CRYSTENGCOMM
·
2021
·Vol. 23
·期 15
·2897-2904
·
IF 3.545
Beixi An,Yibing Luo,Jinglong Bai,Yanrong Wang,Xu Cheng,Jianpeng Li,Qiao Wang,Yifan Yang,Erqing Xie
In this study, we used a hydrothermal method to prepare WO3 nanospheres doped with a bimetal of Pd and Ni and used them in hydrogen sensing. The results show that the bimetal-doped WO3 nanospheres have a higher response, faster response/recovery time, and better selectivity than single metal-doped WO3. Moreover, they still have a high response to hydrogen at a low concentration. With 5 ppb of hydrogen, the sensor's response can reach 1.5, which is 1.5 times greater than that of pure WO3. Furthermore, the bimetal-doped WO3 has a shorter response time (14 s) and recovery time (8 s). This superior performance of the Pd/Ni-doped WO3 to hydrogen is most probably because of the strong adsorption of hydrogen, which results from the synergistic effect of two metals.
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CATALYSIS LETTERS
·
2021
·Vol. 151
·期 8
·2291-2301
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IF 3.186
Fan Xizheng,Yang Jingyi,Pang Qingqing,Liu Zhongyi,Zhang Panke,Yang Jing-He
Abstract Construction of heterogeneous Pd/SiO 2 catalyst via the pollution-free strategy marked strong electrostatic adsorption has been reported for the application to Suzuki–Miyaura cross-coupling reactions. The exposed negatively charged oxygen groups, which were converted from the hydroxyl groups on the surface of silica under the alkaline atmosphere, could effectively anchor palladium species to form ultrafine Pd nanoparticles (Pd NPs) with an average particle size of 1.3 nm and high dispersion (43%). Pd/SiO 2 catalyst was endowed with the excellent catalytic performance which was that the yield of the Suzuki–Miyaura reaction between bromobenzene and phenylboronic acid at 40 °C was > 99% for 30 min and the TOF was ~ 80,000 h −1 . The catalyst could be easily recovered and recycled by facile procedure without a significant decrease in catalytic activity, which was able to maintain the 90% yield after repeated for 8 times. In addition, a continuous flow reaction device was designed using the Pd/SiO 2 catalyst to effectively improve the production efficiency of biphenyl. Graphic Abstract Pd/SiO 2 catalyst constructed with the strategy of strong electrostatic adsorption (SEA) possesses uniformly dispersed and highly exposed Pd sites which can be easily transformed into electron-deficient Pd δ+ and strengthened stability for itself due to its strong interaction with the front surface of the carrier, and has been endowed the outstanding catalytic performance for Suzuki − Miyaura cross-coupling reaction.
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Molecular Catalysis
·
2021
·
IF 5.062
Yue Zhang,Zhiyong Pan,Nan Wang,Li Wang
Silica SBA-15 without removal of template P123 was calcined in an inert atmosphere and the carbon-modified SBA-15 thus obtained was used as the support of Pd catalyst for the hydrogenation of 2-ethylanthraquinone (EAQ). The effects of extraction times of P123 in SBA-15 with water prior to inert calcination and calcination temperature on the structure and catalytic performance of Pd catalyst were studied. The results of elemental analysis, X-ray diffraction, X-ray photoelectron spectroscopy, inductively coupled plasma, Fourier transform infrared spectroscopy, Raman spectra, water contact angle measurement, N 2 adsorption-desorption, transmission electron microscopy and energy dispersive X-ray mapping showed that carbon content of catalysts varied in the range of 3.4 % and 1.1 % with increasing extraction times from 0 to 6 due to the decrease in the residual amount of P123 in uncalcined SBA-15. With rising calcination temperature, the occurrence state of carbon in catalysts was converted from amorphism into graphite. The Pd catalyst supported on SBA-15 extracted for 3 times and calcined at 650 °C had 2.0 % carbon, and exhibited the highest activity (0.37 molH 2 ·gPd −1 ·min −1 ) and selectivity (98.9 %). This is due to the presence of appropriate amount of carbon, which provided a relatively high hydrophobicity without significantly reducing the specific surface area and pore size of SBA-15 support. The high hydrophobicity benefits the adsorption of EAQ from the working solution to the surface of catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Longjie Liu,Qianyu Xu,Gary Owens,Zuliang Chen
