ACS Catalysis
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2024
·
IF 11.3
Xiaoliang Li,Liang Zhao,Mark Douthwaite,Kai Wang,Ouardia Akdim,Isaac T. Daniel,Rena Oh,Lei Liu,Zhe Wang,Fanhui Meng,Samuel Pattisson,Angeles López-Martin,Jian Yang,Xiaoyang Jerry Huang,Richard J. Lewis,Graham J. Hutchings
The spatial separation of Au and Pd nanoparticles supported on carbon has been demonstrated to be highly effective in facilitating aqueous-phase alcohol oxidation reactions, wherein OH– is the oxidant terminal for the oxidative dehydrogenation reaction. However, the application of this methodology in nonaqueous environments has not yet been explored. Supported alloyed Au–Pd nanoparticles are known to be highly active in the solvent-free oxidation of benzyl alcohol with oxygen as the terminal oxidant, leading to benzaldehyde by direct oxidation and toluene by disproportionation. Here, we show that by physically separating Au and Pd nanoparticles supported on carbon, the reaction rate for solvent-free benzyl alcohol oxidation can be further enhanced by coupling the oxidation and disproportionation reactions via H-transfer from Pd to Au.
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CURRENT CANCER DRUG TARGETS
·
2024
·Vol. 25
·期 3
·294-305
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IF 2.3
Yiping Zheng,Jianfeng Cai,Qiuhong Ji,Luanmei Liu,Kaijun Liao,Lie Dong,Jie Gao,Yinghui Huang
BackgroundLung cancer remains a major global health threat due to its complex microenvironment, particularly the role of neutrophils, which are crucial for tumor development and immune evasion mechanisms. This study aimed to delve into the impact of lung cancer cell-conditioned media on neutrophil functions and their potential implications for lung cancer progression.MethodsEmploying in vitro experimental models, this study has analyzed the effects of lung cancer cell-conditioned media on neutrophil IL-8 and IFN-γ secretion, apoptosis, PD-L1 expression, and T-cell proliferation by using techniques, such as ELISA, flow cytometry, immunofluorescence, and CFSE proliferation assay. The roles of IL-8/PD-L1 in regulating neutrophil functions were further explored using inhibitors for IL-8 and PD-L1.ResultsLung cancer cell lines were found to secrete higher levels of IL-8 compared to normal lung epithelial cells. The conditioned media from lung cancer cells significantly reduced apoptosis in neutrophils, increased PD-L1 expression, and suppressed T-cell proliferation and IFN-γ secretion. These effects were partially reversed in the presence of IL-8 inhibitors in Tumor Tissue Culture Supernatants (TTCS), while being further enhanced by IL-8. Both apoptosis and PD-L1 expression in neutrophils demonstrated dose-dependency to TTCS. Additionally, CFSE proliferation assay results further confirmed the inhibitory effect of lung cancer cell-conditioned media on T-cell proliferation.ConclusionThis study has revealed lung cancer cell-conditioned media to modulate neutrophil functions through regulating factors, such as IL-8, thereby affecting immune regulation and tumor progression in the lung cancer microenvironment.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2025
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IF 4.7
Mengdan Shen,Xi Han,Xixi Li,Jiayun Ji,Shunyao Zhu,Beihua Xu,Senlin Shi,Ting Zhang
In this study, emodin (ED) and polysialic acid (PSA) were synthesized into a compound called PSA-ED. The PSA-ED self-assembled into nanoparticles (PE-NS) using a nano-precipitation method. According to the results of particle size analyzer, the particle size of PE-NS was 180.7 ± 1.60 nm, the polydispersity index (PDI) was 0.263 ± 0.090, and the ζ potential was −17.1 ± 0.9 mV. In vitro cellular experiments confirmed that compared to free emodin, PE-NS exhibited significantly higher cellular uptake in RAW264.7 cells. In addition, in vivo imaging demonstrated enhanced fluorescence accumulation in tumors. This indicated that PE-NS possesses the ability to effectively target tumor-associated macrophages (TAMs). We conducted experiments using a mouse model of the B16F10 tumor, treating the mice with PD-1 antibody, PE-NS, and various doses of PE-NS + anti-PD-1 antibody, and compared them with untreated controls. In the PE-NS and anti-PD-1 antibody combination therapy group, there was a notable decrease in the proportion of M2-TAMs and CD4 + Fop3+ T cells, alongside a significant increase in the proportion of M1-TAMs and CD8+ T cells, resulting in an increased tumor inhibition rate. The combination of PE-NS and anti-PD-1 antibody exhibited synergistic antitumor activity, enhancing the effectiveness of PD-1 checkpoint blockers in the mouse melanoma models. In conclusion, the combination of PE-NS and anti-PD-1 antibody immunotherapy holds great promise in improving the therapeutic effects of melanoma treatment and may offer a novel strategy for clinical application.
