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Dyes wastewater treatment by reduction-oxidation process in an electrochemical reactor packed with natural manganese mineral

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Journal of Environmental Sciences 2006年第1期18卷 17-22页

作者： WANG Ai-min QU Jiu-hui LIU Hui-juan LEI Peng-ju State Key Laboratory of Environmental Aquatic Chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Beijing 100085 China

A novel technology which combined electrochemical process catalyzed by manganese mineral with electro-assisted coagulation process was proposed in this study. The mineralization of organic pollutant from simulated dye wastewater containing an azo dye Acid Red B（ARB） was experimentally investigated using this method. It was found that the manganese mineral could catalyze the electrochemical process dramatically. The TOC removal percentage of electrochemical treatment catalyzed by manganese mineral was 43.6% while the TOC removal percentage of the process using the manganese mineral alone and using the electrolysis alone were 9.3% and 20.8%, respectively. Moreover, it was found that combined electroxidation with electro-assisted coagulation process could more effectively eliminate ARB. After a period of 180 min electrooxidation and 300 min electroreduction, almost 66.9% of TOC was removed, and the dissolved Mn^2＋. could be effectivly removed. The effects of the order of oxidation and reduction, the proper ratio electrooxidation/reduction time, and current density on the removal efficiency were investigated in detail. In addition, a proposed mechanism of manganese-mineral-catalyzed electrooxidation-reduction process was discussed in this paper.

关键词： manganese mineral electroreduction electrooxidation catalyze Acid Red B

Synergistic effect between few layer graphene and carbon nanotube supports for palladium catalyzing electrochemical oxidation of alcohols

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Journal of Energy Chemistry 2013年第2期22卷 296-304页

作者： Bruno F. Machado Andrea Marchionni Revathi R. Bacsa Marco Bellini Julien Beausoleil Werner Oberhauser Francesco Vizza Philippe Serp Laboratoire de Chimie de Coordination UPR CNRS 8241 Composante ENSIACET Universit de Toulouse UPS-INP-LCC 4 alle Emile Monso BP 44362 31432 Toulouse Cedex 4 France Istituto di Chimica dei Composti Organometallici (ICCOM-CNR) Via Madonna del Piano 10 50019 Sesto Fiorentino Italy Arkema Groupement de Recherches de Lacq BP 34 RD 817 64170 Lacq France

Few layer graphene （FLG）, multi-walled carbon nanotubes （CNTs） and a nanotube-graphene composite （CNT-FLG） were used as supports for palladium nanoparticles. The catalysts, which were characterized by transmission electron microscopy, Raman spectroscopy and X-ray diffraction, were used as anodes in the electrooxidation of ethanol, ethylene glycol and glycerol in half cells and in passive direct ethanol fuel cells. Upon Pd deposition, a stronger interaction was found to occur between the metal and the nanotube-graphene composite and the particle size was significantly smaller in this material （6.3 nm）, comparing with nanotubes and graphene alone （8 and 8.4 nm, respectively）. Cyclic voltammetry experiments conducted with Pd/CNT, Pd/FLG and Pd/CNT-FLG in 10 wt% ethanol and 2 M KOH solution, showed high specific currents of 1.48, 2.29 and 2.51 mA-/zgp-d, respectively. Moreover, the results obtained for ethylene glycol and glycerol oxidation highlighted the excellent electrocatalytic activity of Pd/CNT-FLG in terms of peak current density （up to 3.70 mAgd for ethylene glycol and 1.84 mAfor glycerol, respectively）. Accordingly, Pd/CNT-FLG can be considered as the best performing one among the electrocatalysts ever reported for ethylene glycol oxidation, especially considering the low metal loading used in this work. Direct ethanol fuel cells at room temperature were studied by obtaining power density curves and undertaking galvanostatic experiments. The power density outputs using Pd/CNT, Pd/FLG and Pd/CNT-FLG were 12.1, 16.3 and 18.4 mW.cm-2, respectively. A remarkable activity for ethanol electrooxidation was shown by Pd/CNT-FLG anode catalyst. In a constant current experiment, the direct ethanol fuel cell containing Pd/CNT-FLG could continuously deliver 20 mA.cm-2 for 9.5 h during the conversion of ethanol into acetate of 30%, and the energy released from the cell was about 574 J.

