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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY · 2024 · IF 4.2

The effect of Ca2+-calcineurin signaling pathway on the antifungal activity of Pd-D-V against Botrytis cinerea

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 .

CAS / MDL: 52-53-9
研究领域: 植物病理学 · 分子生物学 · 真菌学
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Journal of Environmental Sciences · 2021 · IF 5.565

Influence of NOx on the activity of Pd/θ-Al2O3 catalyst for methane oxidation: Alleviation of transient deactivation

Chang Cui,Yan Zhang,Wenpo Shan,Yunbo Yu,Hong He

Alumina supported Pd catalyst (Pd/Al 2 O 3 ) is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900°C and isothermal experiments at 650°C were conducted to investigate the influence of NO x on transient deactivation of Pd/θ-Al 2 O 3 catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient deactivation in the cooling ramp from 800 to 500°C, which was resulted from the in situ formation of NO 2 during the process of methane oxidation. Over the Pd/θ-Al 2 O 3 , thermogravimetric analysis and O 2 temperature programmed oxidation measurements confirmed that transient deactivation was due to the decomposition of PdO particles and the hysteresis of Pd reoxidation, while the metal Pd entities were less active for methane oxidation than the PdO ones. CO pulse chemisorption and scanning transmission electron microscopy characterizations rule out the NO 2 effect on Pd size change. Powder X-ray diffraction and X-ray photoelectron spectroscopy characterizations were used to obtain palladium status of Pd/θ-Al 2 O 3 before and after reactions, indicating that in lean conditions at 650°C, the presence of NO 2 increases the content of active PdO on the catalyst surface, thus benefits methane oxidation. Homogeneous reaction between CH 4 , O 2 , and NO x may be partially responsible for the alleviation above 650°C. The interesting research of alleviation in transient deactivation by NO x , the components co-existing in exhausts, are of great significance for the application.

研究领域: 催化化学 · 环境科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Effective Inhibition of Ethane Generation on Fe5C2 Nanoparticles Doped with ppm Level of Pd for Selective Hydrogenation of Acetylene

Mingshuai Sun,Fumin Wang,Guojun Lv,Xubin Zhang

Overhydrogenation to ethane is most undesired in selective hydrogenation of acetylene. Monometallic Pd supported on common oxide supports such as alumina and silica suffers from susceptibility of ethane formation, and the ethylene selectivity is usually unsatisfactory. Herein, Fe5C2 was carefully synthesized and employed as a new kind support doped with a (5–600) ppm level of Pd for selective hydrogenation of acetylene. The catalyst with appropriate Pd loadings exhibited more efficient ethane suppression and much higher ethylene selectivity than the traditional α-Al2O3 supported Pd catalyst, with full acetylene conversion under 240 °C, and maintained good stability after a 200 h tolerance test. Characterization and DFT calculation results reveal that the excellent ethylene selectivity is mainly derived from the special interaction between Pd atoms and the Fe5C2 support. Hydrogenation of ethylene to ethane needs to cross extremely high activation energy barriers on the catalyst surface, and ethylene desorption more easily occurs on it. Doping the appropriate amount of Pd atoms on the Fe5C2 surface can increase the obstacle for polymerization and will cause the unsaturated C2 species to be more inclined to be hydrogenated into C2H4. This synergy effect also acts as a guide in alkane suppression for selective hydrogenation of other alkynes.

CAS / MDL: 1344-28-1 16940-66-2
研究领域: 化学工程 · 催化科学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2022 · IF 5.876

Preparation of Pd-ZIF-8 single-atom catalyst with supercritical CO2 deposition method

Jian-Lei Qi,Dan Zhou,Qin-Qin Xu,Jian-Zhong Yin,Kun-Peng Yu,Hai-Xin Sun

In recent years, single-atom catalysts (SAC) have emerged as a new frontier in the field of heterogeneous catalysis owing to their unique properties and minimized metal dosage. Herein, the Pd-ZIF-8 single-atom catalyst was successfully fabricated using ZIF-8 as support, and Pd(hfac) 2 as the precursor using the supercritical CO 2 deposition method. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC-HAADF-STEM) images confirmed the formation of uniformly dispersed Pd atoms. Supercritical CO 2 has the advantage of zero-surface tension and high diffusibility, it can carry the molecules of Pd precursor into the micropores of ZIF-8. The dissolution and diffusion of precursor were observed by a visual view cell and the mechanism of the preparation was analyzed. Finally, semi-hydrogenation of phenylacetylene to styrene was performed to evaluate the catalytic activity of the prepared Pd-ZIF-8 catalyst. The conversion rate of 80.7% and selectivity of 92.2% were obtained at 70 °C and 4 h in the semi-hydrogenation of phenylacetylene.

