ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Zihan Wei,Zhenyin Hai,Mohammad Karbalai Akbari,Zhenting Zhao,Yongjiao Sun,Lachlan Hyde,Francis Verpoort,Jie Hu,Serge Zhuiykov
Surface functionalization of two-dimensional (2D) WO 3 nanofilms by noble metal (NM) nanoparticles (NM = Ag, Pt and Pd) was successfully achieved for the first time via combination of the atomic layer deposition (ALD) process and electrochemical deposition method. Deposited NM nanoparticles were uniformly in the particle size and homogeneously dispersed on the surface of 2D WO 3 . They represented electrochemically active metal-semiconductor hybrid nanocomposites with the larger electroactive area, and consequently, substantially enhanced the electrochemical H 2 O 2 detection of the device based on functionalized 2D WO 3 nanofilms. Functionalization by Ag was found to be more efficient compared to the same functionalization by Pt and Pd nanoparticles. Particularly, Ag 200 -WO 3 nanofilms exhibited the best electrochemical performance with a high sensitivity of 282 μA mM cm −2 , extremely wide linear H 2 O 2 concentrations range from 0.2 μM to 33.6 mM, a low detection limit of 0.1 μM, fast response time of 2 s and an excellent selectivity and long-term stability. Surface functionalization by NM nanoparticles approach has clearly demonstrated the great potential in the development of hybrid nanostructured electrode for various devices with enhanced electrochemical capabilities.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2017
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IF 3.154
Ahmed M. Senan,Sicheng Zhang,Miao Zeng,Zhuqi Chen,Guochuan Yin
Utilization of renewable biomass to partly replace the fossil resources in industrial applications has attracted attention due to the limited fossil feedstock with the increased environmental concerns. This work introduced a modified Wacker-type oxidation for transformation of unsaturated fatty acids/esters to the corresponding keto fatty acids/esters, in which Cu2+ cation was replaced with common nonredox metal ions, that is, a novel Pd(II)/Lewis acid (LA) catalyst. It was found that adding nonredox metal ions can effectively promote Pd(II)-catalyzed oxidation of unsaturated fatty acids/esters to the corresponding keto fatty acids/esters, even much better than Cu2+, and the promotional effect is highly dependent on the Lewis acidity of added nonredox metal ions. The improved catalytic efficiency is attributed to the formation of heterobimetallic Pd(II)/LA species, and the oxidation mechanism of this Pd(II)/LA catalyst is also briefly discussed.
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JOURNAL OF EXPERIMENTAL & CLINICAL CANCER RESEARCH
·
2025
·Vol. 44
·期 1
·1-25
·
IF 12.8
Wang Pengyu,Guo Weihua,Liu Shuyue,Li Shouyi,Li Jiaqi,Ding Bowen,Yin Fengyi,Yang Yang,Li Xingjiang,Cao Pei,Ma Chaozhe,Zhang Wanying,Song Yidan,Geng Yating,Liu Lantao,Hu Jing,Hao Jihui,Feng Yukuan
Background Copper accumulation triggers mitochondrial-driven cell death, known as cuproptosis, offering a promising mechanism for targeted cancer therapy. Recent studies have highlighted the critical role of intratumoral copper levels in regulating the expression of programmed cell death ligand-1 (PD-L1), suggesting that copper-induced cuproptosis not only enhances cancer cell death but may also amplify the effects of anti-PD-L1 antibodies (αPD-L1). However, in tumors where monotherapy with αPD-L1 shows limited efficacy, particularly in pancreatic ductal adenocarcinoma (PDAC), the role of copper-induced cuproptosis in enhancing αPD-L1 treatment efficacy and its underlying mechanisms remain unclear. Meanwhile, inadequate tumor drug accumulation and glycolysis significantly restrict the efficacy of cuproptosis. To address these challenges, we have synthesized a novel nanozyme, Pt@PCN-Cu, designed to