APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Mengran Lou,Ruiying Wang,Lili Yang,Dianzeng Jia,Zhipeng Sun,Luxiang Wang,Yong Guo,Xingchao Wang,Jie Zhang,Hongli Shi
Direct formic acid fuel cells have great application potential in the energy field, but their commercialization is hindered by the CO poisoning and low performance of Pd-based anode catalysts. In this study, novel composite catalysts composed of Pd, organic-inorganic hybrid imidazole ionic liquid polyoxometalates, and N,P-codoped coal-based carbon fibers with good dispersion and smaller Pd nanoparticles were synthesized successfully. Physical and electrochemical characterizations revealed that the as-prepared Pd-based composite catalysts have excellent CO poisoning resistance and enhanced electrocatalytic activity in formic acid electrooxidation. Notably, the CO oxidation onset potential of a catalyst modified by imidazole ionic liquid polyoxometalate with long alkyl chain was 0.1 V lower than that of the unmodified catalyst. The mass activity of the as-prepared Pd catalyst in formic acid oxidation was 754.1 mA mg −1 Pd . It is expected that organic-inorganic hybrid polyoxometalates can be further applied to fuel cell catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Fukun Bi,Xiaodong Zhang,Shang Xiang,Yunyun Wang
The effect of Pd loading (0.25, 0.5 and 1.0 wt%) and ZrO 2 support calcined at diverse temperatures (600, 700 and 800 °C) by pyrolysis of UiO-66 was investigated for CO oxidation in this work, respectively. The physicochemical properties of the samples were characterized by various characterization methods. The XRD results exhibited that all ZrO 2 support possessed mixed crystalline phase, the monoclinic ZrO 2 and tetragonal ZrO 2 . And the calcination temperature had a big impact on the composition of ZrO 2 supports. Pyrolysis of UiO-66 at high temperature was favorable for the formation of monoclinic ZrO 2 . Additionally, the introduction of Pd was induced the phase conversion from tetragonal to monoclinic of ZrO 2 . The order of catalytic efficiency was as follows: 0.5Pd/Zr-700 > 0.5Pd/Zr-600 > 0.5Pd/Zr-800. Moreover, 0.5Pd/Zr-700 presented high stability and great reusability. The good catalytic performance of 0.5Pd/Zr-700 was ascribed to the better reduction ability at low temperature and high O ads /O lat and Pd 0 /Pd 2+ on the surface. Importantly, the reaction pathway of CO oxidation over the 0.5Pd/Zr-700 was exposed.
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Electrocatalysis
·
2020
·Vol. 11
·期 5
·522-535
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IF 2.587
Shen Yanmei,Lu Shixiang,Xu Wenguo,Lv Anqi,Wang Ziwen,Wang Hongtao,Liu Guoxiao,Zhang Yan
Incorporation of precious metallic nanoparticles onto a carbon support material is used to obtain an electrocatalyst for ethanol oxidation. A composite material of spherical palladium nanoparticles (Pd NPs), reduced graphene oxide (rGO), and polydopamine (PDA) on three-dimensional nickel foam (NF) substrate (Pd/rGO/PDA@NF) has been synthesized for ethanol electrocatalysis. The Pd nanoparticles were obtained via reduction of precursor K 2 PdCl 4 using ascorbic acid at 60 °C for 80 min. The rGO with large specific surface area was used in catalysts to provide large amounts of active sites for Pd NPs. Meanwhile, Pd NPs as an effective ingredient in catalyst exhibited excellent electrochemical activity of ethanol oxidation. Local surface plasmon resonance was carried out to determine the optimal concentration of precursor K 2 PdCl 4 aqueous solution, and the absorbance peak of Pd NPs was found at about 340–370 nm by UV-visible spectroscopy. An enhanced property of the composite material Pd/rGO/PDA@NF was demonstrated to catalyze the ethanol oxidation reaction in alkaline electrolyte solution. A higher ratio of forward scan peak current intensity ( I f ) to reverse scan peak current intensity ( I b ) was 1.59, which demonstrated the significant anti-poison effect to carbonaceous intermediates of the Pd/rGO/PDA@NF. The value of I f can maintain 90.6% after 400 cycles, indicating the higher cycling stability and better electrocatalytic performance toward ethanol oxidation.
