SYNTHESIS-STUTTGART
·
2019
·Vol. 51
·期 17
·3221-3230
·
IF 2.867
Wei Sun,Mingjuan Zhang,Peilang Li,Yiqun Li
A novel and highly efficient one-pot synthesis of polysubstituted imidazoles from α-hydroxyphenylacetic acids, diphenylacetylene, and amines has been achieved by Pd(OAc)2/Ce(SO4)2/Bi(NO3)3 trimetallic catalytic system. A series of control experiments showed that this overall reaction occurs through a one-pot cascade process combining the steps of decarboxylation of α-hydroxyphenylacetic acids, Wacker-type oxidation of diphenylacetylene, and Debus–Radziszewski annulation of aryl aldehydes and benzil generated in situ, as well as amines. This reaction represents a novel multicomponent reaction using α-hydroxyphenylacetic acids and diphenylacetylene as sources of aryl aldehydes and a β-diketone. This process exhibits a broad substrate scope and a good functional group tolerance to assemble the corresponding polysubstituted imidazoles in excellent yields (72–88%) under mild conditions.
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3 Biotech
·
2026
·Vol. 16
·期 8
·328
·
IF 3.1
Zhu Hengzhou,Zhu Xiaodan,Huang Xiaona,Qian Yiyang,Li Jiahui,Zhang Jiaying,Niu Dong,Jin Chunhui
Gastric cancer (GC) is a prevalent malignancy worldwide with high morbidity and mortality. Its insidious onset and lack of sensitive early biomarkers impede routine screening, so most patients present advanced or metastatic disease at first diagnosis, leading to poor prognosis and scarce curative options. Surgery, chemotherapy and targeted therapy serve as standard GC treatments, however their efficacy is restricted by metastasis, adverse reactions and drug resistance, which drives the rapid development of immune checkpoint inhibitor (ICI)-based immunotherapy. Although monoclonal antibodies targeting programmed cell death protein 1/programmed cell death 1 ligand 1 (PD-1/PD-L1) resulted in significant survival benefits for GC patients, some patients exhibited an ineffective response. Our previous study has shown that Weitiao No. 3 (WD-3) enhanced the efficacy of anti-PD-1 immunotherapy by regulating intestinal flora in gastric cancer (GC) mice, in this study, huPBMC-NOG-dKO mice and MGC803 cells were used for in vivo and in vitro functional validation to explore the regulatory mechanism of WD-3 in GC immunotherapy. 16 S rRNA sequencing analysis of mouse fecal samples demonstrated that WD-3 significantly enriched the intestinal abundance of Lachnospiraceae and Ruminococcaceae in GC model mice. Targeted serum metabolomics further verified that WD-3 markedly elevated serum isobutyric acid level in GC mice. Combined with HE staining and tumor growth monitoring, both the intestinal flora mixture consisting of Lachnospiraceae and Ruminococcaceae and isobutyric acid prominently enhanced the anti-tumor efficacy of PD-L1 inhibitors in GC mice. Mechanistically, RNA sequencing and qRT-PCR assays identified ACOX2 as the most significantly up-regulated gene in isobutyric acid-treated MGC803 cells. Functional experiments using CCK-8 assay and flow cytometry revealed that isobutyric acid inhibited the viability and induced apoptosis of MGC803 cells, and such phenotypic changes were effectively rescued by ACOX2 knockdown. Furthermore, results from the CytoTox 96 cytotoxicity assay and ELISA revealed that combined treatment with isobutyric acid and PD-L1 inhibitor elevated the levels of LDH, IL-2, TNF-α, IFN-γ, Perforin 1 and GzmB, while suppressing IL-8, PD-1 and TIM-3 expression in CD8⁺ T cells co-cultured with MGC803 cells. Notably, all these regulatory effects were abrogated when MGC803 cells were transfected with si-ACOX2. These results suggested that WD-3 modulated intestinal flora to elevate isobutyric acid level, thereby enhancing the inhibitory effect of PD-L1 inhibitor on tumor growth and boosting the anti-tumor activity of CD8⁺ T cells by up-regulating ACOX2 expression in GC. These findings may provide novel targets for improving anti-PD-L1 therapy against GC.