stabilize intracellular copper accumulation and effectively induce cuproptosis. Additionally, we aim to determine whether this strong induction of cuproptosis can synergize with αPD-L1 to enhance cancer therapy, ultimately paving the way for novel strategies to improve PDAC treatment. Methods Pt@PCN-Cu was synthesized via a one-pot method, and its therapeutic potential was assessed in combination with αPD-L1 for the treatment of PDAC. Initially, the material’s properties were characterized, and its efficient cellular uptake was confirmed. Anti-tumor efficacy was evaluated by inducing cuproptosis in PDAC cell lines and xenograft models. RNA sequencing (RNA-seq) was utilized to identify key regulators involved in the modulation of PD-L1 expression by cuproptosis. Lastly, the therapeutic efficacy of Pt@PCN-Cu combined with αPD-L1 was evaluated in vivo, focusing on tumor growth inhibition and immune modulation within the tumor microenvironment (TME). Results Pt@PCN-Cu demonstrates excellent physicochemical properties and remarkable cascade catalytic activity, providing a solid foundation for further in vitro and in vivo studies. In vitro, Pt@PCN-Cu efficiently transports copper and induces cuproptosis primarily through mitochondrial dysfunction. Mechanistic studies show that Pt@PCN-Cu triggers the dissociation of hexokinase 2 (HK2) from mitochondria, leading to a reduction in HK2 activity. This decline in HK2 activity impairs glycolysis, a metabolic pathway essential for tumor energy metabolism, which in turn results in elevated PD-L1 levels. In vivo, Pt@PCN-Cu demonstrates excellent safety and accumulates at the tumor site in a subcutaneous PDAC mouse model, inducing cuproptosis. Moreover, the combination of Pt@PCN-Cu with αPD-L1 further enhanced its therapeutic efficacy and effectively reprogrammed the immunosuppressive TME. Conclusion This study presents strong evidence confirming the safety and therapeutic potential of Pt@PCN-Cu in PDAC treatment. Importantly, Pt@PCN-Cu not only induces cuproptosis but also significantly enhances antitumor efficacy in combination with αPD-L1 by regulating PD-L1 expression through HK2 modulation. These findings underscore a more effective and innovative approach for treating PDAC.
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Frontiers in Chemistry
·
2019
·
IF 3.782
Song Hongbing,Liu Zong,Gai Hengjun,Wang Yongjie,Qiao Lin,Zhong Caiyun,Yin Xiangyang,Xiao Meng
Introducing electron-rich nitrogen atoms to ordered mesoporous carbons (OMC) as supports for noble metal catalysts, not only improves the hydrophilic properties of a mesoporous carbon surface, but also enhances the coordination and binding abilities of metal ion. In the present work, nitrogen-doped ordered mesoporous carbons (NOMCs) were successfully fabricated via a facile hydrothermal self-assembly. The prepared NOMCs were characterized through powder X-ray diffraction (XRD), Raman spectroscopy, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption-desorption isotherm. The analyses demonstrated that the NOMCs prepared at a pyrolysis temperature of 750°C possessed an ordered 2D hexagonal mesoporous structure, a high graphitization degree, large surface area, and a well-distributed pore size. In particular, NOMCs could anchor Pd nanoparticles uniformly because of the introducing N atoms with strong electronegativity, which were selected as efficient catalysts for the partial oxidation of benzyl alcohol to benzaldehyde. Approximately 24.63% conversion with 85.71% selectivity to benzaldehyde was obtained without using any solvent by molecular O2 oxidation. Most importantly, the TOF value of the catalyst in the reaction system was up to 8698 h−1. After five runs reaction, TOF and selectivity of the catalyst remained essentially same. Hence, the proposed catalyst has a potential engineering application value.
