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Catalysts · 2021 ·Vol. 11 ·期 5 ·543 · IF 4.146

Electron-Enriched Pd Nanoparticles for Selective Hydrogenation of Halonitrobenzenes to Haloanilines

Zechen Liang,Mingkai Zhang,Sai Zhang,Yongquan Qu

Selective hydrogenation of halonitrobenzenes into haloanilines represents a green process to replace the environmentally unfriendly non-catalytic chemical reduction process in industry. However, this transformation often suffers from serious dehalogenation due to the easy break of carbon-halogen bonds on metal surfaces. Modulations of the electronic structure of the supported Pd nanoparticles on Lewis-basic layered double hydroxides have been demonstrated to promote catalytic activity and selectivity for hydrogenation of halonitrobenzenes into haloanilines. Mechanism studies suggest that Pd with the enhanced electron density not only improves the capability for hydrogen activation, but also generates the partially negative-charged hydrogen species to suppress the electrophilic attack on the carbon-halogen bond and avoid the dehalogenation.Keywords:Pd nanoparticles;hydrogenation;halonitrobenzenes;haloanilines

CAS / MDL: 121-73-3
研究领域: 化学 · 催化材料科学
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ACS Applied Materials & Interfaces · 2018 · IF 8.097

Flowerlike NiCo2S4 Hollow Sub-Microspheres with Mesoporous Nanoshells Support Pd Nanoparticles for Enhanced Hydrogen Evolution Reaction Electrocatalysis in Both Acidic and Alkaline Conditions

Guoqing Sheng,Jiahui Chen,Yunming Li,Huangqing Ye,Zhixiong Hu,Xian-Zhu Fu,Rong Sun,Weixin Huang,Ching-Ping Wong

Flowerlike NiCo2S4 hollow sub-microspheres are synthesized through Cu2O templates to support Pd nanoparticles as high-efficiency catalysts for the hydrogen evolution reaction (HER). The diameter and shell size of NiCo2S4 hollow sub-microspheres are about 400 and 16 nm, respectively. In addition, the surface of the shells is constructed by petallike nanosheets. About 3 nm Pd particles uniformly incorporate with the flowerlike NiCo2S4 hollow sub-microsphere to form the NiCo2S4/Pd heterostructure. The NiCo2S4/Pd catalysts exhibit significantly lower overpotential of only 87 and 83 mV at 10 mA/cm2 for the HER in both acidic and alkaline conditions, respectively, relative to NiCo2S4 (247, 226 mV) and Pd (175, 385 mV) catalysts. Besides, the NiCo2S4/Pd catalysts also exhibit excellent stability of HER in these two conditions. The superior HER performance of NiCo2S4/Pd might be resulted from the unique architecture of metal nanoparticles anchored on the bimetallic sulfide flowerlike hollow sub-microspheres, which could provide high surface area, lots of active sites, strong synergetic effect, and stable structure.

CAS / MDL: 13820-53-6
研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Excellent catalytic activity and water resistance of UiO-66-supported highly dispersed Pd nanoparticles for toluene catalytic oxidation

Fukun Bi,Xiaodong Zhang,Jinfeng Chen,Yang Yang,Yuxin Wang

The highly dispersed Pd nanoparticles supported UiO-66 catalysts were successfully prepared via ethylene glycol reduction method (Pd-U-EG). And their catalytic performances were evaluated by toluene degradation. A series of characterization methods were carried out to characterize the physicochemical properties of the samples. During the effect of high weight hourly space velocity, stability and reusability test, the catalytic activity of Pd-U-EG remains unchanged, which also indicated good catalytic performance. More importantly, water resistance test (10-20 vol.% water) indicated that Pd-U-EG had a great water resistance. The study of toluene-TPD, toluene-TPSR and in-situ DRIFTS at different temperatures under different conditions over Pd-U-EG indicated the role of H 2 O. The introduction of H 2 O at low temperature was conducive to the adsorption of toluene, but inhibited the degradation of toluene. Differently, the H 2 O presence at high temperature was favorable to toluene degradation. In addition, toluene degradation mechanism was also revealed.

研究领域: 材料科学 · 催化化学
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BIORESOURCE TECHNOLOGY · 2025 · IF 9

Promoted sulfamethoxazole extracellular biodegradation in Citrobacter freundii JH@Pd by launching AcrB efflux pump

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.

CAS / MDL: 13820-53-6 723-46-6
研究领域: 微生物学 · 环境科学
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IET Nanobiotechnology · 2018 ·Vol. 12 ·期 4 ·441-445 · IF 2.059

Dual application of Shewanella oneidensis MR-1 in green biosynthesis of Pd nanoparticles supported on TiO2 nanotubes and assisted photocatalytic degradation of methylene blue

