ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Tianhang Liu,Kaisheng Yao,Hang Li,Qi Wang,Tianhang Han,Aozhou Wang,Haili Zhao,Weiwei Lu
Developing a simple, environmentally friendly, and mild method to one-step prepare bimetallic nanoframes is pretty important but still technically challenging. In this paper, a simple and easy-to-operate ionic liquid (IL)-regulated protocol is proposed to fabricate Au–Pd superbranched trigonal nanoframes (STNFs) in water at room temperature. In the aqueous solution containing precursors (Na2PdCl4 and HAuCl4) and a reducing agent (ascorbic acid), a common IL 1-octyl-3-methylimidazolium chloride ([C8mim]Cl) was used to guide the anisotropic growth and construction of Au–Pd STNFs, brightly showing green and energy-saving characteristics. Au–Pd STNFs take shape as unique two-dimensional (2D) trigonal frameworks containing multilevel orderly branches. It is found that [C8mim]Cl is crucial to the formation of Au–Pd STNFs. Owing to the unique structures, high specific surface areas, large freestanding sizes, and probably electronic effects between Au and Pd, Au–Pd STNFs-1 exhibit dramatically enhanced catalytic activity, selectivity, durability, and convenience for recycling in the 4-nitrostyrene hydrogenation reaction. Specifically, 4-nitrostyrene can be converted completely only within 5.0 min at 25 °C under atmospheric pressure, and the selectivity toward 4-nitroethylbenzene is as high as 100% and maintains good performance after five cycles. It is expected that well-constructed Au–Pd STNFs also display advanced potential in other applications.
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ANALYTICAL CHEMISTRY
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2025
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IF 6.7
Yujun Cheng,Jianping Guan,Zhipeng Zhang,Ruili Li,Yao Yao,Xiaotong Sun,Qi Liu,Xiaoqing Chen
Constructing materials that possess both catalytic properties and surface plasmonic active structures presents an essential requirement in the field of in situ surface-enhanced Raman spectroscopy (SERS) monitoring. In this work, we developed a novel black raspberry-like bifunctional nanoreactor platform (HPRS@Au–Pd) with enhanced surface-enhanced Raman spectroscopy (SERS) activity (EF = 3.11 × 109) and excellent catalytic performance (e.g., |K| = 1.72 × 10–2 s–1 for 4-BTP). This platform enables sensitive and real-time monitoring of Suzuki reactions, providing an efficient and stable system for mechanistic investigations. By fitting a first-order kinetic model, we quantitatively analyzed the reaction kinetics of haloarenes on Pd NPs, revealing the direct involvement of surface-bound Pd NPs in the catalytic process. Furthermore, 4MPBA-blocking experiments using haloarenes devoid of functional groups demonstrated the absence of catalytic activity from dissolved Pd species, conclusively supporting the heterogeneous nature of the reaction. This work extends the applicability of the conclusion regarding heterogeneous catalysis to a broader range of substrates, offering valuable insights into the design and optimization of dual-functional nanoreactors. Beyond the Suzuki reactions, the versatility of this platform opens avenues for applications in other catalytic reactions, showcasing its potential in advanced catalytic studies and real-time monitoring.
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Materials Today Bio
·
2025
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IF 10.2
Yanan Wang,Nan Cheng,Qi Zhang,Fei Chang,Teng Wang,Minrui Kan,Yutong Han,Baiqiang Zhai,Kunlun Huang,Xiaoyun He
Recently, the nanozyme Pd@Pt has garnered attention due to its notable specific surface area and superior enzyme-like catalytic activity, leading to extensive examination and application in previous studies. However, the comprehensive impact of Pd@Pt nanozyme on treating metabolic disorders, such as diabetes and its associated conditions, remains largely unexplored. This research aimed to clarify how Pd@Pt influences metabolic balance at both the transcriptome and microbiome levels and to explore the interactions between microbiota and genes. We conducted an examination of mice subjected to a high-fat diet (HFD) following treatment with Pd@Pt. Transcriptome analysis was performed to identify differentially expressed genes (DEGs), and microbiome analysis was conducted to identify significant bacterial correlations associated with Pd@Pt exposure. The results indicated enhancements in glucose metabolism dysfunctions in the treated mice. Transcriptome analysis revealed that DEGs after Pd@Pt administration were enriched in the PI3K-Akt, NF-κB, and MAPK signaling pathways in the liver. Microbiome analysis identified four significant bacteria that exhibited a strong negative correlation with Pd@Pt exposure, while ten bacteria showed a positive correlation. Furthermore, a correlation network established among the gut microbiota, metabolites, and DEGs demonstrated a robust association. This research enhances our understanding of the mechanisms by which Pd@Pt affects the regulation of metabolic diseases in HFD-exposed environments and proposes a novel strategy for utilizing nanozymes in human health management.
