CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xinyuan Zhou,Qiyan Sun,Xinlin Wang,Ruixue Zhang,Bin Li,Zexing Wu,Dehong Chen,Lei Wang,Guang-Rui Xu
Synthesis of cost-effective electrocatalysts for oxygen reduction reaction (ORR) has received wide attention due to their sluggish kinetics, which limits the development and application of fuel cell technique. In this work, we report a versatile synthetic approach to prepare a series of small-sized Ag@MNi (M = Pd, Pt, Rh, Ru) nanocrystals with core–shell structures by a simple solvothermal method. According to characterization analysis, surface segregation of Pd was proved in the outermost layer with the Pd-rich shell layer, which can regulate the adsorption energy of *OH. Electrochemical results show that the onset potential and half-wave potential of Ag@PdNi nanocrystals (Ag@PdNi NCs) are 1.005 and 0.913 V vs. RHE (reversible hydrogen electrode), respectively, with a Tafel slope of 55.31 mV dec -1 and strong ORR catalytic durability, which is similar to Ag@MNi (M = Pt, Rh, Ru) NCs and slightly higher than that of PdAg alloy nanoparticles (PdAg alloy NPs), PdNi alloy nanoparticles (PdNi alloy NPs), commercial Pd black and even commercial Pt/C, in alkaline medium. Density Functional (DFT) calculations show that the presence of Ag core effectively promotes the segregation of Pd atoms to the outer shell surface, where Ni provides better segregated substitution sites for Pd, which significantly improves the ORR activity and durability due to the electronic synergistic effect between Ag core nuclei and Pd shell can reduce the adsorption strength of OH ads .
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Yanle Li,Dong Liang,Taisheng Zhu,Yumiao Zhou,Rushui Zheng,Na Zhu,Yongxiang Li,Duanlin Cao
Escaping from conventional hazardous methods, an innovative, acidic-free approach for the synthesis of nitro-heterocycles was realized through photocatalytic nitration using Pd-doped g-C 3 N 4 . In this method, chlorate nitrate was initially utilized as a reagent. Spectral analysis and electronic microscopy confirmed the successful doping of Pd nanoparticles (NPs) onto the g-C 3 N 4 surface, which subsequently enhanced the photocatalytic performance. The photogenerated electrons and Pd NPs played pivotal roles in the production of nitro-products. The reactive intermediate, NO 2+ , derived from nitrate, can be captured and elucidated through the shifts in cyclic voltammetry (CV) curves. Herein, the synthesis of 2-nitropyrrole and 2,5-dinitropyrrole was achieved through the nitration of chlorate nitrate in a friendly manner. Moreover, the composite photocatalyst could be readily isolated and recycled in next four tests, demonstrating its practicality and sustainability in photocatalytic applications.
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RSC Advances
·
2024
·Vol. 14
·期 18
·12593-12599
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IF 3.9
Junwei Li,Hongshuai Yin,Sisi Liu,Chaofa Xu,Zhixiong Cai
The catalytic performance of a catalyst is significantly influenced by its ability to activate hydrogen. Constructing frustrated Lewis pairs (FLPs) with the capacity for hydrogen dissociation on non-reducible supports remains a formidable challenge. Herein, we employed a straightforward method to synthesize a layered AlOOH featuring abundant OH defects suitable for constructing solid surface frustrated Lewis pair (ssFLP). The results indicated that the AlOOH-80 (synthesized at 80 °C) possessed an appropriate crystalline structure conducive to generating numerous OH defects, which facilitated the formation of ssFLP. This was further evidenced by the minimal water adsorption in the AlOOH-80, inversely correlated with the quantity of defects in the catalyst. As expected, the Pd loaded onto AlOOH (Pd/AlOOH-80) exhibited excellent catalytic activity in hydrogenation reactions, attributed to abundant defects available for constructing ssFLP. Remarkably, the Pd/AlOOH-80 catalyst, with larger-sized Pd nanoparticles, displayed notably superior activity compared to commercial Pd/Al2O3 and Pd/C, both featuring smaller-sized Pd nanoparticles. Evidently, under the influence of ssFLP, the size effect of Pd nanoparticles did not dominate, highlighting the pivotal role of ssFLP in enhancing catalytic performance. This catalyst also exhibited exceptionally high stability, indicating its potential for industrial applications.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Mingxi Ma,Chao Yu,Hanyuan Liu,Xuepeng Lv,Haidong Zhu,Weiwei Tang,Gaojun Teng,Fei Xiong
Hepatocellular carcinoma (HCC) is a highly fatal malignant tumor. The clinical outcomes of vascular interventional therapy for HCC based on existing drug-eluting microspheres remain unsatisfactory. This study adopted a unique fabrication method to synthesize methacrylated carrageenan/gelatin hydrogel embolic microspheres (MCGs). The interpenetrating network formed by these two biocompatible and absorbable natural macromolecules endows MCGs with outstanding mechanical properties and vascular conformity. MCGs could be delivered through microcatheters smoothly, and they are provided in various sizes to accommodate different clinical requirements. Their in vivo degradation behavior is controlled and predictable. Due to the strong anionic nature of carrageenan, MCGs can efficiently load and sustainably release Lenvatinib, achieving the precise delivery of this antiangiogenic targeted drug in the tumor region. Animal models reveal that the microspheres block blood vessels effectively and MCGs allow for high-dose Lenvatinib to have prolonged contact with HCC. We also propose an HCC treatment strategy by combining PD-L1 inhibitors with MCGs carrying Lenvatinib. This combination therapy is safe and effective, and the additive and synergistic effects showed impressive antitumor potency and great clinical application potential.