Pd/rGO/PDA@NF was synthesized by a simple method with great elecrocatalytic performance and tolerance against carbonaceous intermediate species toward ethanol oxidation.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 34
·17657-17669
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IF 11.301
Xiaoli Li,Ting Wang,Xueqin Tao,Ganhua Qiu,Can Li,Benxia Li
Metal-modified semiconductors are being deemed as one of the most promising photocatalysts for various applications. Although great efforts have been devoted to developing a variety of metal-modified semiconductor photocatalysts, the exact functions of their interfaces in governing photocatalytic processes still remain elusive. Herein, the interfacial synergy of metal sites and defective semiconductor with oxygen vacancies (VOs) was investigated toward the photocatalytic selective oxidation of toluene, by taking the Pd/BiOBr photocatalyst as an example. The presence of Pd induces the generation of more VOs on the BiOBr surface due to the electronic interaction at the Pd–BiOBr interface. The coexistence of the Pd and VO sites on BiOBr enables the favorable adsorption of O2 and toluene molecules. The Pd–BiOBr interface governs the charge separation and prompts the activation of O2 and toluene, leading to 1.5 times the activity of BiOBr–VO for the photocatalytic selective oxidation of toluene to benzaldehyde with a high selectivity (>99%). Moreover, the typical influencing factors, such as the illumination intensity and toluene concentration, were optimized to improve the photocatalytic efficiency. The active species and intermediates in the photocatalytic reaction were identified by a series of controlled experiments, as well as in situ ESR measurements. Therefore, both experimental and theoretical results provide the direct evidence to understand the key roles of the interfacial Pd and VO sites in enhancing photocatalysis toward the selective oxidation of toluene.
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Nanomaterials
·
2019
·Vol. 10
·期 1
·6
·
IF 4.034
Fangke Zhan,Juanjuan Yin,Jingxin Zhou,Tifeng Jiao,Lexin Zhang,Meirong Xia,Zhenhua Bai,Qiuming Peng
With the rapid development of industry, the problem of environmental pollution has become increasingly prominent. Exploring and preparing green, efficient, and low cost catalysts has become the key challenge for scientists. However, some conventional preparation methods are limited by conditions, such as cumbersome operation, high energy consumption, and high pollution. Here, a simple and efficient seed-mediated method was designed and proposed to synthesize a highly efficient bimetallic catalyst for catalyzing nitro compounds. A Pd-Cu bimetallic composite (BCM) can be prepared by synthesizing the original seed crystal of precious metal palladium, then growing the mature nanocrystalline palladium and supporting the transition metal copper. Importantly, after eight consecutive catalytic cycles, the conversion of the catalyzed 2-NA was 84%, while the conversion of the catalyzed 4-NP was still 72%. And the catalytic first order rates of 2-NA and 4-NP constants were 0.015 s−1, and 0.069 s−1, respectively. Therefore, current research of nanocomposites catalyst showed great significance for serious environmental pollution problems and the protection of living environment, providing a new idea for the preparation of new bimetallic catalytic materials.Keywords:seed-mediated;bimetallic catalyst;nanocomposites;catalyst
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NEW JOURNAL OF CHEMISTRY
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2019
·Vol. 43
·期 46
·17954-17962
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IF 3.069
Chang Liu,Xin Ran,Qing Qu,Tiantian Zhang,Guanben Du,Long Yang
Herein, we report a surfactant-controlled strategy for synthesizing Pd–Pt bimetallic nanocrystals (NCs) with different morphologies via a high-yield and one-pot synthesis method in an aqueous solution for catalyzing the ethanol oxidation reaction. Polyallylamine hydrochloride (PAH) was utilized to modulate the reduction kinetics to obtain diverse morphologies. By simply changing the concentration of surface controller PAH in the original growth solution, three different shapes of Pd–Pt NCs (nanospheroids, nanoflowers, and nanoworms) could be prepared by using H2PtCl6 and PdCl2 as metal precursors and CTAB as a stabilizer. Compared with nanoworms and nanospheroids, the as-prepared nanoflowers exhibited the highest electrocatalytic activity and possessed Pd–Pt core–shell nanostructures. The important role of PAH was confirmed to tune the reduction kinetics, resulting in the distinct morphologies of Pd–Pt NCs. To the best of our knowledge, this is the first report in which Pd–Pt NCs with PAH-controlled structures are prepared in a one-pot aqueous phase by adjusting the sequential reduction kinetics. Furthermore, these Pd–Pt NCs exhibited superior catalytic activity for the ethanol electrooxidation in comparison with that of the commercial Pd/C catalyst.