研究领域: 催化化学 · 材料科学 · 纳米技术
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Nanoscale · 2021 ·Vol. 13 ·期 5 ·3208-3213 · IF 7.79

Flexible synthesis of Au@Pd core–shell mesoporous nanoflowers for efficient methanol oxidation

Shuli Yin,Ziqiang Wang,Songliang Liu,Shiqian Jiao,Wenjing Tian,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang

The design of bimetallic core–shell nanostructures with mesoporous surfaces is considered significant to strengthen the catalytic activity and stability for direct methanol fuel cells. Here, we report a flexible method to synthesize Au@Pd core–shell mesoporous nanoflowers (Au@mPd NFs) with Au core coated with mesoporous Pd nano-petals, in which polymeric micelle-assembled structures are used as templates to induce the formation of mesopores. Benefiting from the electronic and structural effects, Au@mPd NFs show excellent electrocatalytic activity and stability for methanol oxidation reaction in alkaline electrolytes. This study demonstrates a versatile strategy for the fabrication of core–shell mesoporous nanoflowers with adjustable composition.

研究领域: 材料科学 · 化学工程 · 能源技术
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MICROPOROUS AND MESOPOROUS MATERIALS · 2020 · IF 4.551

Catalytic performance of morphology-controlled Pd/SBA-15 in hydrogenation of alkyl-anthraquinone

Yue Zhang,Li Wang,Nan Wang,Guohua Gao,Zhiyong Pan,Baoning Zong

Monodispersed mesoporous SBA-15 silica was synthesized by adding n -decane to conventional synthesis recipe. Pd catalysts for 2-alkyl-anthraquinone hydrogenation were then prepared on the as-synthesized SBA-15 and characterized by scanning and transmission electron micrographs, X-ray diffraction, XPS spectroscopy and N 2 adsorption-desorption. At the molar ratio of n -decane to P123 (C10/P123) ranging between 120 and 240, monodispersed SBA-15, together with the shortened length of pore channels, expanded size of mesopores and decreased proportion of micropores could be obtained. The Pd catalyst on SBA-15 synthesized with 240 in C10/P123 exhibited the superior catalytic performance. The initial hydrogenation rate of 2-ethyl-, tert-butyl- and amyl-anthraquinone increases by approximately 300%, 183% and 150% compared with that on SBA-15 synthesized using a recipe without n -decane, with the selectivity to active anthraquinone of >99%.

CAS / MDL: 12125-01-8
研究领域: 化学工程 · 材料科学 · 催化
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PLoS One · 2015 ·Vol. 10 ·期 7 ·e0131450 · IF 3.234

Biodegradation of polychlorinated biphenyls (PCBs) by the novel identified cyanobacterium Anabaena PD-1

Hangjun Zhang,Xiaojun Jiang,Liping Lu,Wenfeng Xiao

Polychlorinated biphenyls (PCBs), a class of hazardous pollutants, are difficult to dissipate in the natural environment. In this study, a cyanobacterial strain Anabaena PD-1 showed good resistance against PCB congeners. Compared to a control group, chlorophyll a content decreased 3.7% and 11.7% when Anabaena PD-1 was exposed to 2 and 5 mg/L PCBs for 7 d. This cyanobacterial strain was capable of decomposing PCB congeners which was conclusively proved by determination of chloride ion concentrations in chlorine-free medium. After 7 d, the chloride ion concentrations in PCB-treated groups (1, 2, 5 mg/L) were 3.55, 3.05, and 2.25 mg/L, respectively. The genetic information of strain PD-1 was obtained through 16S rRNA sequencing analysis. The GenBank accession number of 16S rRNA of Anabaena PD-1 was KF201693.1. Phylogenetic tree analysis clearly indicated that Anabaena PD-1 belonged to the genus Anabaena . The degradation half-life of Aroclor 1254 by Anabaena PD-1 was 11.36 d; the total degradation rate for Aroclor 1254 was 84.4% after 25 d. Less chlorinated PCB congeners were more likely to be degraded by Anabaena PD-1 in comparison with highly chlorinated congeners. Meta - and para -chlorines in trichlorodiphenyls and tetrachlorobiphenyls were more susceptible to dechlorination than ortho -chlorines during the PCB-degradation process by Anabaena PD-1. Furthermore, Anabaena PD-1 can decompose dioxin-like PCBs. The percent biodegradation of 12 dioxin-like PCBs by strain PD-1 ranged from 37.4% to 68.4% after 25 days. Results above demonstrate that Anabaena PD-1 is a PCB-degrader with great potential for the in situ bioremediation of PCB-contaminated paddy soils.