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PubMed
高影响因子
CANCER RESEARCH
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2025
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IF 16.6
Zhang Jie,Chen Weiwu,Zhang Chen,He Qian,Wang Xudong,Han Jiayu,Gao Peng,Wang Kunyu,Xie Haoze,Gao Feng,Guo Yining,Guo Wenhao,Jiang Haofei,Le Jing,Zang Ruichen,Mo Sisi,Fan Haobo,Zhu Xiaoxiao,Jiang Xinrong,Gao Fengbin,Yu Yanlan,Ding Guoqing,Chen Yicheng
PD-1 restrains effective killing of cancer cells by the immune system and is predominantly located on the surface of T cells or other immune cells. However, cancer cells also express PD-1 to varying degrees, which is commonly associated with a poor prognosis. Here, we investigated the regulation and function of PD-1 expression in prostate cancer (PCa) and revealed the impact on the tumor microenvironment. PD-1 expression in cancer cells positively correlated with Gleason grade and metastasis but negatively correlated with CD8+ T cell infiltration in PCa patients. PCa cells secreted PD-1 in exosomes that enhanced the activity of myeloid-derived suppressor cells (MDSCs) by activating JAK/STAT3 signaling. The activated MDSCs in turn reduced the infiltration of CD8+ T cells within the tumor, promoting tumor immune evasion. The ubiquitin-specific protease USP7 induced deubiquitination and elevated the abundance of PD-1 in PCa, and USP7 inhibition sensitized PCa tumors to anti-PD-1 antibody treatment. Given the modest efficacy of current immunotherapeutic approaches for PCa, strategies to inhibit the secretion of PD-1-bearing exosomes or USP7 function may emerge as promising immunostimulatory interventions for treating PCa.
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INTERNATIONAL IMMUNOPHARMACOLOGY
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2025
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IF 4.7
Chunyu Qu,Hui Zhang,Minghao Sun,Siran Jin,Xiaodan Wu,Zhixiang Lan,Guanghui Tan,Zhiqiang Wang,Yujun Bao,Yingxue Jin
Immune checkpoint blockade (ICB) is a tumor therapy that leverages the activation mechanisms of T cells in the immune system. A key challenge in ICB is poor T-cell infiltration and low tumor immunogenicity. Immunogenic cell death (ICD) can increase tumor immunogenicity and make tumors more sensitive to ICB. Programmed death ligand 1 (PD-L1) a major target for ICB. In this paper, a novel carbon nitride/methyl pyrophaeophorbide a‑copper/folate (abbreviated as CNMCF) nanocomposite was prepared for induced ICD. In CNMCF nanostructures, methyl pyrophaeophorbide a (MPPa) serves as the photodynamic therapy (PDT) agent, and copper ion serves as the chemodynamic therapy (CDT) agent. CNMCF not only induced ICD, but also alleviated tumor hypoxia. This led to down-regulation of hypoxia-inducing factor (HIF-1 α ) and PD-L1, promoted T lymphocyte invasion, effectively enhanced tumor immunogenicity, and elicited strong anti-tumor immune response, thereby suppressing primary tumor growth and metastasis. This research expanded the application of natural chlorophyll derivatives and C 3 N 4 -based drug delivery systems in cancer immunotherapy.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Fukun Lei,Zhuaxicairang Niu,Congmei Chen,Wenjing Sun,Maofei Ran
The sustainable application of heterogeneous palladium (Pd) catalysts in Heck coupling is hindered by nanoparticle (NPs) aggregation and leaching. Herein, we propose a strategy of rationally designing the local coordination environment of the support to precisely anchor Pd species. Through systematic computational screening of various doped configurations (C/O doping with different sites and concentrations), we discovered that constructing a BO3 local structure in hexagonal boron nitride optimally modulates the charge environment of adjacent boron sites, thereby creating strong anchoring sites for Pd NPs. This significantly enhances metal-support interaction (MSI) and effectively suppresses Pd migration and aggregation. Guided by this theoretical prediction, we successfully synthesized