PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2024
·
IF 4.2
Yao Yu,Xinru Li,Yiping Hou,Min Wei,Yiyun Qian,Yuxin Zhou,Min Yin,Yanqin Jiang,Pingping Song
Gray mold , caused by Botrytis cinerea is an intractable fungal disease that causes extensive damage to agricultural products. In the search for novel antifungal active ingredients, we discovered a linear pyranocoumarin Pd-D-V was effective against B. cinerea in both in vitro and in vivo assays. Furthermore, this study investigated the effects of Ca 2+ and the Ca 2+ -calcineurin signaling pathway on its antifungal activity against B. cinerea . The results indicated that Pd-D-V reduced the concentration of Ca 2+ in the mycelia of B. cinerea ; CaCl 2 , the Ca 2+ channel blocker verapamil , or the calcineurin inhibitor cyclosporin A could affect the sensitivity of Pd-D-V against B. cinerea ; the expression of genes ( Bccch1, Bcmid1, BccnA, Bccnb1, Bcpmc1, and Bcpmr1 ) of the Ca 2+ -calcineurin signaling pathway decreased after Pd-D-V treatment. In summary, Pd-D-V is compound for developing fungicides against B. cinerea . Pd-D-V can reduce intracellular Ca 2+ concentration and disturb Ca 2+ homeostasis . The Ca 2+ -calcineurin signaling pathway is important in the antifungal activity of Pd-D-V against B. cinerea .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Xu Linsheng,Qin Tian,Li Yuanfeng,Guo Hao,Hu Qiao,Xiong Jing,Ma Yaxiao,Zhang Peng,Yu Xiaolin,Liu Xi,Liu Yunpeng,Zhao Zhen,Zou Jianping,Wei Yuechang
Simultaneous oxidation of soot and CH 4 emitted from natural gas-diesel dual fuel engine is a new challenge. Herein, a robust catalyst of binary Ru-Pd components supported on three-dimensional ordered macro-mesoporous cerium-zirconium oxide (RuPd/3DOMM-CZO) is elaborately constructed. Ordered macro-mesopore structure in novel hierarchical porous cerium-zirconium oxide can respectively enhance mass transfer of soot and gaseous reactants, and binary Ru-Pd active components can improve activation for NO and CH 4 . RuPd/3DOMM-CZO catalyst exhibits excellent catalytic performance and stability during simultaneous soot and CH 4 oxidation. Based on the results of characterizations and theoretical calculations, Ru site in binary Ru-Pd components is responsible for catalyzing NO oxidation to NO 2 , which is key step of NO x -assisted soot oxidation mechanism, while Pd site can activate the C-H bond of CH 4 for boosting oxidation to CO 2 ; the catalytic cooperation between Ru and Pd atoms can promote the rate-determining step to realize simultaneous oxidation of soot and CH 4 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2025
·
IF 4.3
Chaofan Deng,Chun Cai
Pd–Cu bimetallic catalysts were successfully synthesized for the dehydrogenation of Bisphenol Z (BPZ) by an impregnation-reduction method. The obtained catalyst was studied by XRD, HRTEM, XPS, BET, and NH3-TPD techniques and effectively applied in the highly selective cleavage dehydrogenation of BPZ to give PPP > 99% yield at 270 °C and atmospheric pressure in the solvent-free condition. It was demonstrated that the “synergistic effect” of the bimetallic catalysts could effectively promote the cleavage dehydrogenation reaction. Pd species served as the primary active sites for the adsorption and dissociation of H* and the activation of C–H bonds, while the introduced Cu species accelerated the breaking process of the C–H bond. This catalyst demonstrated remarkable stability and could be reused over ten cycles without obvious decrease both in yield and selectivity. The likely reaction pathway was outlined to elucidate the cleavage dehydrogenation mechanism according to experimental results.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Huangtong Chen,Yifei Yang,Xiaofei Li,Huimei Duan
Defect engineering in oxide supports has emerged as a promising approach to enhance the surface chemical properties of active metals for methane catalytic oxidation. Herein, the N-doped Pd/Co 3 O 4 (Pd/N-Co 3 O 4 ) catalysts were successfully synthesized using ZIF-67 as a self-sacrificial template via an H 2 O-soaking treatment. Compared to conventional Pd/Co 3 O 4 catalysts (T 50 : 294 °C), the Pd/N-Co 3 O 4 catalysts exhibited superior catalytic activity (T 50 : 278 °C) and exceptional water resistance, with only a 6% activity loss at 350 °C in the presence of 5 vol% H 2 O, as opposed to a 56% loss for Pd/Co 3 O 4 catalysts. Detailed experimental characterizations revealed that N-doping significantly increased oxygen vacancy concentrations and surface lattice oxygen mobility while stabilizing Pd/PdO x active sites through the electronic metal-support interaction (EMSI) between Pd and N-Co 3 O 4 . In the Pd/N-Co 3 O 4 catalysts, the enhanced oxygen vacancies rendered the N-Co 3 O 4 support electron-rich, which in turn diminishes the electron transfer from Pd to N-Co 3 O 4 supports. This modulation effectively inhibited the excessive oxidation of Pd/PdO x active species into bulk PdO, thereby enhancing catalytic performance and water tolerance in methane oxidation. These findings provide valuable insights into the role of N-doped defect engineering in facilitating efficient methane catalytic combustion, highlighting the significance of EMSI and oxygen vacancies in optimizing catalyst performance.