研究领域: 环境科学 · 微生物学
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CHINESE JOURNAL OF CATALYSIS · 2023 · IF 16.5

Enhanced performance of Pd-[DBU][Cl]/AC mercury-free catalysts in acetylene hydrochlorination

Xingzong Dong,Guangye Liu,Zhaoan Chen,Quan Zhang,Yunpeng Xu,Zhongmin Liu

Compared with the rapid deactivation of the Pd/AC catalyst, an eco-friendly Pd-[DBU][Cl]/AC ([DBU][Cl], 1,8-diazabicyclo[ 5.4.0 ]undec-7-ene hydrochloride) catalyst with enhanced stability was synthesized and applied in the hydrochlorination of acetylene. The Pd-20[DBU][Cl]/AC catalyst exhibits 96.7% acetylene conversion and 98.9% selectivity of vinyl chloride within the 24 h evaluation under the conditions of T = 180 °C, GHSV(C 2 H 2 ) = 360 h –1 and V (HCl)/ V (C 2 H 2 ) = 1.2. The enhanced stability of the Pd-[DBU][Cl]/AC catalyst is attributed to the prevention of the reduction of Pd(II) to Pd(0), the inhibition of the formation of coke deposition on the catalyst surface, and the reduction of the loss of Pd species during the reaction. TPD characterization and DFT theoretical simulations confirmed that the PdCl 2 -[DBU][Cl] complex has stronger adsorption of HCl and weaker adsorption of C 2 H 2 and C 2 H 3 Cl compared to PdCl 2 . Furthermore, the catalytic mechanism of acetylene hydrochlorination over the PdCl 2 and PdCl 2 -[DBU][Cl] site was put forward based on theoretical simulations. The good activity and stability of Pd-20[DBU][Cl]/AC in the 60 h lifetime test indicates that it is likely to be a promising alternative to HgCl 2 catalysts.

CAS / MDL: 6674-22-2 7647-10-1
研究领域: 催化化学 · 环境科学 · 材料科学
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CHINESE JOURNAL OF CHEMISTRY · 2013 ·Vol. 31 ·期 3 ·371-376 · IF 0.917

Study of the Transient Reactive Pd(IV) Intermediate in the Pd(OAc)2-Catalyzed Oxidative Coupling Reaction System by Electrospray Ionization Tandem Mass Spectrometry

Wei Zhu,Haoyang Wang,Haihui Peng,Guosheng Liu,Yinlong Guo

Pd-catalyzed oxidative coupling reaction was of great importance in the aromatic C  H activation and the formation of new C  O and C  C bonds. Sanford has pioneered practical, directed C  H activation reactions employing Pd(OAc) 2 as catalyst since 2004. However, until now, the speculated reactive Pd(IV) transient intermediates in these reactions have not been isolated or directly detected from reaction solution. Electrospray ionization tandem mass spectrometry (ESI-MS/MS) was used to intercept and characterize the reactive Pd(IV) transient intermediates in the solutions of Pd(OAc) 2 -catalyzed oxidative coupling reactions. In this study, the Pd(IV) transient intermediates were detected from the solution of Pd(OAc) 2 -catalyzed oxidative coupling reactions by ESI-MS and the MS/MS of the intercepted Pd(IV) transient intermediate in reaction system was the same with the synthesized authentic Pd(IV) complex. Our ESI-MS(/MS) studies confirmed the presence of Pd(IV) reaction transient intermediates. Most interestingly, the MS/MS of Pd(IV) transient intermediates showed the reductive elimination reactivity to Pd(II) complexes with new C  O bond formation into product in gas phase, which was consistent with the proposed reactivity of the Pd(IV) transient intermediates in solution.