a BNO-700-Air support enriched with local BO3 local structures via controlled thermal calculation and air oxidation. The resulting Pd catalyst achieves ultrahigh dispersion of Pd NPs with an average size of 2.66 nm. In the Heck reaction of iodobenzene and methyl acrylate, it achieves 90 % conversion within 90 min and a low activation energy of 76.03 kJ/mol, outperforming all other examined samples. Moreover, the catalyst maintains stable activity over 10 consecutive cycles, as the BO3-rich environment stabilizes Pd NPs against initial aggregation and provides dynamic anchoring during “leaching-redeposition” process, thereby sustaining high dispersion throughout the cycling process. Substrate scope experiments further demonstrate its broad applicability. This study provides important theoretical and experimental foundations for designing highly active and stable Heck reaction catalysts.
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高影响因子
Food & Function
·
2019
·Vol. 11
·期 1
·456-471
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IF 3.241
Manling Hu,Jing Yang,Linlin Qu,Xuqian Deng,Zhiguang Duan,Rongzhan Fu,Lihua Liang,Daidi Fan
Ginsenoside Rk1 is a substance derived from ginseng and exhibits various activities such as anti-diabetic, anti-inflammatory and anti-cancer effects; however, its anti-tumor effect and target signaling mechanism in lung adenocarcinoma are not well understood. Here, we show that Rk1, a natural drug product, can function as an antitumor modulator that induces apoptosis in lung adenocarcinoma cells by inhibiting NF-κB transcription and triggering cell cycle arrest. Mechanistically, Rk1 suppressed the proliferation and clonal formation of two lung adenocarcinoma cell lines (A549 and PC9) in vitro and caused G1 phase cell arrest. In the A549 xenograft model, Rk1 significantly inhibited tumor growth and had few toxic side effects on normal organs. Western blotting results showed that Rk1 increased the protein expression of Bax, cleaved caspase-3, -8, and -9, and PARP, decreased the expression of Bcl-2 and blocked the NF-κB signaling pathway. Furthermore, ginsenoside Rk1 also reduced the high expression of PD-L1 in lung adenocarcinoma cells by inhibiting NF-κB signaling. These data revealed a previously unreported antitumor mechanism of Rk1, providing new ideas and an experimental basis for further study of the mechanism of action of Rk1 in lung adenocarcinoma.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Tianjiao Meng,Huixian Jia,Siying An,Huan Wang,Xinjian Yang,Yufan Zhang
Herein, a Pd nanoparticles-DNA layered nanoreticulation (Pd NPs-DNA LNR) sensor was assembled to a graphene oxide (GO)-modified electrode by catalytic hairpin assembly (CHA) and a self-assembly process. In this process, GO was modified on the electrode surface to provide -COOH sites for DNA bonding. Moreover, with the CHA circular amplification strategy, many single DNA1 were exposed to be able to be bound with Pd-DNA2 for the formation of the Pd NPs-DNA LNR, which enabled the ultrasensitive detection of microRNA-21 (miR-21) with a low limit of detection 63.1 aM. This strategy combines the amplification technology of CHA and Pd NPs-DNA LNR with Pd NPs. Such a layered nanoreticulation material can support abundant Pd NPs to avoid aggregation and obtain enhanced electrochemical signals. Significantly, this method can be successfully applied in tumor cell lysates and provides a neoteric channel for early disease diagnosis.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Ting Liu,Yinghui Sun,Bo Jiang,Wei Guo,Wei Qin,Yiming Xie,Bo Zhao,Liang Zhao,Zhiqiang Liang,Lin Jiang