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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Meng Li,Diangen Zhou,Hualiang An,Shanshan Dong,Xinqiang Zhao,Yanji Wang
2-Ethylhexanal (2EH) is an important intermediate for the production of 2-ethyhexanoic acid (2-ETA), and studying the direct synthesis of 2EH through heterogeneous catalysis of n-butanal aldol condensation-selective hydrogenation reaction integration is of great significance for the industrial production of 2-ETA. Herein, a series of Pd/TiO2 catalysts were prepared and characterized by XRD, CO pulse adsorption, TEM, CO2/NH3-TPD and H2-TPR. Their catalytic performance for direct synthesis of 2EH from n-butanal was investigated in stainless steel autoclave first. The results showed that the Pd/TiO2 prepared by the excessive impregnation method, loaded with 0.5 wt.% of Pd, and reduced at 400 ℃ showed excellent catalytic performance: 95.4% conversion of n-butanal and up to 99.9% selectivity of 2EH. The particle size of Pd, the base strength and the amount of acid/base of the catalyst are the main factors affecting its catalytic performance. The smaller the particle size of Pd, the greater the base strength and the larger the amount of acid/base of the catalyst, the better its catalytic performance. Then the integrated reaction mechanism was established based on the results of characterization and FT-IR of online sampling. Furtherly, the continuity of the reaction process was achieved on fixed-bed reactor. Under the reaction conditions of a liquid hourly space velocity (LHSV) of 7.2 h-1, a reaction temperature of 190 °C and a H2 pressure of 3.2 MPa, the conversion of n-butanal and the selectivity of 2EH were 91.2% and 89.8%, respectively. During the continuous operation for 300 h under optimal conditions, the conversion of n-butanal decreased slightly first and then stabilized, while the selectivity of the target product 2EH remained basically unchanged.
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JOURNAL OF NANOBIOTECHNOLOGY
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2024
·Vol. 22
·期 1
·1-18
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IF 10.6
Zou Ting,Huang Yun,Zhou Zongtao,He Shuangyan,Liu Jia,Chen Yalan,Liu Hongdu,Luo Zhonghui,Liu Miaoxin,Wei Hua,Yu CuiYun
Clinical treatment of hepatocellular carcinoma (HCC) with 5-fluorouracil (5-FU), the primary anticancer agent, remains unsatisfactory due to the glutathione (GSH)-associated drug resistance and immunosuppressive microenvironment of HCC. To develop a facile yet robust strategy to overcome 5-FU resistance for enhanced immunotherapy treatment of HCC via all dimensional GSH exhaustion, we report in this study construction of a minimalist prodrug consisting of 5-FU linked to an indoleamine-(2,3)-dioxygenase (IDO) inhibitor (IND) via a disulfide bridge, FU-SS-IND that can further self-assemble into stabilized nanoparticles, FU-SS-IND NPs. Specifically, besides the disulfide linker-induced GSH exhaustion, IND inhibits GSH biosynthesis and enhances the effector function of T cells for turning a “cold” tumor to a “hot” one, which synergistically achieving a tumor inhibition rate (TIR) of 92.5% in a 5-FU resistant mice model. Most importantly, FU-SS-IND NPs could upregulate programmed death ligand 1 (PD-L1) expression on the surface of tumor cells, which enables facile combination with immune checkpoint blockade (ICB) for a ultimate prolonged survival lifetime of 5-FU-resistant tumors-bearing mice. Overall, the minimalist bioreducible nano-prodrug developed herein demonstrates great translatable potential for efficiently reversing drug resistance and enhancing immunotherapy of HCC.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Huan Su,Chao Shan,Xiaolin Zhang,Bingcai Pan