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Xiaoli Luo,Limin Chen,Jianying Yang,Shuting Li,Manting Li,Qian Mo,Yinbao Li,Xinchun Li
Methods that can directly and sensitively quantify a set of correlative substances lack of chromophores in pharmaceuticals are persistently desired. Here, by facile preparation of Pt-Pd nanoparticles/chitosan/nitrogen-doped graphene (N-Gra) nanocomposite, we establish an electroanalytical method for simultaneous detection of ascorbic acid (AA), sulfite and oxalic acid (OA) that are closely involved with Vitamin C injection, a widely-used clinical drug. One-step electrodeposition of Pt-Pd bimetallic nanoparticles on chitosan/N-Gra decorated glassy carbon electrode was proposed to construct a well-performing electrocatalyst possessing notable electrochemical activity to the electrooxidation of both sulfite and OA. The electrocatalytic ability was evidenced by the increased current response and decreased oxidation overpotential. More importantly, sufficiently electrochemical resolution of multiple oxidative peaks allowed simultaneous quantitation of the three species of interest. The peak currents measured by differential pulse voltammetry were linear to the analytical concentration of AA, sulfite, and OA, yielding good linear ranges of 2 ~ 400 μM, 8 ~ 600 μM, and 1.5 ~ 500 μM, respectively. Correspondingly, the limit of detection was 0.97 μM, 5.5 μM, and 0.84 μM. This work opens a vista for multiplex assays of pharmaceuticals, including drug principal ingredient, toxic preservative, and decomposed impurity without chromatographic separation, and thus holds promise for the overall quality control for clinical drug.
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FUEL
·
2024
·
IF 6.7
Junqian Wang,Yi Wang,Yuqi Wang,Xinyi Li,Caichao Wu,Tianyu Zhang,Bin Tian,Lili Qian,Yang Guo,Le Wu,Lan Zheng,Yanan Li,Xin Ding
Currently, traditional hydrodeoxygenation (HDO) catalysts have various shortcomings such as low activity levels and vulnerability to deactivation. Therefore, a series of MXene-supported Ni-M (M = Pd, Pt, Ru) bimetallic catalysts were designed and prepared. The above catalysts were also comprehensively characterized using XRD, BET, H 2 -TPR, NH 3 -TPD, XPS, SEM and TEM methods. Moreover, due to the largest particular specific surface area, moderate amount of acid sites and the strongest three-electron transfer channels between support and active metals of Ni-Pd/MXene catalyst, it exhibited the superior catalytic performance to achieve 100 % guaiacol conversion and 35.15 % highest overall yields of HDO products (Y HDO ) under the optimal reaction conditions (at 340 °C for 8 h, utilizing in-situ hydrogen source: formic acid). Furthermore, a detailed discussion on the main reaction pathways and mechanism of guaiacol HDO catalyzed by Ni-Pd/MXene was provided, an unique bimetallic synergistic “relay catalytic” theory has been proposed. Kinetic studies revealed that phenol, one of the main HDO products, is primarily generated via guaiacol demethoxylation, while catechol dehydroxylation to phenol acts as the rate-determining step. This work introduces a new strategy for the development of HDO catalysts.
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ANALYTICAL CHEMISTRY
·
2024
·
IF 6.7
Mengdie Lei,Xilin Ding,Jin Liu,Yinjun Tang,Hongxiang Chen,Yu Zhou,Chengzhou Zhu,Hongye Yan
The urgent need for sensitive and accurate assays to monitor acetylcholinesterase (AChE) activity and organophosphorus pesticides (OPs) arises from the imperative to safeguard human health and protect the ecosystem. Due to its cost-effectiveness, ease of operation, and rapid response, nanozyme-based colorimetry has been widely utilized in the determination of AChE activity and OPs. However, the rational design of nanozymes with high activity and specificity remains a great challenge. Herein, trace amount of Bi-doped core–shell Pd@Pt mesoporous nanospheres (Pd@PtBi2) have been successfully synthesized, exhibiting good peroxidase-like activity and specificity. With the incorporation of trace bismuth, there is a more than 4-fold enhancement in the peroxidase-like performance of Pd@PtBi2 compared to that of Pd@Pt. Besides, no significant improvement of oxidase-like and catalase-like activities of Pd@PtBi2 was found, which prevents interference from O2 and undesirable consumption of substrate H2O2. Based on the blocking impact of thiocholine, a colorimetric detection platform utilizing Pd@PtBi2 was constructed to monitor AChE activity with sensitivity and selectivity. Given the inhibition of OPs on AChE activity, a biosensor was further developed by integrating Pd@PtBi2 with AChE to detect OPs, capitalizing on the cascade amplification strategy. The OP biosensor achieved a detection limit as low as 0.06 ng mL–1, exhibiting high sensitivity and anti-interference ability. This work is promising for the construction of nanozymes with high activity and specificity, as well as the development of nanozyme-based colorimetric biosensors.