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Molecular Catalysis
·
2021
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IF 5.062
Hanlin Huang,Jiajun Dai,Xiaobin Liu,Kok Bing Tan,Jiale Huang,Guowu Zhan,Qingbiao Li
In recent years, high value utilization of waste biomass has been a hot topic in scientific research. Herein, waste eggshell (ES) rich in sulfonic groups was utilized as a natural modified support to load Pd and Ag nanoparticles (NPs), leading to efficient Pd-Ag/ES catalysts for the catalytic hydrogenation of 1,3-butadiene. Through series of characterizations such as SEM, TEM, BET, XPS, and FTIR, it was found that the porous ES not only has hierarchical structures to facilitate the metal dispersion, but also interacts strongly with Pd and Ag NPs via the inherent surface sulfonic groups, which are responsible for the enhanced catalytic performance. The optimized Pd-Ag/ES catalyst exhibited butenes selectivity of 95.8% and 1,3-butadiene conversion of 95% at 45 °C with excellent stability for at least 30 h on-stream. Furthermore, the first-principles density functional theory (DFT) calculation and in situ DRIFTS were performed to explore the plausible mechanism underlying the enhanced catalytic performance due to sulfonic groups. It is suggested that the sulfonic groups can effectively reduce the adsorption energy of butenes and 1,3-butadiene on the surface of Pd NPs which are beneficial to the selectivity of butenes. This work exemplifies that the waste ES with inherent sulfonic groups can be used as excellent support materials for loading active metal nanoparticles for selective hydrogenation reactions. Collectively, we verified that biological waste like eggshell has a great potential in serving as catalyst carrier due to its unique advantages.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 32
·15789-15796
·
IF 9.931
Jiali Sheng,Jiahui Kang,Zhixiong Hu,Yan Yu,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
Exploring effective electrocatalysts is in urgent demand to boost their large-scale applications for direct ethanol fuel cells. Herein, for the first time, we report nanoparticle-assembled Pd nanocages with efficient catalytic activity towards ethanol electrochemical oxidation. The catalysts are prepared from the second template of a nanosheet surface of amorphous Co(OH)2 octahedral nanocages, which are prepared from the original template of octahedral Cu2O. These Pd octahedral nanocages exhibit a porous rough surface, which consists of smaller Pd nanoparticles, endowing them with highly active surface area and many active sites. For the electrochemical oxidation of ethanol, the Pd nanocages demonstrate superior activity (3765 mA mgPd−1), 4.8 times and 5.9 times those of commercial Pd/C and Pd nanocatalysts, respectively, prepared directly from an octahedral Cu2O original template. Furthermore, the Pd nanocages demonstrate excellent long-term durability.
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CHINESE JOURNAL OF CHEMISTRY
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2021
·Vol. 39
·期 10
·2745-2754
·
IF 6
Yinbing Tian,Zijie Tang,Yu Ru,Yuanyuan Wang,Liyi Dai
Main observation and conclusion Three diamines (1,8-diaminooctane/ p -phenylenediamine/biphenylenediamine) with different alkyl groups were used to synthesize the functionalized graphene networks. Pd as the common metal catalyst was used to explore the effects of alkyl types of diamines on anti-stacking, metal anchoring ability of functional graphene and hence the catalytic performance. The results were discussed by characterization of the material and its catalytic properties. All catalysts showed excellent catalytic performance on the Suzuki cross-coupling reaction with a high yield of up to 100%. The p -phenylenediamine and biphenylenediamine functionalized graphene with larger specific surface area was beneficial to improve the stability of the graphene catalyst and maintain good catalytic activity after 5 cycles. The Pd nanoparticles in 1,8-octanediamine materials have smaller size and a smaller loading with the same or even better catalytic performance than p -phenylenediamine, biphenylenediamine materials, due to the stronger electron donating ability of N of octanediamine than that of p -phenylenediamine.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 19
·5336-5344
·
IF 9.405
Da Yang,Huan Liu,Lei Liu,Wen-Di Guo,Yong Lu,Ye Liu