Chemical oxidation is essential in treating P(I)/P(III)-bearing wastewater, while conventional oxidation processes suffer from low selectivity and high cost induced by oxidant reagents. Herein, a low-cost catalyst PdNi 10 was developed to rival the noble metal Pd, which had been known as the only catalyst enabling chemical-free oxidation of P(I)/P(III) into P(V) by ambient O 2 . The PdNi 10 fabricated via optimized method even outperformed Pd in catalytic activity at identical dosage (0.10 g L −1 ), achieving efficient conversion of 1.00 mM of P(I) into P(V) (>94% in 30 min) with wide applicable pH range from 3.0 to 9.0. The aerobic oxidation of P(I) and P(III) over PdNi 10 was confirmed via scavenging experiments to be both dominated by non-radical pathways with apparent activation energies of 44.5 and 21.3 kJ mol −1 , respectively. Interestingly, the individual roles of Ni components of PdNi 10 in the catalytic oxidation were found negligible. The H 2 O-methanol binary solvent experiment suggested that H 2 O mediated the catalytic reaction and the interfacial OH groups as a result of H 2 O dissociation served as the main reactive oxidant species for P(I)/P(III) oxidation. Furthermore, synergistic mechanism was proposed for the Ni and Pd sites with favorable roles in the essential reaction steps of dehydrogenation and hydroxylation, respectively. This study is believed to advance the treatment strategy of P(I)/P(III)-rich wastewater and to shed new light on the development of low-cost catalysts enabling chemical-free aerobic oxidation processes under facile condition.
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Materials Today Bio
·
2025
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IF 10.2
Liangyin Wei,Hong Wang,Xietao Ye,Junfan Yue,Hong Guo,Dengxuan Mao,Xia Li,Yeyang Sun,Congyan Liu,Yuping Liu,Yan Chen
The response rate of programmed cell death protein-1 (PD-1) inhibitors in breast cancer remains unsatisfactory, primarily due to the limited infiltration and activity of tumor-infiltrating T lymphocytes (TILs). Previous studies demonstrated that oxymatrine (Om) and astragaloside IV (As) could enhance TIL infiltration and function by inhibiting cancer-associated fibroblasts (CAFs) and promoting mitochondrial activity in TILs, respectively. Thus, combining Om and As may be a promising strategy to improve the antitumor effects of PD-1 inhibitors in breast cancer. However, co-delivery above drugs into breast cancer tissue is challenging due to their low bioavailability and distinct physicochemical properties. This study addresses this challenge by formulating Om and As co-loaded liposomes (Om-As-Lip) and comparing the scale-up production methods: high-pressure homogenization (EP-HPH) and microfluidics. Om-As-Lip prepared via microfluidics demonstrated superior entrapment efficiency (As: 99.03 ± 0.04%, Om: 67.01 ± 0.02%) and a significantly higher production rate (22.12 mL/min) compared to EP-HPH (1.19 mL/min). Additionally, Om-As-Lip produced by microfluidics increased the area under the curve (AUC) (Om: 6.17-fold, As: 2.07-fold) and maximum concentration (Cmax) (Om: 1.58-fold, As: 3.49-fold) compared to the free drugs. Importantly, Om-As-Lip enhanced the antitumor efficacy of α-PD-1 by inhibiting CAF activation and boosting TIL activity, resulting in a tumor inhibition rate of 61.2% and extended survival in mice. This work presents a novel perspective for scaling up co-delivered formulations of drugs with differing polarities to improve breast cancer immunotherapy.