关键词： electrooxidation alcohols fuel cells palladium graphene nanotube-graphene composites

Synthesis of Pt and Pt-Fe nanoparticles supported on MWCNTs used as electrocatalysts in the methanol oxidation reaction

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Journal of Energy Chemistry 2014年第4期23卷 483-490页

作者： J.R.Rodriguez R.M.Félix E.A.Reynoso Y.Gochi-Ponce Y.Verde Gómez S.Fuentes Moyado G.Alonso-Núez Universidad Nacional Autónoma de Mxico Centro de Nanociencias y Nanotecnología Ensenada B.C. C.P.22860 Mexico Instituto Tecnológico de Tijuana Centro de Graduados e Investigación Tijuana B.C. C.P.22000 Mexico Instituto Tecnológico de Oaxaca Departamento de Ingeniería Química y Bioquímica Oaxaca Oax. C.P.68030 Mexico Instituto Tecnológico de Cancún Av.Kabah Km.3 Cancún Q.R. C.P.77500 Mexico

This work reports a feasible synthesis of highly-dispersed Pt and Pt-Fe nanoparticles supported on multiwall carbon nanotubes （MWCNTs） without Fe and multiwall carbon nanotubes with iron （MWCNTs-Fe） which applied as electrocatalysts for methanol electrooxidation. A Pt coordination complex salt was synthesized in an aqueous solution and it was used as precursor to prepare Pt/MWCNTs, Pt/MWCNTs-Fe, and Pt-Fe/MWCNTs using FeC12.4H20 as iron source which were named S 1, S2 and S3, respectively. The coordination complex of platinum （TOA）2PtC16 was obtained by the chemical reaction between （NH4）2PtC16 with tetraoctylammonium bromide （TOAB） and it was characterized by FT-IR and TGA. The materials were characterized by Raman spectroscopy, SEM, EDS, XRD, TEM and TGA. The electrocatalytic activity of Pt-based supported on MWCNTs in the methanol oxidation was investigated by cyclic voltammetry （CV） and chronoamperometry （CA）. Pt-Fe/MWCNTs electrocatalysts showed the highest electrocatalytic activity and stability among the tested electrocatalysts due to that the addition of ＂Fe＂ promotes the OH species adsorption on the electrocatalyst surface at low potentials, thus, enhancing the activity toward the methanol oxidation reaction （MOR）.

关键词： coordination complex salt MWCNTs nanoparticles catalysts electrooxidation

Ternary Pd-Ni-P nanoparticle-based nonenzymatic glucose sensor with greatly enhanced sensitivity achieved through active-site engineering

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Nano Research 2017年第8期10卷 2712-2720页

作者： Jingwen Ma Yueguang Chen Lin Chen Leyu Wang State Key Laboratory of Chemical Resource Engineering School of Science Beijing University of Chemical Technology Beijing 100029 China

We develop a unique ternary Pd-Ni-P nanocatalyst for the sensitive enzyme- free electrooxidation detection of glucose under alkaline conditions. By reducing the distance between the Pd and Ni active sites in the Pd-Ni-P nanoparticles （NPs） via atom engineering, the catalyst structure is transformed from Pd@Ni-P dumbbells into spherical NPs, greatly enhancing the catalyst sensitivity. The glassy carbon electrode modified with Pd-Ni-P ternary NPs, which behaves as an efficient nonenzymatic glucose sensor, offers excellent electrocatalytic performance with a high sensitivity of 1,136 μA·mM^-1·cm^-2, a short response time of 2 s, a wide linear range of 0.5 μM to 10.24 mM, a low limit of detection of 0.15 μM （signal-to-noise ratio = 3）, and good selectivity and reproducibility. Moreover, owing to its superior catalytic performance, the Pd-Ni-P modified electrode has excellent reliability for glucose detection in real samples of human serum. Our study provides a promising alternative strategy for designing and constructing high-performance multicomponent nanocatalyst-based sensors.