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BIOMASS & BIOENERGY
·
2024
·
IF 5.8
Zhenjing Jiang,Wuyu Wang,Xuelai Zhao,Xinghua Zhang,Qi Zhang,Longlong Ma
Production of jet fuel is not only promising but challenging in the field of biomass utilization. Here we proposed a novel route to produce highly branched alkanes with ultra-low freezing point using n-butyraldehyde as feedstock by self-aldol condensation and subsequent hydrodeoxygenation (HDO). The catalyst characterization revealed that the MgO-SiO 2 catalyst played an acid-base synergetic effect role in the self-aldol condensation of n-butyraldehyde using n-butanol as solvent, which obtained C8 oxygenate and C12 oxygenate with yield of 69.3 % and 26.8 % respectively. The medium Brønsted base site of the catalyst captured α-H to promote the formation of enolate from n-butyraldehyde, and the Lewis acid sites promoted the dehydration of intermediate products. DFT simulation showed that n-butanol activated α-C in enolate in aldol condensation, and deactivated the oxygen atoms in enolate by hydrogen bonds to inhibit side reactions. Finally, the obtained condensation products were subjected to HDO reaction over the 5 wt% Pd/C and HZSM-5 catalysts, obtaining the highly branched alkanes with an ultra-low freezing point of -120.7 °C for C8 alkane and -78.7 °C for C12 alkane suitable for bio-jet fuels.
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Biomaterials Advances
·
2025
·
IF 6
Xin Zhang,Li Li,Haiqing Niu,Zixin Liang,Liuqi Sang,Ning Wang,Fengli Huang,Xingzhi Han,Zhihao Liu,Xiao Shi,Qun Zhang,Jing Hu,Xiaoping Qian
Background The prognosis of patients with colorectal liver metastasis (CRLM) is poor. The 5-year survival rate of those who cannot be treated by surgery is less than 5 %, thus, the management of patients with CRLM remains a significant challenge. Based on the anti-tumor activity of traditional Chinese medicine monomer and the local immune activation caused by low dose radiotherapy combined with immune checkpoint inhibitors, we jointly applied it to explore the tumor inhibitory effect and the change of local immune microenvironment in liver metastasis model. Methods We engineered biomimetic nanoparticles through macrophage membrane encapsulation of gambogic acid (GA)-loaded PLGA cores, employing a double emulsion-solvent evaporation method to fabricate M-PLGA@GA nanoparticles. In tumor-bearing mice with surgically induced colorectal liver metastasis via hemisplenectomy, therapeutic efficacy was evaluated through intratumoral administration of M-PLGA@GA combined with triple-modality therapy: low-dose radiotherapy (LDRT; 5 Gy), anti-programmed cell death protein 1 monoclonal antibody (anti-PD-1 mAb; 200 μg), and nanoparticle delivery. This combinatorial approach leveraged spatial-temporal control of tumor microenvironment modulation. Results The nanoparticles augmented the targeted delivery ability of drugs to tumor cells and in vivo circulation duration, coupled with improved aqueous solubility of the encapsulated therapeutic agent, all while preserving its therapeutic potency. The radiotherapy notably augments the population of Dendritic cells (DCs) and bolsters the presentation of antigens to the tumor cells. Moreover, the administration of GA induces modifications in the tumor's immune microenvironment and escalates the fraction of CD8+ T cells. Within the context of the mouse CRLM model, the amalgamation of M-PLGA@GA with low-dose radiotherapy and immunotherapy markedly attenuates the pace of tumor proliferation and extends the survival of mice. Conclusions Our findings propose that a novel therapeutic regimen combining radiotherapy, immunotherapy, and Nanoparticle gambogic acid can effectively impede tumor progression in the mouse model of CRLM. Therefore, our study provides novel insights into the role of combined antitumor therapy on innate and adaptive antitumor immunity modulation for CRLM.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yaxin Li,Wei Qin,Xinyang Li,Qi Zhu,Fu-quan Bai,Tao Tian
It is highly desirable to enhance the charge separation and introduce catalytic functions for efficient water splitting into hydrogen on g-C 3 N 4 . Herein, heterojunctions of PCN-222(M)/g-C 3 N 4 -AA were successfully synthesized through the in-situ hydrothermal method, where metallic ions (M) were strategically incorporated into porphyrinic metal-organic framework (MOF) ligands. This heterojunction design strategy is considered to establish directional charge transfer channels for photogenerated electron-hole (e − -h + ) pairs and thereby enhance its separation efficiency. Remarkably, the 1 % PCN-222(Pd)/g-C 3 N 4 -AA composite demonstrated superior photocatalytic hydrogen evolution performance, achieving a rate of 2338.17 μmol·g −1 ·h −1 . This rate was 3.23 times higher than that of pure g-C 3 N 4 and 2.79 times higher than that of g-C 3 N 4 -AA. The composite morphology was characterized by a series of physicochemical properties. Bandgap analysis via Tauc plot revealed that metal ion doping in the porphyrin center effectively modulates the HOMO-LUMO levels at the composite interface. First-principles calculations coupled with hydrogen adsorption free energy analysis elucidated how interfacial engineering between PCN-222(M) and g-C 3 N 4 -AA governs heterostructure formation and charge transfer pathways. This work systematically deciphers the synergistic effects of bimetallic MOF integration and provides insights into the underlying photocatalytic reaction mechanism.