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Nanomaterials
·
2024
·Vol. 14
·期 6
·512
·
IF 4.4
Yuan Chen,Jiaxing Wang,Daidi Chen,Boxi Wang,Jinchuan Wu,Rongrong Liu,Qingxin Li
Many studies have been conducted on the microbial reduction of Pd (II) to palladium nanoparticles (Pd-NPs) due to the environmental friendliness, low cost, and the decreased toxicity of Pd (II) ions. In this study, we investigate the reduction mechanism of Pd (II) byBacillus megateriumY-4 through proteomics. The data are available via ProteomeXchange with identifier PXD049711. Our results revealed thatB. megateriumY-4 may use the endogenous electron donor (NAD(P)H) generated by nirB, tdh, and fabG and reductase to reduce Pd (II) to Pd-NPs. The expression levels of fabG, tdh, gudB, and rocG that generate NAD(P)H were further increased, and the number of reduced Pd-NPs was further increased with the exogenous electron donor sodium formate. Endogenous electron mediators such as quinones and flavins inB. megateriumY-4 can further enhance Pd (II) reduction. The findings provided invaluable information regarding the reduction mechanism of Pd (II) byB. megateriumY-4 at the proteome level.
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ChemCatChem
·
2025
·
IF 3.9
Cheng-Long Li,Rui-Ping Zhang,Lu Hou,An-Hui Lu
Pd-catalyzed semihydrogenation of alkynols to enols is a pivotal industrial process for synthesizing fine chemicals like fragrances and vitamins. The selection of carbon-based supports is crucial due to their advantages in good chemical and thermal stability, tunable surface properties, and facile metal recovery via combustion. Herein, we constructed the wood-based monolithic carbon support with a sulfur-doped mesoporous carbon layer to anchor high-dispersed Pd nanoparticles. This mesoporous carbon layer was fabricated via co-polymerization of 2-thiophenemethanol and tetraethoxysilane monomers formed by decomposition of the tetrakis(2-thiophenemethoxy)silane on wood substrates, followed by pyrolysis, and removal of silica. The resultant Pd/C catalyst exhibited high catalytic activity (4323 mol mol Pd −1 h −1 ) and selectivity (93% at 99% conversion) under mild conditions (298 K, 2 bar H 2 ) in 2-methyl-3-butyn-2-ol (MBY) semihydrogenation. The thiophene-like sulfur and mesoporous framework synergistically promoted Pd dispersion, thereby boosting catalytic activity. Meanwhile, the electron-rich Pd 0 sites, which originated from electron donation of thiophene-like sulfur species, significantly enhanced catalytic selectivity. Additionally, the sulfur-modified monolithic catalyst presented good stability over five cycles and facile separation from the solution. It also displayed broad applicability in diverse alkynol semihydrogenation reactions, demonstrating high potential for liquid-phase catalytic applications. Graphical Surface sulfur-doped monolithic carbon with mesoporous structures is constructed to anchor high-dispersed Pd nanoparticles. Thiophene-like sulfur synergizes with mesopores to enhance Pd dispersions and donates electrons to form electron-enriched Pd sites, thereby boosting catalytic activity and selectivity. This monolithic design facilitates separation, demonstrating high potential for liquid-phase reactions.