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2025
·
IF 14.1
Zongge Li,Wenjie Tian,Kunsheng Hu,Yajie Guo,Xiaotan Tian,Wenjun Kang,Rui Li,Konggang Qu,Lei Wang,Fanpeng Meng,Huayang Zhang,Haibo Li
Here, a template-engaged galvanic replacement strategy is developed to construct hollow PdAg alloy nanotubes, where interfacial oxygen drives surface reconstruction and stabilizes quasi-single Pd active sites. The interplay of atomic-scale characterizations and theoretical calculations reveals that the oxygen-induced atomic rearrangement downshifts the Pd d -band center, optimizes the adsorption-desorption energetics of ORR intermediates, and lowers the energy barrier for * OH desorption. The optimized Pd 0.30 @Ag catalyst achieves an onset potential of 0.951 V and a half-wave potential of 0.868 V in alkaline media, surpassing commercial Pt/C even at an ultra-low Pd loading (3 wt.%). Furthermore, Pd 0.30 @Ag-based electrodes deliver outstanding performance in both zinc-air batteries (ZABs) and anion-exchange membrane fuel cells (AEMFCs), demonstrating high power densities, excellent cycling stability, and strong potential for scalable platinum-free energy conversion devices. This work provides a general strategy for engineering interface-confined active sites through surface reconstruction, offering new insights into the rational design of next-generation electrocatalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Lei Xia,Fang-Jing Liu,Meng-Jie Wang,Han-Bing Zhang,Jing Zhang,Yao Lu,Le-Le Qiu,Xian-Yong Wei,Yun-Peng Zhao
Production of cyclohexanone through selective hydrogenation of phenol under mild conditions has attracted much attention. Herein, a NaOH-modified Pd/WO 3 rich in oxygen vacancies for selective hydrogenation of phenol was prepared through impregnation method. The highest catalytic activity was exhibited on NaOH-Pd/WO 3 with 25 wt % addition of NaOH, and phenol achieved 100 % conversion at 90 °C and 0.7 MPa H 2 for 2 h, with a cyclohexanone selectivity of 95.3 %. The turnover frequency (TOF) of NaOH-Pd/WO 3 is approximately 3.5 times higher than that of the Pd/WO 3 . Detailed catalyst characterization and theoretical calculations reveal that the high activity and selectivity of NaOH-Pd/WO 3 for phenol hydrogenation to cyclohexanone are highly correlated with the concentration of oxygen vacancies in the catalyst. In-situ infrared and Raman analyses reveal that the OH - introduced by NaOH reacted with the lattice oxygen in WO 3 to abstract oxygen from the lattice, generating a significant number of oxygen vacancies. The possible reaction mechanisms for phenol hydrogenation were elucidated through combined density functional theory calculations and isotopic labeling experiments. This strategy of improving catalytic activity and selectivity by regulating the concentration of oxygen vacancies provides a theoretical basis for the design and optimization of industrial catalysts.