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Catalysis Science & Technology
·
2017
·Vol. 7
·期 6
·1415-1422
·
IF 5.773
Zheng Chen,Hongyan Pan,Qian Lin,Xin Zhang,Sheng Xiao,Shun He
Pd core–silica shell catalysts (PdX@SiO2, X = KBr, CTAB, SC) were prepared with and without the addition of three different functional molecules, potassium bromide (KBr), cetyltrimethyl ammonium bromide (CTAB) and sodium citrate dihydrate (SC), by the reverse micelle method, and then characterized by TEM, XRD, EDS, XPS and N2 adsorption/desorption. Results showed that the addition of functional molecules decreased the Pd particle size of the catalysts, and Br− of KBr and CTAB were selectively adsorbed on the surface of Pd particles. Among the prepared catalysts, the catalyst PdKBr@SiO2 had the highest H2O2 selectivity (98%) and productivity (716 mmol gPd−1 h−1). Compared with the catalyst Pd@SiO2 prepared without any additional functional molecules, whose H2O2 selectivity and productivity were 26% and 396 mmol gPd−1 h−1, respectively, the H2O2 selectivity and productivity of the catalyst PdKBr@SiO2 were 277% and 81% higher, respectively, than those of the catalyst Pd@SiO2. The reason for this was that the Br− of KBr can be easily selectively adsorbed on the coordinatively unsaturated sites of the Pd particle surface, which could decrease the energy of the Pd surface and restrain side reactions by inhibiting the O–O bond cleavage of O2 and H2O2. And the catalyst PdKBr@SiO2 has better stability and recyclability than the conventional supported catalyst Pd/SiO2. In contrast, the catalyst PdSC@SiO2 had the lowest H2O2 selectivity (23%) and productivity (395 mmol gPd−1 h−1) because the catalyst PdSC@SiO2 prepared with the functional molecule SC and without Br− had the smallest Pd particle size, which can lead to more coordinatively unsaturated sites and increase side reactions.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yanmei Shi,Liqin Chao,Xiaobing Liu,Zhihong Chen,Zhenghui Chang,Sisen Zhang,Shusheng Zhang,Kai Hu
Development of advanced in vivo sampling tools for the synchronous monitoring of drugs and endogenous biomarkers is critical for integrated pharmacokinetic-pharmacodynamic (PK-PD) studies. Herein, a novel solid-phase microextraction (SPME) fiber coating was engineered based on a zwitterionic covalent organic framework (EB-TTB-DABSA COF), strategically functionalized with sulfonate and quaternary ammonium groups. This rationally designed coating provides synergistic electrostatic, π–π, and hydrophobic interactions, enabling the efficient and simultaneous extraction of both cationic alkaloids and neurotransmitters. Coupled with LC-MS/MS, the developed platform achieved highly sensitive (limits of detection down to 3.3 × 10 −3 ng·mL −1 ), minimally invasive, and synchronous monitoring of these analytes in paired blood and brain matrices of living rats. Application in a Parkinson's disease (PSD) model revealed altered pharmacokinetics of Coptis chinensis alkaloids, including significantly increased area under the curve (AUC) values ( p < 0.01) and prolonged elimination half-lives compared to controls. These findings indicate enhanced systemic absorption and improved bioavailability of alkaloids under PSD conditions. Crucially, pharmacodynamic analysis showed that alkaloid administration triggered a synchronized restoration of key depleted neurotransmitters in PSD brains. A correlation with a characteristic hysteresis pattern further established a delayed neuroprotective relationship between alkaloid concentrations and neurotransmitter levels. This study not only introduces a robust zwitterionic COF-SPME platform for concurrent in vivo biosampling but also provides the first quantitative neuropharmacological perspective on Coptis chinensis alkaloids, offering a foundational framework for mechanistic research and therapeutic development in PSD.