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Science Bulletin
·
2025
·
IF 21.1
Xiangcheng Zhang,Silian Cheng,Xue Wen,Weiyao Hu,Ziyi Chen,Hongshuai Cao,Panzhe Qiao,Xue Li,Lizhi Zhang,Mingce Long
Hydrogen peroxide (H 2 O 2 ) photosynthesis from H 2 O and O 2 remains a significant challenge due to the sluggish hydrogen donation process, which stems from the high O–H bond dissociation energy of water. In this study, we propose an effective strategy to accelerate the water oxidation reaction (WOR) by anchoring single palladium atoms (Pd–CNO 2 ) onto a keto-anthraquinone covalent organic framework (KfAQ-Pd), achieving remarkable H 2 O 2 production rates of 3828 μmol h −1 g −1 under visible light irradiation ( λ > 420 nm) in neutral water. Both experimental observations and theoretical simulations reveal that the Pd–CNO 2 configuration induces an upward shift in the d-band center and enhances the hydrophilicity of KfAQ. This modification effectively disrupts the hydrogen-bond network within adsorbed water clusters, thereby promoting the cleavage of the dangling O–H bonds in H 2 O molecules and facilitating efficient hydrogen donation. The generated H 3 O + species are subsequently reduced in-situ by photogenerated electrons, leading to the hydrogenation of anthraquinone moieties and ultimately driving efficient H 2 O 2 photosynthesis. Overall, these findings highlight the pivotal role of single Pd atoms in enhancing water dissociation and hydrogen transfer, offering a promising new paradigm for solar-driven, environmentally friendly H 2 O 2 synthesis in neutral aqueous systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Qian Zhang,Yuanyu Shi,Xianjin Shi,Tingting Huang,Shuncheng Lee,Yu Huang,Jun-ji Cao
Photo-oxidative NO x removal often encountered with sluggish charge carrier separation kinetics and poor selectivity. Herein, Pd/ferroelectric Bi 4 Ti 3 O 12 nanoflakes (Pd/BTO NF) were constructed to investigate the photo-excited charge separation, O 2 activation and the generated reactive oxygen species (ROS) in dictating NO removal. Results showed that the depolarization field of ferroelectric BTO NF significantly promoted bulk charge separation, leading to boosted NO removal reaction kinetics (10 times higher) for Pd/BTO NF comparing with Pd/TiO 2 . Revealed by electronic paramagnetic resonance and radical scavenging tests, it is observed that the primary O 2 activation species differed among Pd, Ag and Pt supported BTO NF photocatalysts, which resulted in different selectivity. The underlying mechanism of NO photo-oxidative conversion pathway was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy. This work illustrate that metal/ferroelectric interfaces can be tuned to obtain differing O 2 activation species, and notable selectivity changes in photocatalysis mediated environmental remediation reactions.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Xin Li,Yue Ma,Xuning Wang,Jianguo Wu,Dong Cao,Daojian Cheng
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd 0 /Pd 2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C 3 N 4 –300 catalyst with a Pd 0 /Pd 2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd 0 and Pd 2+ in Pd/g–C 3 N 4 –300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
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BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Jian Gao,Jingyu Wu,Yuancai Chen
This study found that bio-Pd 0 nanoparticles could launch proton motive force (PMF)-mediated antibiotics efflux pump (AEP) to confer the detoxification capability on Citrobacter freundii , as evidenced by the highest sulfamethoxazole (SMX) specific degradation rate (81.7 μg L −1 mg −1 protein d −1 ) at high PMF (pH 6). The batch experiment and RT-qPCR results indicated that bio-Pd 0 activated the AcrB efflux pump through upregulating the AEP transcriptional regulation factor ramA (2.7–3.1 times), which benefited the intra/extracellular respiration and ATP production/utilization. Path analysis revealed that the prosperity of metabolic activity and extracellular electron output capacity enabled SMX biodegradation, mainly through the electron redistribution and energy optimization with the formate dehydrogenase/hydrogenase based Short-chain (FDH/Hase-S-chain). The upregulation of hypE (2.7–8.6 times) and atpD (1.9–2.3 times) genes encoding the Hase respiratory chain and the F-type ATP synthase, respectively, further supports this mechanism. These novel findings provided a new strategy to improve the biodegradation efficiency of antibiotics wastewater.