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 6
·544
·
IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2025
·
IF 12.6
Shijin Xu,Naidi Yang,Fangning Du,Ziying Zhang,Yin Zhang,Yixuan Zhang,Jiawei Liang,Yihan Zhao,Jiajun Zhang,Ziwei Zhang,Xiaoxuan Han,Zena Chen,Zhiqiang Zhou,Shu Zhang,Lin Li,Ying Lv
Pancreatic ductal adenocarcinoma (PDAC) remains one of the most lethal malignancies, marked by extensive stromal fibrosis and a profoundly immunosuppressive, immune-excluded tumor microenvironment (TME) that hampers the efficacy of immune checkpoint blockade. Although photodynamic therapy (PDT) can induce immunogenic cell death (ICD) and stimulate anti-tumor immunity, its effectiveness against PDAC is limited by insufficient immune activation and persistent stromal-mediated immunosuppression. To address these challenges, we develop a liposomal nanodrug that co-encapsulates a mitochondrial-targeted photosensitizer (MP) and a TGF-β receptor inhibitor (LY2109761) to synergize PDT with PD-1 checkpoint blockade. MP selectively accumulates in mitochondria and, upon light activation, amplifies mitochondrial reactive oxygen species production, inducing mitochondrial damage. This damage triggers the release of mitochondrial DNA and damage-associated molecular patterns, activating the STING pathway and eliciting potent ICD and anti-tumor immune responses. Simultaneously, liposome-mediated delivery of LY2109761 mitigates stromal desmoplasia and reverses TGF-β-driven immune suppression, enhancing effector T cell infiltration and activity. In murine PDAC models, this dual-action strategy transforms the immune-cold TME into an immune-inflamed phenotype, sensitizing tumors to PD-1 therapy and leading to pronounced tumor regression and prolonged survival. Our findings present a promising nanodrug-based approach to remodel the fibrotic and immunosuppressive TME of PDAC and enhance immunotherapeutic outcomes.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Binghui Zhou,Xinlei Ding,Yun Chen,Hanyang Wang,Yadong Liu,Chengfei Wang,Guangmei Bai,Wenge Qiu
The activation process is a key step in preparing porous carbon. Herein, three kinds of green activators were separately used to successfully prepare N-doped porous carbons through a two-step strategy: hydrothermal carbonization and chemical activation using microcrystalline cellulose as the carbon source and urea as the nitrogen source. Palladium was deposited on these N-doped microcrystalline cellulose-based carbons (NMC-X, where X represents the activator) via a traditional deposition–precipitation method, and the resulting Pd nanoparticle catalysts (Pd/NMC-X) showed high activity in the selective hydrogenation of quinoline under mild conditions, particularly Pd/NMC-ZC (ZC, zinc carbonate), which achieved complete conversion of quinoline within 100 min at 40 °C and 4 atm H2. Characterization results suggest that the high activity of Pd/NMC-ZC is mainly attributed to the special electronic structure of its Pd species, particularly the distribution of valence states and reducibility of Pd and the high hydrogen spillover capacity between Pd and NMC-ZC. The chemical activation by ZC leads to the formation of multiple defect sites on the carbon skeleton, modifying the carbon surface properties to enhance hydrogen spillover. This also provides an excellent environment for Pd nanoparticle anchoring, thus increasing the Pd-support interactions and regulating the electronic structure of Pd.
✓ 已验证
DOI
高影响因子
Science China-Technological Sciences
·
2025
·Vol. 68
·期 11
·1-11
·
IF 4.9
Zhang Ruixue,Miao Yu,Wei Shuhan,He Shuai,Li Jiayi,Sun Qiyan,Wang Lei,Xu Guang-rui
The chlorine evolution reaction (CER) serves as the cornerstone and crucial step in the conversion of chloride ions to chlorine gas, while accompanied by the occurrence of the oxygen evolution reaction (OER) in practical processes that lead to difficulty in achieving the purity requirements of the product Cl 2 for industrial applications. Pd-doped Co 3 O 4 nanoneedles (Pd-Co 3 O 4 NNs) were synthesized via hydrothermal-calcination methods. Pd sites induce electron delocalization, creating asymmetric active Co sites in Co 3 O 4 , enhancing CER performance. The unique nanoneedle arrays of the designed catalysts increase the number of exposed active sites, facilitating electron transfer and endowing the Pd-Co 3 O 4 NNs with a tip catalytic effect, further optimizing the catalytic reaction kinetics of CER with an overpotential of 118 mV at 100 mA cm −2 and a Tafel slope of 53.93 mV dec −1 . The density functional theory (DFT) calculations reveal that Pd incorporation at octahedral sites triggers charge redistribution and d-band center downshift, weakening intermediate adsorption and sustaining catalytic activity. This work offers new insights into noble-metal-doped spinel oxides, highlighting their potential for industrial applications.