Xiaojie Song,Xianyang Shi,Mi Yang

Biosynthesised nanocomposites have attracted growing interests attributed to their ‘green’ synthesis nature in recent years. Shewanella oneidensis MR-1, a dissimilatory metal-reducing bacterium, was used to reduce palladium (II) nitrate to palladium (0) nanoparticles (Pd NPs) under anaerobic conditions, resulting in the in situ formation of Pd NPs immobilised on TiO 2 nanotubes (TNTs) (Pd/TNTs nanocomposites). The Pd/TNTs nanocomposites were characterised by transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, energy dispersive X-ray, and electron spin resonance, respectively. The results indicated that Pd NPs are successfully grown on the TNTs without aggregation. Photocatalytic degradation of methylene blue (MB) by Pd/TNTs nanocomposites under simulated sunlight was also investigated. Pd/TNTs nanocomposites had photocatalytic efficiency superior to that of single TiO 2 nanomaterials. The photocatalytic activity of Pd/TNTs nanocomposites can be enhanced by S. oneidensis MR-1. The results showed that after only 10 min, the degradation ratio of MB reached 98.7% by Pd/TNTs nanocomposites when simultaneously assisted with S. oneidensis MR-1.

CAS / MDL: 13463-67-7 10102-05-3
研究领域: 环境科学 · 材料科学 · 微生物学
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JOURNAL OF CATALYSIS · 2019 · IF 7.723

Insight into synergetic mechanism of Au@Pd and oxygen vacancy sites for coupling light-driven H2O oxidation and CO2 reduction

Jiaxuan Fan,Lingxiang Cheng,Yanan Liu,Yufei He,Yanfei Wang,Dianqing Li,Junting Feng

Photocatalytic reduction of CO 2 with H 2 O into CH 4 is a promising way to realize solar energy utilization and CO 2 conversion, in which the key issue is how to enhance and couple CO 2 reduction as well as H 2 O oxidation. In this work, we precisely fabricated a binary functional photocatalyst by loading Au@Pd nanoparticles onto V O -rich TiO 2 through a surfactant-free deposition-reduction method, whose fine structure was confirmed by aberration-corrected HAADF-STEM, EELS, EPR and XPS. Combining photocatalytic performance with a series of in situ FTIR measurements, we clarified the role of metallic sites and semiconductor support in coupling CO 2 reduction and H 2 O oxidation. Specifically, H 2 O oxidation process was facilitated by the V O -rich TiO 2 to contribute more protons, followed by the activation of CO 2 and protons primarily by the metallic Au@Pd sites to form the surface bounded Au@Pd-CO 2 − and Au@Pd-H species. By adjusting the ratio of Au@Pd nanoparticles and V O concentration to manipulate the Au@Pd-CO 2 − /Au@Pd-H ratio, CH 4 yield of 26.32 μmol/(g·h) and selectivity of electron toward CH 4 of 96% can be observed with minimal concomitant H 2 generation. These findings could open a feasible and universal route to enhance the photocatalytic efficiency of CO 2 conversion.

研究领域: 材料科学 · 环境科学 · 化学
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SENSORS · 2024 ·Vol. 24 ·期 7 ·2110 · IF 3.4

Enhanced Acetone Sensing Properties Based on Au-Pd Decorated ZnO Nanorod Gas Sensor

Yinfeng Shen,Yiping Liu,Chao Fan,Qudong Wang,Ming Li,Zhi Yang,Liming Gao

The mature processes of metal oxide semiconductors (MOS) have attracted considerable interest. However, the low sensitivity of metal oxide semiconductor gas sensors is still challenging, and constrains its practical applications. Bimetallic nanoparticles are of interest owing to their excellent catalytic properties. This excellent feature of bimetallic nanoparticles can solve the problems existing in MOS gas sensors, such as the low response, high operating temperature and slow response time. To enhance acetone sensing performance, we successfully synthesized Au-Pd/ZnO nanorods. In this work, we discovered that Au-Pd nanoparticles modified on ZnO nanorods can remarkably enhance sensor response. The Au-Pd/ZnO gas sensor has long-term stability and an excellent response/recovery process. This excellent sensing performance is attributed to the synergistic catalytic effect of bimetallic AuPd nanoparticles. Moreover, the electronic and chemical sensitization of noble metals also makes a great contribution. This work presents a simple method for preparing Au-Pd/ZnO nanorods and provides a new solution for the detection of acetone based on metal oxide semiconductor.

CAS / MDL: 5970-45-6
研究领域: 材料科学 · 传感器技术 · 化学工程
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MATERIALS RESEARCH BULLETIN · 2016 · IF 2.435

Synthesis of heterostructured Pd@TiO2/TiOF2 nanohybrids with enhanced photocatalytic performance

Xixia Zhao,Guijuan Wei,Junxue Liu,Zhaojie Wang,Changhua An,Jun Zhang

TiO 2 /TiOF 2 heterostructured nanocomposites has been synthesized through a solvothermal method and characterized by X-ray diffraction, scanning electronic microscopy, transmission electronic microscopy, nitrogen adsorption–desorption isotherms, UV–vis and photo-luminescent spectroscopy. It was found that, compared with single TiOF 2 or TiO 2 , the as-prepared TiO 2 /TiOF 2 nanocomposites exhibited superior photoactivity towards the degradation of organic pollutants, i.e . rhodamine B and solar hydrogen evolution. The results are in accordance with the prohibition of photogenerated electrons and holes recombination in these two samples under light illumination. The photocatalytic activity can be further boosted by introducing Pd nanoparticles onto the surfaces of TiO 2 /TiOF 2 through a simple deposition method without using any stabilizers, which is probably attributed to the enhanced visible-light absorption as well as the facilitated charge-carrier separation after the introduction of Pd nanoparticles. The synergistic effect between TiOF 2 and TiO 2 was discussed and was responsible for the enhancement of their activity in comparison with single counterpart.