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Marine Drugs
·
2024
·Vol. 22
·期 5
·193
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IF 4.9
Baoxiang Wang,Lihua Geng,Jing Wang,Yuxi Wei,Changhui Yan,Ning Wu,Yang Yue,Quanbin Zhang
Parkinson’s disease (PD) is a prevalent neurodegenerative disorder, and accumulating evidence suggests a link between dysbiosis of the gut microbiota and the onset and progression of PD. In our previous investigations, we discovered that intraperitoneal administration of glucuronomannan oligosaccharides (GMn) derived fromSaccharina japonicaexhibited neuroprotective effects in a 1-methyl-4-phenyl-1,2,3,6-tetrahydropyridine (MPTP)-induced PD mouse model. However, the complicated preparation process, difficulties in isolation, and remarkably low yield have constrained further exploration of GMn. In this study, we optimized the degradation conditions in the preparation process of GMn through orthogonal experiments. Subsequently, an MPTP-induced PD model was established, followed by oral administration of GMn. Through a stepwise optimization, we successfully increased the yield of GMn, separated from crude fucoidan, from 1~2/10,000 to 4~8/1000 and indicated the effects on the amelioration of MPTP-induced motor deficits, preservation of dopamine neurons, and elevation in striatal neurotransmitter levels. Importantly, GMn mitigated gut microbiota dysbiosis induced by MPTP in mice. In particular, GM2 significantly reduced the levels ofAkkermansia, Verrucomicrobiota, andLactobacillus, while promoting the abundance ofRoseburiaandPrevotellacompared to the model group. These findings suggest that GM2 can potentially suppress PD by modulating the gut microbiota, providing a foundation for the development of a novel and effective anti-PD marine drug.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Yuanjie Xu,Run Hou,Kunxiang Chi,Bo Liu,Zemin An,Lizhi Wu,Li Tan,Xupeng Zong,Yihu Dai,Zailai Xie,Yu Tang
Palladium-based catalysts have long been considered the benchmark for methane combustion; however, the authentic phase of catalytic active sites remains a subject of ongoing debate. Additionally, challenges like water-poisoning and long-term stability need to be addressed to advance catalyst performance. Herein, we investigate Pd on Co 3 O 4 nanorods as a highly effective catalyst for catalytic oxidation of methane, demonstrating long-term stability and water tolerance during a 100-h continuous operation at 350 °C. Comprehensive characterizations reveal the presence of an active Pd-oxygen vacancy (O v )-cobalt interface in Pd/Co 3 O 4 , which effectively adsorbs molecular O 2 . The absorbed oxygen species on this interface are activated and directly participate in methane combustion. Moreover, near-ambient pressure X-ray photoelectron spectroscopy demonstrates that Pd nanoparticles undergo a rapid phase transition and predominantly remain in the metallic state during the reaction. This behavior is attributed to the electronic metal-support interaction between Pd and Co 3 O 4 . Furthermore, in situ Fourier transformed infrared spectrum reveals that under reaction conditions, HCO 3 * species are formed initially and subsequently transformed into formate species, indicating that the formate pathway is the dominant mechanism for CH 4 oxidation.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 8
·1-17
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IF 5.3
Liang Jintao,Li Canru,Zhou Yu,Fan Lingling,Liu Lin,Liang Jianlu,Tan Xiaohong,Zhou Zhide,Li Guiyin
Golgi protein 73 (GP73) is highly expressed in hepatocellular carcinoma (HCC) and considered a sensitive serum biomarker for HCC diagnosis. Herein, a label-free electrochemical aptasensor for ultrasensitive detection GP73 based on nitrogen-doped reduced graphene oxide-ferrocene-platinum@palladium nanoparticles (NRGO-Fc-Pt@Pd NPs) was constructed. The NRGO-Fc-Pt@Pd NPs offered excellent conductivity, biocompatibility, and large surface area, serving as both an electrode modifier and a redox probe due to Fc's good electroactivity. GP73 aptamer (GP73 Apt ) was covalently bound with the NRGO-Fc-Pt@Pd NPs to form the signal probe. When GP73 specifically bound to GP73 Apt to form GP73-GP73 Apt complex and fell off from the electrode, it leads to an increased Fc(Fe(II)/Fe(III)) peak current in differential pulse voltammetry (DPV) due to the enhancing of the sensing interface's electroactivity. Under optimized conditions, the label-free electrochemical aptasensor demonstrated a linear relationship with GP73 concentration in the range 1.0 ng/mL-300 ng/mL, with R 2 of 0.99594 and a limit of detection (LOD) of 0.3524 ng/mL. In addition, the aptasensor showed good specificity, reproducibility, and stability. Furthermore, the developed aptasensor was applied to detect the GP73 in actual serum samples with good recoveries (97.85%-107.48%) and relative standard deviations (RSDs) (0.37%–7.85%) via the spiked recovery method. All the results may provide a new approach for HCC clinical detection. Graphical