Antibiotics are an emerging class of persistent contaminants that are now of major environmental concern because they pose potential risks to both environmental and human health. Here reduced graphene oxide composited with bimetallic iron/palladium nanoparticles (rGO@ n Fe/Pd) was synthesized via a green tea extract and used to remove a common antibiotic, rifampicin from aqueous solution. The innate physical rifampicin removal efficiency of the composite (79.9 %) was increased to 85.7 % when combined with Fenton-oxidation. The mechanism and the main factors controlling Fenton-oxidation of rifampicin by rGO@ n Fe/Pd were investigated. Oxidation followed a pseudo-second-order degradation kinetic model with an activation energy of 47.3 kJ mol −1 . rGO@ n Fe/Pd were characterized by Brunauer-Emmett-Teller (BET), fourier transform infrared (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray energy spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), X-Ray powder diffraction (XRD), and zeta potential. Rifampicin degradation products observed by LC-UV, where subsequently confirmed to be mainly 5,6,9-trihydroxynaphtho [2,1-b] furan-1(2 H)-one, 5,6-dihydroxy-1-oxo-1,2-dihydronaphtho [2,1-b] furan-2-yl formate and ( S )-5,6,9-trihydroxy-2-(3-methoxypropoxy)-2-methylnaphtho [2,1-b] furan-1(2 H)-one by LC–MS. Finally, the practical effectiveness of the composite material for antibiotic removal was demonstrated by the treatment of representative wastewaters, where rifampicin removal efficiencies of 80.4, 77.9 and 70.2 % were observed for river, aquaculture wastewater and domestic wastewater, respectively.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Boxuan Yang,Zheng Zhang,Chen Tian,Wenjing Yuan,Zhongqiu Hua,Shurui Fan,Yi Wu,Xuemin Tian
Gas sensors based on Pd-loaded SnO 2 were prepared with printed zeolite films on the top of the sensor layer to enhance selective response to methane. As expected, Pd-loaded SnO 2 has a sensitive response to CH 4 and VOCs, such as ethanol and acetone vapors. Pt catalyst was dispersed onto the surface to promote the catalytic activity of zeolite. According to the catalytic characterizations, it was indicated that interfered gases, CO and ethanol were catalytically oxidized into CO 2 and water vapor. Whereas the catalytic combustion of methane is a negligible and sensitive response to the interested analyte was significantly promoted. Thus, the selective response to CH 4 was greatly improved even in a mixture of CO and VOCs. Based on the power-law response to oxygen, it was found that the resistive responses of all sensors were highly oxygen-dependent, suggesting that oxygen adsorbates on the surface were involved in the sensing process and no difference with zeolite coated sensors. Thus, it can be concluded that zeolite films printed onto the sensing layer surface serve as a catalytic filter and responsible for the enhanced sensitive and selective response of methane.
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JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 4
·1525-1535
·
IF 3.442
Zhang Jian,Jiang Yuting,Zhang Jiaxin,Zhang Lanhe,Wang Bing,Li Zheng,Liu Congze,Wang Haonan
2,4-Dichlorophenol (2,4-DCP) is a kind of toxic organic compound listed as a priority pollutant by the environmental protection agency, which will endanger the environment and human health. The accumulation of 2,4-DCP in the environment has become a serious problem today since 2,4-DCP is difficult to be degraded by traditional methods. In this study, a novel palladium/graphene oxide/indium tin oxide (Pd/GO/ITO) composite electrode was prepared by constant current electrodeposition method. And the surface morphology, crystal structure and surface element valence state of the electrode were observed and analyzed by SEM, XRD and XPS, respectively. Finally, by studying the influence of different conditions on the performance of the electrodes, the electrochemical degradation efficiency of the new electrodes on 2,4-DCP was investigated. It was found that the degradation of the Pd/GO/ITO electrodes on 2,4-DCP followed a quasi-first-order reaction under different conditions.