The large amount of 4-nitrophenol (4-NP) wastewater produced by the chemical industry has received increased concern over the growing risk of environmental pollution. The ability to catalyze the reduction of highly concentrated 4-NP wastewater is highly desirable for the practical treatment of industrial wastewater, yet it remains a significant challenge. Herein, we report Pd nanoparticle-decorated 3D-printed hierarchically porous TiO2 scaffolds (Pd/TiO2 scaffolds) for the efficient reduction of highly concentrated 4-NP wastewater (2 g·L–1, ∼14.38 mM). The millimeter-sized interconnected channels in the scaffolds are conducive to rapid mass and ion transportation; meanwhile, the abundant micrometer- and nanometer-sized pores on the surface of the scaffolds offer adequate anchoring sites for Pd nanoparticles. The turnover frequency of the hierarchically porous Pd/TiO2 scaffold (16 layers) is up to 2.69 min–1, which is 1063 times higher than that of the Pd/TiO2-bulk material with the same size (0.00253 min–1). Importantly, no obvious deactivation of the catalytic activity is observed even after 20 cycles of catalytic reduction of 4-NP, showing excellent catalytic stability and reusability. Our strategy of loading the nanostructured catalyst on 3D-printable hierarchically porous structures put forward a flexible and versatile approach for boosting the catalytic performance of the catalysts, including catalytic activity, stability, and reusability, which can help promote their practical application in industry.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiaoliang Li,Jiangjiang Feng,Michal Perdjon,Rena Oh,Wei Zhao,Xiaoyang Huang,Shusen Liu
Au-Pd bimetallic nanoparticles immobilized on series of CeO 2 supports with different morphologies, e.g. , rod, cube, and polyhedrons were prepared through the deposition-precipitation method with a consequent investigation on their catalytic performances for benzyl alcohol oxidation in the absence of solvent. The experimental results exhibited that the morphology of CeO 2 has a markedly impact on the catalytic performance of Au-Pd/CeO 2 . In which Au-Pd supported on CeO 2 rod could achieve higher benzyl alcohol conversion than that supported on CeO 2 polyhedrons and CeO 2 cube, however, CeO 2 cube supported Au-Pd showed the highest selectivity towards the production of benzaldehyde. ICP-AES, XRD, Raman, N 2 -BET, TEM, HAADF-STEM, and XPS were conducted to characterize the catalysts. The results revealed that the excellent behavior of Au-Pd/CeO 2 -rod in benzyl alcohol oxidation was closely related with the smaller size of CeO 2 particle, the higher concentration of oxygen defects in support and the higher number of Ce 3+ and Pd 2+ species on the catalyst surface. The present study on the morphologies of CeO 2 support in solvent-free benzyl alcohol oxidation would offer a notable approach for the future catalyst design.
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高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Zonggao Hu,Guoli Zhou,Li Xu,Jinghe Yang,Bing Zhang,Xu Xiang
The heterogeneous catalysts based on ternary Pd/CeO 2 -nitrogen-doped graphene (NG) were prepared and utilized for solvent-free aerobic oxidation of benzyl alcohol to benzaldehyde in the presence of green oxidant O 2 . Characterization results revealed that CeO 2 dramatically enhanced the dispersion of Pd nanoparticles, reduced their particle size and inhibited the Pd oxidation formation. With high lattice oxygen storage capability of CeO 2 , excellent electrical conductivity of NG and high catalytic activity of Pd, the ternary catalyst was designed by combining the complementary superiorities of these three components. The ternary composite Pd/5CeO 2 -NG exhibited significantly higher catalytic activity with turnover frequency (TOF) of 30.74 s −1 for solvent-free aerobic oxidation of benzyl alcohol compared with the corresponding binary composites including 5CeO 2 -NG, Pd/NG and Pd/CeO 2 , verifying the synergistic effect among Pd, CeO 2 and NG. The ternary composite was stable and could be recycled up to 6 times without remarkable loss in the activity and selectivity towards benzaldehyde. Owing to its excellent activity, high selectivity, and exceptional stability and recyclability, the Pd/CeO 2 -NG composite has great application potential in the fields of organic synthesis, electrochemical biosensors and fuel cells.
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