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Biomaterials Research
·
2022
·Vol. 26
·期 1
·1-21
·
IF 15.863
Wu Hao,Wei Guoli,Luo Lixia,Li Lingchang,Gao Yibo,Tan Xiaobin,Wang Sen,Chang Haoxiao,Liu Yuxi,Wei Yingjie,Song Jie,Zhang Zhenhai,Huo Jiege
Background Combination of chemotherapy and immune checkpoint inhibitor therapy has greatly improved the anticancer effect on multiple malignancies. However, the efficiency on triple-negative breast cancer (TNBC) is limited, since most patients bear “cold” tumors with low tumor immunogenicity. Doxorubicin (DOX), one of the most effective chemotherapy agents, can induce immunogenic cell death (ICD) and thus initiating immune response.Methods In this study, to maximize the ICD effect induced by DOX, chitosan and cell-penetrating peptide (R6F3)-modified nanoparticles (PNPs) loaded with ginsenoside Rg3 (Rg3) were fabricated using the self-assembly technique, followed by co-encapsulation with DOX based on thermo-sensitive hydrogel. Orthotopic tumor model and contralateral tumor model were established to observe the antitumor efficacy of the thermo-sensitive hydrogel combined with anti-PD-L1 immunotherapy, besides, the biocompatibility was also evaluated by histopathological.Results Rg3-PNPs strengthened the immunogenic cell death (ICD) effect induced by DOX. Moreover, the hydrogel co-loading Rg3-PNPs and DOX provoked stronger immune response in originally nonimmunogenic 4T1 tumors than DOX monotherapy. Following combination with PD-L1 blocking, substantial antitumor effect was achieved due to the recruitment of memory T cells and the decline of adaptive PD-L1 enrichment.Conclusion The hydrogel encapsulating DOX and highly permeable Rg3-PNPs provided an efficient strategy for remodeling immunosuppressive tumor microenvironment and converting immune “cold” 4T1 into “hot” tumors.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chaoyi Zhou,Guojun Lv,Xuyang Zou,Jiangzhang Wang,Yan Chen,Jialing Shen,Shihao Su,Weilong Xing,Deling Fan,Yangbin Shen
Room-temperature ambient air is cheap and easy to obtain, hence the application of room-temperature ambient air as sole oxidant for pollutant degradation is extremely fascinating. In this work, core–shell coordination sponge-Fe 0 @Cu-Pd trimetal catalyst was synthesized via a simple step displacement plating process employing first displacement of Cu and the subsequent displacement of Pd, and applied as heterogeneous catalyst for synergistic catalytic degradation of composite pollutants including TC and PNP. The prepared s-Fe 0 @Cu-Pd trimetal sample was characterized with XRD, SEM, TEM, VSM and XPS. The characterization results revealed the obtained s-Fe 0 @Cu-Pd trimetal sample was a 20 ∼ 30 nm core–shell spherical morphology composed of Fe 0 aggregates core wrapped by a Cu-Pd shell layer. The obtained sponge-Fe 0 @Cu-Pd trimetal catalyst could efficiently activate room-temperature dissolved ambient oxygen and achieve the largest TC removal rate of 99.08 % and PNP removal rate of 97.16 % as well as the biggest removal rate constant of 8.76 min −1 for TC degradation and 7.55 min −1 for PNP degradation within 60 min at experimental conditions: [TC] = 30 mg/L, [PNP] = 30 mg/L, [Catalyst] = 25.52 g/L, pH = 3, 298 K ascribed to the strongest oxidation and reduction ability confirmed by CV characterizations, the lowest charge transfer and contact resistance affirmed by EIS measurements, the strongest O 2 activation ability verified by O 2 -TPD characterizations and DFT analyses, the largest external surface area and mesoporous volume validated by Nitrogen adsorption and desorption characterizations as well as the synergistic catalysis effect for wrapped Cu and Pd. Quenching experiments and EPR characterizations revealed that •OH, •O 2 − , 1 O 2 and •H are all the reactive species and meanwhile •O 2 − served as the main reactive oxygen species. Furthermore, possible mechanisms of TC and PNP degradation via sponge-Fe 0 @Cu-Pd trimetal catalyst were proposed.
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