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Journal of the American Chemical Society
·
2019
·
IF 14.695
Yonggang Feng,Weiwei Xu,Bolong Huang,Qi Shao,Lai Xu,Shize Yang,Xiaoqing Huang
The pursuit of efficient hydrogenation nanocatalysts with a desirable selectivity toward intricate substrates is state-of-the-art research but remains a formidable challenge. Herein, we report a series of novel PdCdx nanocubes (NCs) for ultraselective hydrogenation reactions with flexible tuning features. Obtaining a desirable conversion level of the substrates (e.g., 4-nitrophenylacetylene (NPA), 4-nitrobenzaldehyde (NBAD), and 4-nitrostyrene (NS)) and competitive selectivity for all potential hydrogenation products have been achieved one by one under optimized hydrogenation conditions. The performance of these PdCdx NCs displays an evident dependence on both the composition and the use of Cd and a need for a distinct hydrogen source (H2 or HCOONH4). Additionally, for the selectivity of hydrogen to be suitably high, the morphology of the NCs has a very well-defined effect. Density functional theory calculations confirmed the variation of adsorption energy for the substrate and hydrogenation products by carefully controlled introduction of Cd, leading to a desirable level of selectivity for all potential hydrogenation products. The PdCdx NCs also exhibit excellent reusability with negligible activity/selectivity decay and structural/composition changes after consecutive reactions. The present study provides an advanced strategy for the rational design of superior hydrogenation nanocatalysts to achieve a practical application for desirable and selective hydrogenation reaction efficiency.
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Small Methods
·
2022
·Vol. 7
·期 1
·2201225
·
IF 15.367
Zemeng Dong,Qiyan Sun,Guang-Rui Xu,Zexing Wu,Yanyan Li,Jianping Lai,Guangjiu Li,Lei Wang
The electrocatalytic nitrogen reduction reaction (NRR) is emerging as a great promise for ambient and sustainable NH 3 production while it still suffers from the high adsorption energy of N 2 , the difficulty of *NN protonation, and inevitable hydrogen evolution, leading to a great challenge for efficient NRR. Herein, we synthesized a series of amorphous trimetal Pd-based (PdCoM (M = Cu, Ag, Fe, Mo)) nanosheets (NSs) with an ultrathin 2D structure, which shows high efficiency and robust electrocatalytic nitrogen fixation. Among them, amorphous PdCoCu NSs exhibit excellent NRR activity at low overpotentials with an NH 3 yield of 60.68 µg h −1 mg cat −1 and a corresponding Faraday efficiency of 42.93% at −0.05 V versus reversible hydrogen electrode as well as outstanding stability with only 5% decrease after a long test period of 40 h at room temperature. The superior NRR activity and robust stability should be attributed to the large specific surface area, abundant active sites as well as structural engineering and electronic effect that boosts up the Pd 4d band center, which further efficiently restrains the hydrogen evolution. This work offers an opportunity for more energy conversion devices through the novel strategy for designing active and stable catalysts.
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JOURNAL OF POWER SOURCES
·
2012
·
IF 4.951
Haiting Lu,Yang Fan,Ping Huang,Dongli Xu
SnO 2 nanospheres were employed as the support material for Pd catalyst. The as-prepared Pd/SnO 2 catalyst exhibited remarkably improved electrocatalytic activity and stability towards formic acid oxidation , in comparison with that of the Vulcan XC-72 carbon black and the commercial SnO 2 nanopowder supported Pd catalyst. The enhanced catalytic performance may arise from the unique structure and surface properties of the SnO 2 nanospheres, which process extraordinary promotional effect on Pd catalyst.
