Molecular Catalysis
·
2024
·
IF 3.9
Shengya Ge,Chenzhang Li,Peiyan Bi,Wei Hong
The operation of direct ethylene glycol fuel cells (DEGFCs) to generate electric energy from ethylene glycol rely on the effective electrocatalysts for the ethylene glycol oxidation reaction (EGOR). The fabrication of EGOR electrocatalysts with high activity, high durability and high resistance for corrosion, is essential important for the DEGFCs. Herein, we report a fabrication of Pd nanoparticles immobilized by the Ce-doped ZIF-67-derived carbon (Pd-CeO 2 /ZDC). The Pd nanoparticles are generated by the in-situ reduction reaction between the H 2 PdCl 4 and the Co nanoparticles formed during the ZIF-67 pyrolysis. Owe to the porous structure and N-doping inherited from the ZIF-67, the Pd and CeO 2 nanoparticles show a uniform distribution. Due to the enhanced EGOR electrooxidation kinetic promoted by the ZIF-67-derived support, the multiple-components and structure synergies, the resultant Pd-CeO 2 /ZDC catalyst affords a EGOR current density of 32.4 mA cm -2 , which is higher than the commercial Pd/C as well as the counterpart Pd/ZDC catalyst without CeO 2 . Furthermore, the Pd-CeO 2 /ZDC catalyst also present a better EGOR durability. This work provides a strategy for the design of EGOR catalyst with multiple-components and desired structure, which may inspire the new tactics for controllable design and synthesis of other electrocatalysts for various electrocatalysis.
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Oral Science
·
2024
·Vol. 16
·期 1
·1-13
·
IF 10.8
Li Shujin,Feng Tian,Liu Yuantong,Yang Qichao,Song An,Wang Shuo,Xie Jun,Zhang Junjie,Yuan Bifeng,Sun Zhijun
N 1 -methyladenosine (m 1 A) RNA methylation is critical for regulating mRNA translation; however, its role in the development, progression, and immunotherapy response of head and neck squamous cell carcinoma (HNSCC) remains largely unknown. Using Tgfbr1 and Pten conditional knockout (2cKO) mice, we found the neoplastic transformation of oral mucosa was accompanied by increased m 1 A modification levels. Analysis of m 1 A-associated genes identified TRMT61A as a key m 1 A writer linked to cancer progression and poor prognosis. Mechanistically, TRMT61A-mediated tRNA-m 1 A modification promotes MYC protein synthesis, upregulating programmed death-ligand 1 (PD-L1) expression. Moreover, m 1 A modification levels were also elevated in tumors treated with oncolytic herpes simplex virus (oHSV), contributing to reactive PD-L1 upregulation. Therapeutic m 1 A inhibition sustained oHSV-induced antitumor immunity and reduced tumor growth, representing a promising strategy to alleviate resistance. These findings indicate that m 1 A inhibition can prevent immune escape after oHSV therapy by reducing PD-L1 expression, providing a mutually reinforcing combination immunotherapy approach.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Lanlan Shi,Xiaojun Wang,Feike Zhang,Jingxian Li,Yuanming Liu,Weijie Fu,Shuyun Yao,Shiyu Wang,Kang Ji,Yingjie Ji,Zhiyu Yang,Liwen Zhang,Jiangzhou Xie,Yi-Ming Yan
Palladium metal catalysts have emerged as the preferred choice for alkaline formate oxidation reaction (FOR) due to their high activity. However, their strong binding with adsorbed H (Had) allows Had to occupy the active site, resulting in slow FOR kinetics. Herein, we developed a ZrO2/Pd/C catalyst to decrease the Had binding strength on Pd active sites, thereby enhancing the FOR in alkaline media. Through experimental investigations and density functional theory (DFT) calculations, we elucidated the relationship between the d-band center of Pd and hydrogen binding energy (HBE). Our findings reveal that electron transfer from ZrO2 to Pd, driven by the work function disparity, results in a downshift of the d-band center of Pd. This shift weakens the HBE at Pd active sites, facilitating the desorption of Had intermediates and thereby improving catalytic efficiency. As a result, the ZrO2/Pd/C catalyst demonstrated a 2.8-fold increase in activity over commercial Pd/C, exhibiting a lower peak potential and a significantly higher peak current of 1787 mA mg–1. This work advances our understanding of the interplay between electronic structure and catalytic performance, setting a benchmark for high-performance electrocatalysts in energy conversion technologies.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jun-Yang Yan,Gui-Ping Cao,Chun-Yan Cao,Peng Gao,Mustapha Sani Shehu,Hui Lv,Alaaddin M. M. Saeed