An amphiphilic tri-functional ligand (L1) containing a Lewis acidic phosphonium cation, a phosphino-fragment and a hydrophilic sulfonate anion (–SO3−) enabled Pd(OAc)2 to efficiently co-catalyze the hydroxycarbonylation of terminal alkynes towards α,β-unsaturated carboxylic acids. These incorporated functional groups synergistically promoted the reaction, which proved more effective than the ligands lacking –SO3− and/or phosphonium and the mechanical mixtures of the individual functional groups independently. The molecular structure of Pd-L1 indicated that –SO3− in L1 served as a secondary O-donor ligand with reversible coordinating ability, cooperating with the phosphino-fragment to stabilize the Pd-catalyst. The in situ FT-IR analysis verified that the formation and stability of Pd–H active species in charge of hydroxycarbonylation were dramatically facilitated by the presence of L1. It was believed that, over the L1-based Pd-catalyst, H2O was cooperatively activated by the Lewis acidic phosphonium via “acid–base pair” interaction (H2O → P(V)+) and by the hydrophilic SO3−via hydrogen bonding (SO3−⋯H2O), giving rise to the formation of dimeric and mono-nuclear Pd–H species driven by reversible SO3−-coordination. In addition, the L1-based Pd-catalyst could be immobilized in the ionic liquid [Bmim]NTf2 for six-run recycling uses without obvious activity loss and detectable metal leaching.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wanchen Zhu,Zhongyang Luo,Feiting Miao,Longyi Liu,Akira Nakayama
Biomass hydropyrolysis (HP) vapor upgrading (VU) is highly promising for producing sustainable aviation fuel, yet challenges remain. This study focused on PdMo/γ-Al 2 O 3 and Mo/γ-Al 2 O 3 catalyzed HP-VU of biomass in a pressurized continuous fixed-bed and the reaction mechanism. The results demonstrated that the introduction of Pd enhanced the hydrodeoxygenation activity through multiple effects, including the generation of surface acidic sites, the formation of oxygen vacancies, and the effect of hydrogen spillover. Beyond this, the effects of upgrading temperature and pressure on the catalytic performance of PdMo/γ-Al 2 O 3 were also investigated. Under optimal conditions of 400 °C and 1.0 MPa, the organic phase achieved a mass yield of 12.03 wt%, with the selectivity of C4+ aliphatic hydrocarbons and monocyclic aromatic hydrocarbons reaching 77.01 %, leading to an HHV of 42.41 MJ/kg and high mass balance (98.71 %). Density functional theory calculations further provided insights into the role of defect sites in facilitating C–O/C=O bond cleavage and the contribution of Pd sites to C C bond activation. By integrating theoretical calculations with model compound experiments, the study revealed the potential reaction pathways including hydrodeoxygenation, hydrogenation, and C C coupling. This study provides practical and theoretical insights into the bimetallic-catalyzed HP-VU process of biomass.
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Acta Pharmaceutica Sinica B
·
2025
·
IF 14.6
Chaoyan Yao,Lei Wang,Weidong Liu,Ning Shi,Ziling Liao,Yuxuan Fu,Jinhao Ouyang,Xuan Lei,Qianping Huang,Siyu Li,Yihua Zhouyang,Pinnan Zhao,Jie Wang,Hongjuan Xu,Wenhu Zhou,Xingjun Jiang,Xiang Gao,Caiping Ren,Longlong Luo
The effective treatment of nasopharyngeal carcinoma (NPC) is challenged by an immunosuppressive tumor microenvironment (TME) and insufficient immune effector cell activation. Herein, we design a synergistic tri-modal therapeutic strategy to overcome these barriers. This platform integrates: (1) a CD109-targeted liposomal doxorubicin (S3-Lip-DOX) for precise chemotherapy and induction of immunogenic cell death (ICD); (2) non-genetically engineered natural killer (NK) cells armed with dual aptamers (targeting CD109 and PD-L1) via bio-orthogonal chemistry for enhanced tumor recognition (S3-P-NK); and (3) an Fc-engineered anti-PD-L1 antibody (Atezolizumab/IgG1) that restores antibody-dependent cellular cytotoxicity (ADCC). Crucially, we uncovered a key mechanistic synergy: S3-Lip-DOX treatment, as a stress-adaptive response, upregulates PD-L1 expression on NPC cells. This finding provides a compelling rationale for the integration, turning a potential immune escape mechanism into a therapeutic vulnerability. The complete regimen, comprising S3-Lip-DOX, S3-P-NK, and Atezolizumab/IgG1, demonstrated potent synergistic antitumor effects in vitro and in vivo . This triple-combination therapy not only achieved significant tumor regression but also robustly reprogrammed the innate tumor microenvironment, evidenced by enhanced dendritic cell (DC) maturation and pro-inflammatory macrophage activation. This work establishes a mechanism-driven, modular therapeutic platform that effectively coordinates targeted chemotherapy with innate immunotherapy, holding significant translational potential for solid tumors.
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APPLIED SURFACE SCIENCE
·
2020
·
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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JOURNAL OF EXPERIMENTAL & CLINICAL CANCER RESEARCH
·
2024
·Vol. 43
·期 1
·1-22
·
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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