CAS / MDL: 7647-10-1
研究领域: 材料科学 · 环境科学
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Materials Science & Engineering C-Materials for Biological Applications · 2019 · IF 4.959

Fabrication of hollow ZnO-Co3O4 nanocomposite derived from bimetallic-organic frameworks capped with Pd nanoparticles and MWCNTs for highly sensitive detection of tanshinol drug

Cong Zhang,Jujie Ren,Yifei Xing,Min Cui,Na Li,Peng Liu,Xiaofang Wen,Meng Li

In this work, PdNPs@ZnO-Co 3 O 4 was synthesized via the facile oxidation treatment of bimetallic ZnCo-zeolitic-imidazolate-framework (ZnCo-ZIF) followed by in situ chemical reduction of PdNPs on the surface of the nanocrystals. After combined with MWCNTs, the PdNPs@ZnO-Co 3 O 4 -MWCNTs nanocomposites were formed, which were then exploited as novel electrode materials to construct the non-enzyme electrochemical sensors for high-sensitivity detection of tanshinol. Due to the high catalytic activity of multi-metallic PdNPs@ZnO-Co 3 O 4 , and the excellent charge transfer property between imidazole groups of the ligands in MOFs and MWCNTs, the obtained sensor exhibited high sensitivity for tanshinol detection under optimum experimental conditions. The sensor shows two well linear relationship between the current and tanshinol concentration in the range of 0.002–0.69 mM (R 2  = 0.989) and 0.69–3.75 mM (R 2  = 0.994) with the corresponding sensitivity of 59.16 μA mM − 1 and 19.08 μA mM − 1 . And the limit of detection (LOD) was calculated to be 0.019 μM (S/N = 3). Furthermore, with the advantages of good repeatability, stability and selectivity, the fabricated sensor can be successfully applied to measurement of tanshinol in real medicinal liquids samples. Our results would accelerate the applications of MOFs in electrochemical field and provide insights into design of multifunctional non-enzyme sensing materials for various applications in biocatalysis, bioanalysis and drug testing.

研究领域: 材料科学 · 生物医学工程 · 分析化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Pd nanoparticles-DNA layered nanoreticulation biosensor based on target-catalytic hairpin assembly for ultrasensitive and selective biosensing of microRNA-21

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.

研究领域: 生物传感器技术 · 分子诊断学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2018 · IF 3.649

Enhanced performance of Pd nanoparticles on SBA-15 grafted with alkyltrialkoxysilane in 2-ethyl-anthraquinone hydrogenation

Qingqing Ma,Nan Wang,Guozhu Liu,Li Wang

Pd catalysts on mesoporous silica SBA-15 functionalized with alkyltriethoxysilane (alkyl = methyl, ethyl, propyl and isobutyl) were prepared. The effects of grafting sequence on the grafting amount were studied. The catalysts were characterized by XRD , FT-IR, elemental analysis , thermogravimetric analysis , nitrogen adsorption-desorption, TEM and XPS , and evaluated using catalytic hydrogenation of 2-ethyl-anthraquinone. The grafting amount increases with increasing the alkyl chain length of alkyltriethoxysilane. The highest grafting amount with the carbon content of 1.56% is obtained using an ante-grafting procedure where the grafting is performed prior to the removal of template, and this catalyst shows the highest activity and selectivity (98.3%). The accordant relationship between the activity of Pd/SBA-15 catalysts and their grafting amount indicates a positive effect of hydrophobicity of SBA-15 created by grafting on the catalytic hydrogenation of 2-ethyl-anthraquinone.

研究领域: 催化化学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Hydrogen generation over Ni@Pd NCs through an active H-exchange from formic acid-water system

Qu Tang,Xiaobo Zhou,JinXia Liu,Mingmin Wu,Haiwei Ji,Qi Wang,Guo Li,Hui Cong,Yuling Qin

The use of Formic acid as an alternative to fossil fuels is promising, both from economical and ecological standpoints, and has received great of attention owing to its inherently superiority in recent decades. Nevertheless, efficient and low-cost solid catalyst for formic acid dehydrogenation at room temperature still constitutes a biggish challenge. Moreover, comparing to increase the catalytic performance of catalysts, very little attention payed to the kinetic mechanism of dehydrogenation reaction because of the lack of effective characterization artifice. Here, the as-prepared Ni@Pd nanoparticles by a sequential reduction process can be useful catalyst for formic acid decomposition at room temperature without a promoter. Thanks to the effective catalyst and isotope distribution technique, preliminary mechanistic results firstly reveal that hydrogen is obtained via a H-atom recombination on isolated sites after the proton exchange randomly between activated H and solvent.

研究领域: 材料科学 · 催化化学 · 能源科学
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