研究领域: 有机化学 · 金属有机化学 · 分析化学 · 催化化学 · 质谱学
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Water · 2021 ·Vol. 13 ·期 11 ·1543 · IF 3.103

Removal of AOX in Activated Sludge of Industrial Chemical Dyestuff with Bimetallic Pd/Fe Particles

Cancan Xu,Rui Liu,Wei Zheng,Lichu Lin,Lvjun Chen

Pd/Fe bimetallic particles were synthesized by chemical deposition and used to remove absorbable organic halogens (AOX) in the activated sludge of a chemical dyestuff wastewater treatment plant. Bath experiments demonstrated that the Pd/Fe bimetallic particles could effectively remove AOX. It indicated several factors, such as Pd loading, the amount of Pd/Fe used, initial activated sludge pH, and reaction time, which could affect the removal effect. The results showed that increasing the Pd content in Pd/Fe particles, from 0.01 to 0.05 wt %, significantly increased the removal efficiency of AOX in activated sludge. The Pd/Fe particles had a much higher removal efficiency of AOX in the activated sludge than bare Fe particles. A slightly acidic condition with a Pd content of 0.05% and 10 g/L of Pd/Fe was beneficial to the process of removing AOX in activated sludge. In detail, the removal efficiency of AOX in the activated sludge could reach 50.7% after 15 days of reaction with 10 g/L of Pd/Fe (Pd loading 0.05 wt %) and at an initial pH of 6.0 during the experiments. It also showed that the control samples without Fe0and Fe/Pd additions only removed 7.9% of AOX under the same conditions. Meanwhile, the concentrations of AOX in the supernatant of activated sludge were lower than the initial AOX concentration in the supernatant during the activated sludge remediation with Pd/Fe bimetallic particles. The results indicated that the AOX removal from the activated sludge matrix might be mainly due to the Pd/Fe bimetallic particles, and not just by phase transfer.

研究领域: 环境科学 · 废水处理 · 材料科学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Amino acid (histidine) modified Pd/SiO2 catalyst with high activity for selective hydrogenation of acetylene

Qinglei Wu,Chenyang Shen,Chang-jun Liu

Suppressing the excessive hydrogenation capacity of palladium has great significance for selective hydrogenation of acetylene. Herein, an amino acid (histidine or His in abbreviation) modified Pd/SiO 2 catalyst (Pd-His/SiO 2 ) for selective hydrogenation of acetylene was prepared by incipient wetness impregnation, followed by hydrogen reduction at 240 °C. The intense interaction between Pd and histidine greatly affects the structure and properties of Pd-His/SiO 2 . The Pd nanoparticles are highly dispersed on the support with an average diameter of 1.0 nm and positively charged. The use of histidine weakens the adsorption of acetylene and ethylene on the metal. Especially, the adsorption of di-σ-bonded ethylene is significantly impaired on the catalyst, which is beneficial to improve the ethylene selectivity. The conversion of acetylene is up to 100.0 % at 160 °C on Pd-His/SiO 2 while the ethylene selectivity reaches 81.5 %. A 50-hour test at 160 °C confirms the good stability of Pd-His/SiO 2 .

研究领域: 催化化学 · 材料科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2017 · IF 5.401

Efficient hierarchical mixed Pd/SnO2 porous architecture deposited microheater for low power ethanol gas sensor

Li Xiao,Shengrui Xu,Geng Yu,Shantang Liu

A novel gas microsensor combining SnO 2 submicron/nanostructured porous sensitive film with Micro-Electro-Mechanical systems (MEMS) microheater was successfully fabricated. The film was made of hierarchically mixed Pd/SnO 2 (HM-PTO) composites composed of Pd/SnO 2 hollow submicrospheres (Pd/SnO 2 -HSs) and Pd/SnO 2 nanoparticles (Pd/SnO 2 -NPs) deposited on the microheater platform using the microdispensing method. The as-prepared HM-PTO sensors exhibited high sensitivities, fast response/recovery rates, good selectivity, reliable reversibility, and relevant stability towards ethanol at low power consumption. The resulting superior sensing performances were attributed to the unique hierarchical structure. The internal void architecture of Pd/SnO 2 -HSs provided large specific surface areas, proper mesopore size distribution, large number of active adsorption/interaction sites, as well as promoted the chemisorption and dissociation of gas molecules due Pd-doping to yield superior gas response. In particular, the nano-sized SnO 2 particles ensured the uniform deposition of the materials to yield enhanced local conductivities, and possibly faster phase transfer reactions responsible for the extremely good response/recovery performance. This simple fabrication procedure combined with high sensing performances look promising for the development of hierarchical morphologies of novel materials for gas sensing applications.

CAS / MDL: 18282-10-5
研究领域: 材料科学 · 传感器技术
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