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Analytical Methods
·
2019
·Vol. 11
·期 47
·6053-6061
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IF 2.378
Man Du,Yue Zhang,Yifeng Yu,Hua Zhao,Yue Guo,Yunxu Yang
A novel “off–on” fluorescent probe ACBT, using a readily available dye 2-(2′-aminophenyl) benzothiazole as the fluorophore, for the determination of Pd2+ was designed and synthesized in this work. Based on a palladium triggered cleavage reaction, the probe ACBT exhibited rapid response time (<2 min), and high selectivity and sensitivity towards Pd2+ in aqueous solution under mild conditions. The detection limit of probe ACBT towards Pd2+ was estimated to be as low as 2.6 nM. Furthermore, fabrication of probe ACBT test strips was achieved for a convenient visual detection of palladium. In addition, it also has been successfully applied to detect Pd2+ in environmental water samples with satisfactory results, indicating that the use of probe ACBT could be a potential and feasible method to detect Pd2+ in environmental systems.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2011
·Vol. 19
·期 4
·1305-1314
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IF 2.87
Zhong Li-feng,Yan Wen,Li Jie,Tu Xiang-lin,Liu Bao-ming,Xia Zhen
Purpose This study assessed the concentrations of platinum (Pt) and palladium (Pd) in surface sediments and sedimentary cores collected from the Pearl River Estuary with a view of evaluating the distribution, background levels, possible sources, and contamination level of anthropogenic Pt and Pd. Materials and methods Thirty-six samples of surface sediments and 12 samples from sedimentary cores were collected. Al 2 O 3 was analyzed on fused glass disks by X-ray fluorescence spectrometer. Heavy metal elements were measured by inductively coupled plasma–mass spectrometry. Pt and Pd were separated from the sample matrix by anion exchange chromatography and subsequent solvent extraction after samples had been digested in Carius tubes using aqua regia. The analysis of Pt and Pd was performed by isotopic dilution-inductively coupled plasma-mass spectrometry. Results and discussion Pt and Pd concentrations in surface sediments were 0.28–2.11 and 0.39–38.30 ng/g, respectively, and Pt and Pd concentrations in sedimentary cores were 0.19–1.18 and 0.15–1.76 ng/g, respectively. Background values of Pt and Pd were 0.20–1.17 and 0.10–1.34 ng/g, respectively. The spatial distribution of the enrichment factor differed between Pt and Pd in surface sediments. Down-core variations in Pt, Pd, and other heavy metal elements were similar in all cases and were related to sediment type. Conclusions Some of the Pt and Pt in surface samples were derived from anthropogenic emissions. Pt and Pd were delivered to the sediment by fluvial input. In addition to vehicle exhaust catalysts, Pt and Pd were derived from other sources (e.g., industrial process). An important post-burial remobilization process of Pt and Pd is likely to be particle mixing by billows caused by typhoon.
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Foods
·
2023
·Vol. 12
·期 23
·4260
·
IF 5.2
Yuan Fang,Shusen Ding,Weiran Li,Jingjing Zhang,Hui Sun,Xiaodong Lin
Silver ions (Ag+) exist widely in various areas of human life, and the food contamination caused by them poses a serious threat to human health. Among the numerous methods used for the detection of Ag+, fluorescence and colorimetric analysis have attracted much attention due to their inherent advantages, such as high sensitivity, simple operation, short time, low cost and visualized detection. In this work, Pd/Pt nanoflowers (NFs) specifically responsive to Ag+were synthesized in a simple way to oxidize o-phenylenediamine (OPD) into 2,3-diaminophenazine (DAP). The interaction of Ag+with the surface of Pd/Pt NFs inhibits the catalytic activity of Pd/Pt NFs towards the substrate OPD. A novel dual-channel nanosensor was constructed for the detection of Ag+, using the fluorescence intensity and UV-vis absorption intensity of DAP as output signals. This dual-mode analysis combines their respective advantages to significantly improve the sensitivity and accuracy of Ag+detection. The results showed that the limit of detection was 5.8 nM for the fluorescence channel and 46.9 nM for the colorimetric channel, respectively. Moreover, the developed platform has been successfully used for the detection of Ag+in real samples with satisfactory recoveries, which is promising for the application in the point-of-care testing of Ag+in the field of food safety.Keywords:silver ions;Pd/Pt nanoflowers;fluorescent sensor;colorimetric sensor
