proposed, which is considered to be a transition state appearing during the cooling process between BP I and N* and having memory for the original lattice network of BP I. The BPmem state was analyzed in detail, and it proved to be influenced by the molecular structure, the cooling rate, and the surface anchoring. For the planar-aligned sample, the macroscopic color of BPmem is the superposition of two selective reflection wavelengths, different from those of conventional N* and BPs, which has potential application value.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Ke Li,Xiaoyi Sun,Hua Yin,Kun Yang,Pei Dai,Ling Han,Longgui Zhang,Riwei Xu
Preparing biobased high-performance thermosetting resins is one of the most important factors for sustainable development. In this work, two kinds of phthalonitrile resins containing spirocycle acetal structures were synthesized from pentaerythritol and renewable vanillin and isovanillin by an efficient two-step process. The structures of vanillin- and isovanillin-based phthalonitrile (VPN and IVPN) monomers were characterized by Fourier transform infrared (FTIR), NMR, matrix-assisted laser desorption/ionization time-of-flight mass spectrometry, and elemental analysis. The curing behaviors of these monomers were studied by differential scanning calorimetry and FTIR. The thermal stability and dynamic mechanical properties of the cured resins were investigated by thermogravimetric analysis and dynamic mechanical thermal analysis. The processing properties were studied by a rheological analysis. Compared with traditional petroleum-based phthalonitrile resins such as bisphenol A and bisphenol, cured VPN and IVPN resins exhibited good thermal stability and thermomechanical properties, high glass transition temperature (Tg), and excellent processability.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Yurong Zhuang,Chenchen Wang,Yong Wang,Yuhui Chen,Songqin Liu,Wei Wei
It’s the first time we found that vanillin and 3,3′,5,5′-tetramethylbenzidine (TMB) can reduce Tollens’ reagent to different types of Ag nanoparticles (Ag NPs) because of their different reducibility . Vanillin reduced the Tollens’ reagent to small size of Ag NPs (Ag45 NPs) which was colorless and has the maxmium absorption at 350 nm, while pink large Ag NPs (Ag100 NPs) with the maxmium absorption at 490 nm was reduced by TMB. Based on different types of AgNPs reduced by vanillin and TMB, dual-mode detection of vanillin by colorimetry and surface-enhanced Raman scattering (SERS) was designed. The solution changed from pink to colorless with the increasing concentration of vanillin (within 3 min). On the other hand, the reduced Ag45 NPs shows a high SERS enhancement factor, which can be applied for ultra-sensitive detection of vanillin in situ. The SERS had a low detection limit of 25.8 pM, which was 5-orders lower than the colorimetric method and most previously reported methods. Importantly, It avoids the additional procedures to prepare SERS-active substrates and can be used to discriminate vanillin from ethylvanillin, both of which are very difficult to be distinguished because of their much highly similar structure and property. Therefore, the visual, fast and high-sensitive dual-mode strategy has great potential in food safety assessment.
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GREEN CHEMISTRY
·
2024
·
IF 9.3
Zuzhi Li,Ya Ma,Xingjie Guo,Yang Cao,Qian Jiang,Mi Gao,Xudong Liu,Daniel C. W. Tsang,Zhicheng Jiang,Bi Shi
Efficient catalytic hydrogenation of lignin-based derivative vanillin (VAN) into valuable chemicals with a high selectivity is important yet challenging because of the lack of selective and active catalysts. Herein, a mixture of polyacrylonitrile (PAN) and water-insoluble tannin (Tan) was employed to create composite fibers through the electrospinning process, resulting in PAN–Tan composite fibers. The formation of hydrogen bonds between the –CN group of PAN and the phenolic –OH group of Tan proved advantageous for high dispersion and reduced physical entanglement, resulting in the production of thinner fibers. Leveraging abundant ortho-phenolic –OH groups of Tan, the PAN–Tan fibers were used to adsorb Pd2+ ions, which were reduced by in situ reduction process to Pd0 particles. Higher solute concentrations in the spinning solution improved the homogeneity of the electrospun PAN–Tan fibers, facilitating the dispersion and reduction of adsorbed Pd2+ on the fiber surface. Subsequently, these Pd/PAN–Tan fibers served as catalysts for the selective hydrogenation of the –CHO group of VAN to produce vanillyl alcohol (VAL) in an aqueous phase. Over 99% of VAN could be hydrogenated into VAL at 50 °C for 60 min under 0.5 MPa H2. Moreover, the catalyst exhibited universal applicability for the hydrogenation of diverse typical lignin-based aromatic aldehydes. The catalytic hydrogenation of VAN was then extended to a fixed-bed reactor for 24 h, and only VAL was detected in the effluent. Our study underscored the low energy consumption for catalyst preparation without additional reducing agents and high temperature carbonization process, the stability and reusability of the Pd/PAN–Tan fiber catalyst and its potential for large-scale industrial applications.
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ChemCatChem
·
2024
·
IF 3.8
Yuhao Zhang,Shuhui Huang,Wan-Qiu Liu,Jian Li
Graphical 4′-O-Methylnorbelladine (4′-MB) is a key precursor for the synthesis of Amaryllidaceae plant-derived alkaloids. In this study, an efficient biosynthetic system for the production of 4′-MB was developed through a comprehensive optimization strategy that includes protein engineering, enzyme immobilization, by-product recycling, and cofactor regeneration. This approach paves the way for the large-scale production of pharmaceuticals derived from Amaryllidaceae plants. Amaryllidaceae alkaloids (AAs) are plant-derived natural compounds with diverse bioactivities. To biosynthesize AAs, 4′-O-methylnorbelladine (4′-MB) is a key precursor that is first formed by C–N coupling between tyramine and 3,4-dihydroxybenzaldehyde catalyzed by a NADPH-dependent reductase. However, 3,4-dihydroxybenzaldehyde is oxygen sensitive and not stable due to its catechol moiety when constructing an in vitro enzymatic system for 4′-MB synthesis. To address this issue, we design an artificial biosynthetic route to synthesize 4′-MB. First, we choose isovanillin instead of 3,4-dihydroxybenzaldehyde as an alternative substrate. Then, a short-chain dehydrogenase/reductase (SDR) from Zephyranthes treatiae is utilized to couple tyramine and isovanillin. After demonstrating the synthesis of 4′-MB, we optimize the whole biocatalytic system with enhanced performance. The final enzymatic system can be reused for multiple cycles with the help of a crystalline inclusion protein (CipB)-mediated enzyme immobilization. Additionally, we scale up the reaction system from 50 µL to 10 mL, generating approximately 800 µM of 4′-MB. We envision that our work will provide an efficient and sustainable approach to produce 4′-MB, which could support the large-scale production of Amaryllidaceae plant-originated natural products.
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