关键词： Pd-Ni-P ternary nanocatalysts electrooxidation glucose sensing

Active sites contribution from nanostructured interface of palladium and cerium oxide with enhanced catalytic performance for alcohols oxidation in alkaline solution

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Journal of Energy Chemistry 2018年第2期27卷 395-403页

作者： Fulong Wang Huaguang Yu Zhiqun Tian Huaiguo Xue Ligang Feng School of Chemistry and Chemical Engineering Yangzhou University Collaborative Innovation Center of Renewable Energy Materials Guangxi University

Nanostructured interface is significant for the electrocatalysis process. Here we comparatively studied the electrooxidation of alcohols catalyzed by nanostructured palladium or palladium-cerium oxide. Two kinds of active sites were observed in palladium-cerium oxide system, attributing to the co-action of Pd-cerium oxide interface and Pd sites alone, by CO stripping technique, a structure-sensitive process generally employed to probe the active sites. Active sites resulting from the nanostructured interfacial contact of Pd and cerium oxide were confirmed by high resolution transmission electron microscopy and electrochemical CO stripping approaches. Electrochemical measurements of cyclic voltammetry and chronometry results demonstrated that Pd-cerium oxide catalysts exhibited much higher catalytic performances for alcohols oxidation than Pd alone in terms of activity, stability and anti-poisoning ability.The improved performance was probably attributed to the nanostructured active interface in which the catalytic ability from each component can be maximized through the synergistic action of bi-functional mechanism and electronic effect. The calculated catalytic efficiency of such active sites was many times higher than that of the Pd active sites alone. The present work showed the significance of valid nanostructured interface design and fabrication in the advanced catalysis system.

关键词： Alcohols oxidation Fuel cells Pd catalysts electrooxidation CO stripping

Erratum to:Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation

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Nano Research 2019年第8期12卷 1973-1973页

作者： Yanchao Xu Xiaoqiang Cui Shuting Wei Qinghua Zhang Lin Gu Fanqi Meng Jinchang Fan Weitao Zheng State Key Laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials oj MOE and Jilin UniversityChangchun 130012China Laboratory of Advanced Materials and Electron Microscopy Beijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China

The article Highly active zigzag-like Pt-Zn alloy nanowires with high-index facets for alcohol electrooxidation, written by Xiaoqiang Cui and Weitao Zheng, was erroneously originally published electronically on the publisher’s internet portal (currently SpringerLink) on 6 April 2019 with incomplete Electronic Supplementary Material (ESM), which should contain 16 figures and 3 tables. You will find the complete supplementary material file online linked to this publisher’s erratum.

关键词： Erratum electrooxidation nanowires

Composition optimized trimetallic PtNiRu dendritic nanostructures as I versatile and active electrocatalysts for alcohol oxidation

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Nano Research 2019年第3期12卷 651-657页

作者： Yan Lu Wei Wang Xiaowei Chen Yuhui Zhang Yanchen Han Yong Cheng Xue-Jiao Chen Kai Liu Yuanyuan Wang Qiaobao Zhang Shuifen Xie College of Materials Science and Engineering Huaqiao University Xiamen 361021 China Department of Physics Xiamen University Xiamen 361005 China Shenzhen Research Institute of Xiamen University Shenzhen 518000 China Department of Materials Science and Engineering Xiamen University Xiamen 361005 China