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APPLIED CATALYSIS A-GENERAL
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2023
·
IF 5.5
Shuang Wang,Cheng Li,Rujie Shang,Huihui Zhang,Kehui Qi,Yao Yao,Chunyan Yu,Qing Liu,Guorui Li,Shitao Yu,Lu Li
Producing vanillin from lignin model compounds in an elegant and efficient manner is a focus of chemical utilization in lignocellulosic biomass. The facile synthesis of a cobalt-palladium bimetallic alloy anchored on activated carbon (Co-Pd/C), which excels in the selective oxidation of the lignin model compound 4-methylguaiacol to vanillin, is reported here. The characterization results of Co-Pd/C indicate that the catalysts enhance the catalytic efficiency by forming a cobalt-palladium alloy to modulate the number of d-band cavities and influence the O 2 adsorption. Meanwhile, the synergistic effect between the alloys causes the Co-Pd/C catalyst exhibits good activity and stability in cycling experiments. A series of controlled experiments offer insight into the mechanism of catalytic generation of vanillin from 4-methylguaiacol. This work opens a new opportunity for achieving the valuable aromatic products from lignin.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
·Vol. 415
·期 29
·7103-7115
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IF 4.3
Li Guiyin,Li Xinhao,Xu Wenfeng,Li Shennan,Tan Xiaohong,Liang Jintao,Zhou Zhide
1,5-anhydroglucitol (1,5-AG) is of considerable clinical relevance as a biochemical marker of glucose metabolism in the assessment and monitoring of diabetes. Herein, a simple colorimetric biosensor was constructed for the identification and detection of 1,5-AG by using pyranose oxidase (PROD) enzyme cascaded with reduced graphene oxide/persimmon tannin/Pt@Pd (RGO-PT/Pt@Pd NPs) nanozyme. The as-prepared RGO-PT/Pt@Pd NPs had excellent peroxidase-like activity and can be applied as a nanozyme. First, PROD enzyme reacts with the target 1,5-AG, decomposing 1,5-AG into 1,5-anhydrofuctose (1,5-AF) and H 2 O 2 . At this point, the highly catalytic RGO-PT/Pt@Pd NPs nanozyme produces a cascade with PROD enzyme which catalyzes the decomposition of H 2 O 2 to produce O 2 . This in turn oxidizes the substrate 3,3′,5,5′-tetramethylbenzidine (TMB) and produces a color change in the solution. Finally, the detection of 1,5-AG was achieved by measuring the absorption peak at 652 nm with an ultraviolet visible (UV-vis) spectrophotometer. Under optimal conditions, the linear operating range of the 1,5-AG enzyme cascade colorimetric sensor was 1.0–100.0 μg/mL, and the limit of detection (LOD) was 0.81 μg/mL. The proposed colorimetric biosensor was successfully applied to detect 1,5-AG in spiked human serum samples with the recoveries of 97.2–103.9% and RSDs of 1.94–4.48%. It provides a promising developmental assay for clinical detection of 1,5-AG.
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Thermal Science and Engineering Progress
·
2023
·
IF 4.8
Jing Yi,Pan Wang,Feixiang Li,Qi Chen,Lili Lei
Catalytic combustion of C 2 H 6 at equivalence ratios of 1.0 and 1.4 over non-thermal plasma (NTP) modified Pd/Al 2 O 3 was studied experimentally to examine the effect of O 2 and N 2 plasma on the catalyst activity and physico-chemical property. C 2 H 6 conversion, chemical product distribution and selectivity were taken into account to evaluate the performance of modified catalysts in C 2 H 6 oxidation at 200–500 ℃. The results showed that the plasma modification had suppressive effects on the activity of Pd/Al 2 O 3 . When compared to Pd/Al 2 O 3 , T 30 for the modified Pd/Al 2 O 3 were shifted to higher temperatures by approximately 30–50 ℃. For catalysts modified by plasma, significantly more CO was formed in the C 2 H 6 combustion at high temperature region. Moreover, the structure, morphology and chemical states of Pd/Al 2 O 3 after modification were thoroughly analyzed with the means of N 2 adsorption–desorption, XRD, XPS and SEM. The surface area of modified catalysts decreased, resulting in the activity degradation. The leaching of Pd species and transform of γ-Al 2 O 3 to θ-Al 2 O 3 were observed after the NTP treatment with highly energetic electrons. It should to be highlighted that the reduction of Pd 2+ to Pd 0 by NTP modification on the catalyst surface from XPS analysis. The NTP had the potential to reduce catalysts while employing oxidizing or inert gases.
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