This work investigated the loading of active metals on monolithic carrier NCNTs@FN through simulation and characterization and found that the active metal (Pd) had a stronger binding with NCNTs and a more uniform dispersion. Meanwhile, the π–π stacking effect between NCNTs and polystyrene (PS) molecules is more significant than that between PS and CNTs, making PS more easily adsorbed. Therefore, the highly active catalyst Pd-NCNTs@FN was prepared. The hydrogenation degree of Pd-NCNTs@FN catalyzed PS reached 92.7%, significantly higher than that of Pd-CNTs@FN (78.1%) under the same conditions. Uniform experiments on PS hydrogenation kinetics were designed. Power law and hyperbolic kinetic models were established, and the corresponding parameters were calculated. From the models, it was found that whether H2 concentration reaches a critical value determines whether H2 pressure affects the hydrogenation rate. In addition, the adsorption of PS is the rate control step in the reaction. The activation energy of Pd-NCNTs@FN catalyzed PS hydrogenation is 47.326 kJ/mol, which is lower than those of other traditional powder heterogeneous catalysts (50–55 kJ/mol), demonstrating the excellent activity of the catalyst.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Ke Huang,Shicheng Yuan,Rongyan Mei,Ge Yang,Peng Bai,Hailing Guo,Chunzheng Wang,Svetlana Mintova
A chlorine-free catalyst consisting of zeolite Y modified with Pd (Pd/NaY) catalyst has been prepared and used in the indirect oxidative carbonylation of methanol to dimethyl carbonate (DMC). The activity and stability of the catalyst were further improved by introducing molybdenum into Pd/NaY using a top-down approach (Pd-Mo/NaY catalyst). The Pd-Mo/NaY catalyst exhibited higher stability compared to the Pd/NaY. A high CO conversion of 97% and DMC selectivity of 80% during a 30-hour catalytic test for the Pd-Mo/NaY were obtained. Furthermore, the incorporation of Mo was found to partially heal the silanols and hinder the aggregation of Pd in the Pd-Mo/NaY catalyst. The interactions between Mo and Pd increased the amount of active Pd 2+ species and enhanced the adsorption of CO reactant on the Pd-Mo/NaY catalyst. The key reaction intermediate of COOCH 3 * was captured by in situ diffuse reflectance infrared Fourier transform spectroscopy . The stabilization of active Pd 2+ species contributed to the enhanced catalytic activity of the Pd-Mo/NaY catalyst in the indirect oxidative carbonylation of methanol to DMC reaction.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yangzi Zheng,Jiapeng Huang,Ruiyun Guo,Tianou He,Yanan Li,Yaming Liu,Weicong Wang,Qi Zhan,Shangdong Ji,Mingshang Jin
The formic acid oxidation reaction (FAOR) in direct formic acid fuel cells (DFAFCs) relies heavily on the use of Pd catalysts. To improve the performance of DFAFCs, it is crucial to develop highly active and stable Pd catalysts for FAOR. In this work, we demonstrate a novel approach to enhance the electrocatalytic activity and stability of Pd nanocatalysts by incorporating a palladium phosphide (Pd-P) interlayer. The introduction of the Pd-P interlayer can facilitate electron transfer and enhance the vacancy formation energy of the active Pd sites on the surface of Pd@Pd-P@Pd nanocrystals. As a result, the Pd@Pd-P@Pd catalyst can exhibit exceptional long-term durability, with a mass activity of 4.56 A mg -1 Pd and a specific activity of 28.06 mA cm −2 towards FAOR, which are 11.5 and 18.1 times higher than those observed for the commercial Pd/C catalyst, respectively. By leveraging the unique properties of the interlayer in Pd nanocatalysts, this work opens up a promising pathway for enhancing the performance of catalysts in sustainable energy conversion systems.
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
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.
✓ 已验证
产品关联
DOI
高影响因子
CURRENT CANCER DRUG TARGETS
·
2024
·Vol. 25
·期 3
·294-305
·
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL IMMUNOPHARMACOLOGY
·
2025
·
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）