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CHEMOSPHERE
·
2015
·
IF 3.34
Ya-Li Chen,Lu Xiong,Xiang-Ning Song,Wei-Kang Wang,Yu-Xi Huang,Han-Qing Yu
Electrocatalytic hydrodehalogenation is a cost-effective approach to degrade halogenated organic pollutants in groundwater, and Pd-based catalysts have been found to be an efficient cathode material for this purpose. In this work, a novel Cu@Pd bimetallic catalyst loaded on Ti plate was prepared via combined electrodeposition and galvanic replacement for electrocatalytic hydrodehalogenation of atrazine, a typical halogenated pollutant. The obtained bimetallic catalyst with uniformly dispersed Pd nanoparticles possessed a large electrochemically active surface area of 572 cm 2 . The Cu@Pd/Ti cathode exhibited a higher electrocatalytic efficiency towards atrazine reduction than the individual Pd/Ti or Cu/Ti cathodes, and achieved up to 91.5% within 120 min under a current density of 1 mA cm −2 . Such an electrocatalytic reduction followed pseudo-first-order kinetics with a rate constant of 0.0214 min −1 . Atrazine was selectively transformed to dechlorinated atrazine, and its degradation pathway was identified. Current density was found to have a critical influence on the atrazine reduction due to the competitive hydrogen evolution reaction at a higher current density. The fabricated bimetallic catalyst also exhibited a good stability. This work provides an efficient and stable electrocatalyst for chlorinated contaminate removal and groundwater remediation.
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Interdisciplinary Materials
·
2024
·
IF 24.5
Mingwei Wang,Zhiyi Hu,Jieheng Lv,Zhiwen Yin,Zhewei Xu,Jingfeng Liu,Shihao Feng,Xiaoqian Wang,Jiazhen He,Sicheng Luo,Dafu Zhao,Hang Li,Xuemin Luo,Qi Liu,Damin Liu,Baolian Su,Dongyuan Zhao,Yong Liu
Compositions and morphologies of Pt-based electrocatalysts have great impact on the electrocatalytic activity and stability of oxygen reduction reaction (ORR). Herein, we report a novel design of one-dimensional (1D) Pt–Pd dendritic nanotubular heterostructures (DTHs) by controlling the degree of Pt 2+ -Pt reduction reaction and Pd-Pt galvanic replacement reaction with uniform Pd nanowires as sacrificial templates. The obtained Pt–Pd bimetallic DTHs catalyst exhibited uniform and dense Pt dendritic nanobranches on the surface of 1D hollow Pt–Pd alloy nanotubes, possessing superior catalytic activity for ORR compared to state-of-the-art commercial Pt/C catalysts. Typically, the Pt 4 Pd DTHs catalyst showed efficient mass activity (MA, 1.05 A mg Pt −1 ) and specific activity (SA, 1.25 mA cm Pt −2 ) at 0.9 V (vs. RHE), and the catalyst exhibited high stability with 90.4% MA retention after 20 000 potential cycles. The Pt–Pd bimetallic DTHs configuration combines the advantages of 1D hollow nanostructures and dense Pt dendritic nanobranches, which results in rich electrochemical active surface sites, fast charge transport, and multiple dendritic anchoring points contact on carbon support, thus boosting its catalytic activity and stability towards electrocatalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2016
·
IF 3.014
Xiaomeng Li,Ming Wen,Dandan Wu,Qingsheng Wu,Jiaqi Li
For the exploration of catalysts with excellent performance in alkaline fuel cells, high-performance two-dimensional (2D) Pd-on-NiCu nanosheets were synthesized through the kinetics controlling synthesis of NiCu nanosheets followed by Pd nanoparticles (NPs) embedding treatment at room temperature. In which case, well-dispersed Pd NPs with the average diameter of ∼4 nm are embedded on NiCu nanosheets (BET surface area of 180.7 m 2 g −1 ). Pd-on-NiCu nanosheets exert remarkable high performance in electrocatalytic activity, methanol-tolerance and stability, the electrocatalytic mass activity of Pd-on-NiCu nanosheets is 1827 mAmg −1 , which is over 6-fold higher than that of commercial Pd/C (289 mAmg −1 ), and the current density of the electrocatalyst decreases after 300 cycles of only 6%. Therefore, Pd-on-NiCu nanosheets can be considered as one of the most promising candidates for fuel cells applications.
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