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Electrocatalysis
·
2024
·Vol. 15
·期 4
·281-290
·
IF 2.7
Xiang Qun,Wang Yizhong,Wang Shuang,Fu Xucheng,Gao Guiqi,Yan Ruiwen
In this work, the CeO 2 nanoparticles were dispersed onto the surface of graphene oxide (GO), followed by electrodeposition of Pt–Pd alloy nanoparticles on the CeO 2 surface to fabricate Pt–Pd@CeO 2 /graphene oxide composites (Pt–Pd@CeO 2 /GO). Morphological investigation was conducted using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The results of morphological characterization revealed that CeO 2 nanoparticles acted as cores, while Pt–Pd alloy nanoparticles formed shells. The electrocatalytic oxidation performance of Pt–Pd@CeO 2 /GO composites for methanol electro-oxidation reaction (MOR) was systematically investigated. The mass activity for MOR on Pt 1 Pd 1.3 @CeO 2 /GO electrocatalyst was 1128 mA·mg Pt+Pd −1 , which was 5.0-fold higher than that of Pt/C catalysts. The synergistic effect between Pt and Pd, along with the active oxygen-containing species of CeO 2 effectively enhanced catalytic activity. This work presents a novel approach to developing catalysts with high catalytic performance for MOR. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chao Feng,Yuxi Bi,Chong Chen,Yunxia Wang,Shuangju Li,Yuan Pan,Hongchuan Xin,Yukun Lu,Fang Liu,Xuebing Li,Yunqi Liu,Runduo Zhang,Zhong Wang
Photothermal synergistic low-temperature catalytic volatile organic compounds (VOCs) degradation has an advantage on energy efficiency and reduction of carbon emissions. Herein, an impregnation-pyrolysis-oxidation strategy was adopted to synthesize Pd/Mn 3 O 4 heterojunction catalyst. Under photothermal synergistic conditions, 0.60Pd/Mn 3 O 4 catalyst exhibited an excellent activity for propane total oxidation, with a T 90 value of 219.1 ℃, which was 115.3 ℃ lower than that of Mn 3 O 4 . Enhancement effect of the heterojunction structure on photothermal synergy was detected by various characterization techniques and density functional theory calculation. The presence of Pd species enhanced the low-temperature reducibility of Mn 3 O 4 . Meanwhile, O 2 molecules were more easily activated at the Pd sites and overflow to the surface of Mn 3 O 4 for reaction. Besides, the formation of p-n junction between Pd species and Mn 3 O 4 in heterojunction structure promoted the charge separation and the migration of carriers, and boosted the generation of oxygen free radical, resulting in a significant improvement in photothermal catalytic activity. Overall, this study provided new strategy and deep insight for constructing heterojunction to enhance photothermal catalytic performance of VOC elimination.
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ChemSusChem
·
2025
·
IF 6.6
Qian Jiang,Zuzhi Li,Javier Remón,Hui Xin,Zhicheng Jiang,Bi Shi
Finding new catalytic applications for tannin, a biomass resource, exploiting its structural features and renewable nature, helps contribute toward carbon neutrality in catalysis. In this study, novel Pd-supported, carbon-neutral catalysts have been synthesized using tannic acid. First, tannic acid was cross-linked and coated on the surface of nano-SiO2. This material was then subjected to controllable carbonization, with the temperature being optimized, to obtain the catalyst support SiO2@TA-T (T: carbonization temperature). Experimental results demonstrated that carbonizing at 400 °C remained part of the phenolic hydroxyls of tannin with satisfactory reducing ability. Meanwhile, the condensation and the deoxygenation of tannin increased the thermal stability of this support and introduced porous structures and abundant defect sites. This material was then used to adsorb and in situ reduce Pd2+ to develop Pd-based catalysts. To this end, this synthesized Pd/SiO2@TA-400 catalyst was then used to hydrogenate vanillin, with a conversion of 99% to vanillyl alcohol at a pressure of 0.5 MPa initial H2 and a temperature of 20°C for 60 min. Such remarkable results were corroborated in the hydrogenation of several lignin-derived aromatic aldehydes, with our catalyst achieving high conversion and outstanding recyclability (5 recycles).
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