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JOURNAL OF EXPERIMENTAL & CLINICAL CANCER RESEARCH
·
2024
·Vol. 43
·期 1
·1-22
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IF 11.4
Tu Xiaoxuan,Chen Longxian,Zheng Yi,Mu Chenglin,Zhang Zhiwei,Wang Feiyu,Ren Yiqing,Duan Yingxin,Zhang Hangyu,Tong Zhou,Liu Lulu,Sun Xunqi,Zhao Peng,Wang Lie,Feng Xinhua,Fang Weijia,Liu Xia
Background The paucity of reliable biomarkers for predicting immunotherapy efficacy in patients with advanced hepatocellular carcinoma (HCC) has emerged as a burgeoning concern with the expanding use of immunotherapy. This study endeavors to delve into the potential peripheral biomarkers capable of prognosticating efficacy in HCC patients who are poised to receive anti-PD-1 monotherapy within the phase III clinical trial, KEYNOTE394. Additionally, we sought to elucidate the underlying molecular mechanisms for resistance to immune checkpoint blockade (ICB) and propose innovative combination immunotherapy strategies for future clinical application.Methods Patient blood samples were collected for single-cell RNA sequencing to evaluate the immune cell signature before receiving ICB therapy. Subsequently, in vitro assays and in vivo murine model experiments were conducted to validate the mechanism that S100A9+CD14+ monocytes play a role in ICB resistance.Results Our study demonstrates a notable enrichment of S100A9+CD14+ monocytes in the peripheral blood of patients exhibiting suboptimal responses to anti-PD-1 therapy. Moreover, we identified the Mono_S100A9 signature as a predictive biomarker, indicative of reduced efficacy in immunotherapy and decreased survival benefits across various tumor types. Mechanistically, S100A9 activates PD-L1 transcription by directly binding to the CD274 (PD-L1) gene promoter, thereby suppressing T-cell proliferation and cytotoxicity via the PD-1/PD-L1 axis, consequently diminishing the therapeutic effectiveness of subsequent anti-PD-1 treatments. Furthermore, our in vivo studies revealed that inhibiting S100A9 can synergistically enhance the efficacy of anti-PD-1 drugs in the eradication of hepatocellular carcinoma.Conclusion sOur study underscores the significance of S100A9+CD14+ monocytes in predicting inadequate response to ICB treatment and provides insights into the monocyte cell-intrinsic mechanisms of resistance to ICB therapy. We also propose a combined therapeutic approach to enhance ICB efficacy by targeting S100A9.
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APPLIED SURFACE SCIENCE
·
2020
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IF 6.182
Huiyong Li,Zemin Zheng,Mofan Liu,Hao Jiang,Dafeng Hu,Xudong Zhang,Lei Xia,Xuemin Geng,Jiangwei Lu,Xinran Cheng,Yanfen Wan,Peng Yang
A novel Pd nano-skeleton (Pd NSs) modified Bi 2 MoO 6 balls photocatalyst was prepared by a facile hydrothermal treatment. The characterization by multiple techniques demonstrated the excellent light absorption and effective photo-generated electron-hole pairs separation performance of the composite catalyst, which further proved its superior photocatalytic property. Compared to the pure Bi 2 MoO 6 nanosheets, carbon quantum dots (CQDs) modified Bi 2 MoO 6 balls and Pd nanoparticles (Pd NPs) modified Bi 2 MoO 6 balls catalysts, 1.3% Pd NSs@Bi 2 MoO 6 sample exhibited the optimal catalytic performance for removing methyl orange (MO), methylene blue (MB), K 2 Cr 2 O 7 , phenol and the simulated wastewater mixture formed by the first three above under the illumination of visible light. Above all, the degradation efficiency increased about 5 times that of the pure Bi 2 MoO 6 balls for the degradation of MO. This great improvement was mainly attributed to Pd NSs with many contact edges, which provided more active sites for the adsorption reaction of organic dye molecules, following its better near-infrared light absorption capacity in the catalytic system. The active species mainly involved in the reaction were verified by ESR technique and the trapping test, mainly involving O 2 − , holes, OH, etc., and a possible photocatalytic reaction mechanism and pollutant degradation pathway were also proposed.
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