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 5
·455
·
IF 4
Wenjun Lei,Yan Fu,Shipeng Gu,Shuaishuai Qiu,Jie Chang
Catalytic hydrogenolysis of lignin to produce high-value monophenols has emerged as a pivotal strategy in modern biorefineries. In this study, we synthesized spherical nitrogen-doped porous carbon (SNCB) materials by using Al/Co-BTC as a precursor, introducing melamine as a supplementary carbon and nitrogen source, and activating the material with NaOH solution. The SNCB framework was decorated with Cu-Pd bimetallic nanoparticles, exhibiting outstanding catalytic activity in the hydrogenolytic depolymerization of organosolv lignin. The Cu-Pd@SNCB catalyst exhibited remarkable activity, attributed to the hierarchical porous structure of SNCB that facilitated metal nanoparticle dispersion and reactant accessibility. The synergistic effect between Cu as the reactive site for reactant adsorption and Pd as the reactive site for H2adsorption enhanced the catalytic activity of the catalyst. Systematically optimized conditions (2 MPa H2, 270 °C, 3 h) yielded 43.02 wt% phenolic monomers, with 4-(3-hydroxypropyl)-2,6-dimethoxyphenol dominating the product profile at 46.3% selectivity. The catalyst and its reaction products were analyzed using advanced characterization techniques, including XPS, XRD, TEM, SEM, BET, GC-MS, GPC, 2D HSQC NMR, and FT-IR, to elucidate the reaction mechanism. The mechanism proceeds through: (1) nucleophilic substitution of the β-O-4 hydroxyl group by MeOH, followed by (2) simultaneous hydrogenolytic cleavage of Cβ-O and Cα-O bonds mediated by Cu-Pd@SNCB under H2atmosphere, which selectively produces 4-(3-hydroxypropyl)-2,6-dimethoxyphenol and 4-propyl-2,6-dimethoxyphenol. This study proposes a bimetallic synergistic mechanism, offering a general blueprint for developing selective lignin valorization catalysts.
✓ 已验证
产品关联
DOI
高影响因子
Acta Pharmaceutica Sinica B
·
2025
·
IF 14.6
Yuhong Wang,Lin Hu,Lei Wang,Chonghai Zhang,Wenhao Shen,Hongli Yang,Min Li,Xin Zhang,Mengmeng Xu,Muxing Zhang,Kai Yang,Xiaopeng Tian
Inflammatory bowel disease (IBD) is an autoimmune disorder involving complex immune regulation, where balancing localized and systemic immunosuppression is a key challenge. This study aimed to enhance the therapeutic efficacy by engineering the probiotic Escherichia coli Nissle 1917 (EcN). We removed endogenous plasmids pMUT1 and pMUT2 from wild-type EcN and expressed the mPD-L1 (19‒238 aa)-mFc fusion protein on the bacterial surface using a cytolysin A (ClyA) fragment. This modification stabilized mPD-L1 (19‒238 aa) protein expression and promoted its recruitment to outer membrane vesicles (OMVs). The engineered strain, EcNΔ pMUT1/2 -ClyA-mPD-L1-mFc (EcN-ePD-L1-mFc), features conditional ePD-L1-mFc expression under the araBAD promoter, enhancing gut-targeted release and reducing systemic side effects. This strain improved treatment targeting and efficiency by enabling direct ePD-L1-mFc interaction with immune cells at inflammation sites. OMVs from this strain induced Treg proliferation, inhibited effector T cell proliferation in vitro , and significantly improved intestinal inflammation and colonic epithelial barrier repair in vivo . Additionally, the bacterium restored intestinal microbiota balance, increasing Lactobacillaceae and reducing Bacteroides . This study highlights the engineered bacterium's potential for targeted intestinal immune modulation and offers a novel local IBD treatment approach with promising clinical prospects.
✓ 已验证
产品关联
DOI
PubMed
高影响因子