Platinum-based nano crystals are the most effective electrocatalysts for accelerati ng the chemical tran sformatio ns on the anode in direct alcohol fuel cells. To facilitate practical applications and overcome the drawbacks of diverse alcohols, it is significant to develop electrocatalysts with high activities and a wide fuel flexibility. Here, we demonstrate a practicable solution method for fabricating composition tun able trimetallic PtNiRu den dritic nano structures (DNSs) which can serve as versatile and active catalysts for electrooxidatio n of a variety of liquid alcohols. A series of trimetallic DNSs with tun able Pt/Ni/Ru atomic ratios were successfully syn thesized by simply adjusti ng the feeding of precursors. Detailed electrochemical test indicates that, among other compositions, the Pt66Ni27Ru7 DNSs present much superior electroactivity in catalyzing electrooxidation of liquid alcohols in acidic mediums. Specifically, the mass activity and specific activity on the Pt66Ni27Ru7 DNSs, for electrooxidation of methanol, ethanol, and ethylene glycol, are 4.57 and 4.34 times, 3.55 and 3.42 times, and 2.37 and 2.28 times that of the commercial Pt black, respectively. X-ray photoelectron spectroscopy and CO stripping studies reveal the adsorption of CO on these PtNiRu DNSs is much weaker than on pure Pt. Meanwhile, the surface Ru sites can provide neighbouring -OH groups to facilitate the oxidati on and removal of the adsorbed in termediates (-CO) on the surface Pt sites, effectively improvi ng the CO tolera nee of the catalysts. The PtNiRu DNSs also show effectively boosted capacity for breaking the C-C bond in C2-alcohols, showing great potential for fuel-flexible fuel cell applications.

关键词： platinum-based nanocrystals dendritic nanostructures fuel flexibility electrooxidation of alcohols CO toleranee

Electrochemical Behavior of Methanol Influenced by Polyaniline Incorporated with Ferrocenesulfonic-carboxylic Acid

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Chemical Research in Chinese Universities 2005年第4期21卷 431-435页

作者： NDAMANISHA Jean Chrysostome Faculty of Chemistry Northeast Normal University Changchun 130024 P. R. China

After the synthesis of polyaniline in the presence of ferrocenesulfoniccarboxylic acid, its influence on the electrochemical reaction of methanol was studied. The result indicates that the ferrocenyl in ferrocenesulfoniccarboxylic acid plays an important role in the electrocatalytic oxidation of methanol. CH_ 3OH is adsorbed on PANI-Fc before its electrocatalytic oxidation. When the concentration of methanol is 2 mol/L, it begins to be oxidized. The effect of scan rate on the electrochemical reaction of methanol was also studied and 5 mV/s was favourable. It is another method to insert a metal catalyst in polyaniline without its electrodeposition.

关键词： Polyaniline Ferrocenesulfonic-carboxylic acid Methanol electrooxidation Catalyst

Chemical oscillation in electrochemical oxidation of methanol on Pt surface

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Science China Chemistry 2008年第4期51卷 322-332页

作者： LI LanLan WEI ZiDong QI XueQiang SUN CaiXin YIN GuangZhi State Key Laboratory of Safety and New Technology for Electric Transmission&Distribution Chongqing UniversityChongqing 400044China School of Chemical Engineering Chongqing UniversityChongqing 400044China School of Material Science and Engineering Chongqing UniversityChongqing 400044China Key Laboratory of Exploitation of Southwestern Resources&the Environmental Disaster Control Engineering Chongqing Univer-sityChongqing 400044China

Based on dual path reaction mechanism, a nonlinear dynamics model reflecting the potential oscilla- tion in electrooxidation of methanol on Pt surface was established. The model involves three variables, the electrode potential (e), the surface coverage of carbon monoxide (x), and adsorbed water (y). The chemical reactions and electrode potential were coupled together through the rate constant ki = exp(ai(e ? ei)). The analysis to the established model discloses the following: there are different kinetics be- haviors in different ranges of current densities. The chemical oscillation in methanol electrooxidation is assigned to two aspects, one from poison mediate CO of methanol electrooxidation, which is the in- duced factor of the chemical oscillation, and the other from the oxygen-containing species, such as H2Oa. The formation and disappearance of H2Oa deeply depend on the electrode potential, and directly cause the chemical oscillation. The established model makes clear that the potential oscillation in methanol electrooxidation is the result of the feedback of electrode potential e on the reactions in- volving poison mediates CO and oxygen-containing species H2Oa. The numerical analysis of the estab- lished model successfully explains why the potential oscillation in methanol galvanostatic oxidation on a Pt electrode only happens in a certain range of current densities but not at any current density.

关键词： methanol electrooxidation electrochemical kinetics dual path reaction mechanism electrochemical oscillation bifurcation