Polyaniline Electrodes Containing Tri-Atomic Au/Pd Clusters: Effect of Ordering

Jonke, Alex P.; Josowicz, Mira; Janata, Jiřı́

doi:10.1007/s10562-013-1116-1

Cited by 11 publications

(32 citation statements)

References 9 publications

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“…The double-junction reference electrode was Ag/AgCl in 1 M KCl//1 M KNO 3 . All potentials mentioned in this work are referred to this electrode (E = 0.235 V vs. SHE).…”

Section: Methodsmentioning

confidence: 99%

“…© The Author ( The preparation of composite materials that function as electrocatalysts is an active field of research. The in-situ incorporation of metal clusters on an atomic scale, such as Au n and Au n Pd m (1 ≤ n,m ≤ 8), in a polyaniline matrix has been developed [1][2][3][4][5] and their use for oxidation of alcohols in alkaline media has been demonstrated. [6][7][8] It has been shown that the number of atoms, and the order in which they are added, tracks their electrocatalytic activity in excellent agreement with calculated electron affinity.…”

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confidence: 99%

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Preparation of a Carbon-Platinum-Polyaniline Support for Atomic Metal Deposition

Gawron

Křížek

Kowalik

et al. 2015

J. Electrochem. Soc.

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A low-cost, thin, graphitized carbon electrode with electrodeposited platinum and polyaniline has been characterized for electrochemical oxidation of aliphatic alcohols in alkaline medium and for possible further incorporation of atomic metals and alloys. Our previously developed atomic metal polyaniline composites used solid platinum as the electrode material. The replacement of this solid platinum with a small amount of electrochemically annealed Pt on a carbon support was optimized for alcohol oxidation. An HPLC procedure for analysis of oxidation products of 1-propanol has also been utilized for the characterization of the composite electrode. © The Author ( The preparation of composite materials that function as electrocatalysts is an active field of research. The in-situ incorporation of metal clusters on an atomic scale, such as Au n and Au n Pd m (1 ≤ n,m ≤ 8), in a polyaniline matrix has been developed [1][2][3][4][5] and their use for oxidation of alcohols in alkaline media has been demonstrated. [6][7][8] It has been shown that the number of atoms, and the order in which they are added, tracks their electrocatalytic activity in excellent agreement with calculated electron affinity. 9,10 In order to generate maximum interaction between the active atomic metal centers embedded in polyaniline (PANI), the close coupling and synergistic effects of the composite components in the support cannot be overlooked. Carbon supported platinum is widely used as a composite electrode due to its known activity toward alcohols, 11 and composites of carbonplatinum-polyaniline have been studied in acidic media.12 Among all the different preparation procedures of Pt clusters -e.g. dispersement in paste and powders, 11 ion exchange, 13 impregnation, 13 colloidal precipitation, 13 vapor deposition, potential-step, 11,14 potential cycling, 13 and chronoamperometric 15 -the potentiostatic electrodeposition method 16,17 remains one of the best due to its high reproducibility and controllability. The forms of carbon that are ideal for potentiostatic deposition include glassy carbon, 18 nanotubes, 16 pyrolytic, 14,17 graphite cloth, fiber, and paper. 15 Platinum is known to have the highest activity for the oxygen reduction reaction (ORR) in alkaline media. 19Size and structural effects have remained the main issue for loading Pt nanoparticles into the different types of carbon support but an indirect influence of the support may also affect the rate of metal dispersion, the accessibility of active sites or even its own catalytic activity. One of the attractive features of composites prepared on atomic scale is dramatic reduction of the amount of precious metals in the composite electrode. In the case of atomic gold, such reduction is estimated to be on the order of 10,000. However, all of our previous preparations have been done on a solid Pt substrate coated with PANI matrix. Thus, the primary goal of this study has been replacement of expensive Pt with a less expensive electroactive material, e.g. carbon. However, a small amo...

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“…The double-junction reference electrode was Ag/AgCl in 1 M KCl//1 M KNO 3 . All potentials mentioned in this work are referred to this electrode (E = 0.235 V vs. SHE).…”

Section: Methodsmentioning

confidence: 99%

mentioning

confidence: 99%

Preparation of a Carbon-Platinum-Polyaniline Support for Atomic Metal Deposition

Gawron

Křížek

Kowalik

et al. 2015

J. Electrochem. Soc.

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“…Furthermore, it has been shown that electrodes modified with such PANI*(at.metal) materials have unique and highly selective electrocatalytic behavior. The reaction selected for this demonstration has been the oxidation of lower aliphatic alcohols in strongly alkaline media . Although convincing, such reaction is only an example of a much broader application of these novel materials.…”

Section: New Sensing Materialsmentioning

confidence: 99%

“…The most remarkable discovery has been the fact that the order in which heteroatoms are deposited in the atomic alloy structures plays a major role in the electrocatalytic efficiency of the material . This is illustrated in Fig.…”

Section: New Sensing Materialsmentioning

confidence: 99%

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Vision of new olfactory sensing array

Janata

Nakamoto

2016

IEEJ Transactions Elec Engng

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A newly synthesized material with highly controllable, but partial selectivity is proposed for the construction of catalytic sensors comprising an olfactory array. The transduction principle proposed for this array is that of a fuel-cell-type amperometric sensor. In the example discussed here, it is based on electrochemical oxidation of lower aliphatic alcohols in an alkaline medium. Since a cyclic voltammogram of each sensor in the olfactory array provides high-dimesional data, a pattern recognition technique including mutidimensional data generation, feature extraction, and classification is indispensable. The combination of the new sensor array with a sophisticated pattern recognition algorithm might lead to the next generation of olfactory sensing array.

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Quantized Electrodes: Atomic Palladium and Gold in Polyaniline

2021

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Electrochemically deposited Pd m Au n metal clusters on a polyaniline-coated Pt electrode have been shown to exhibit an "ordering effect", in which the catalytic activity for n-propanol oxidation depends sensitively on the precise order that the metal atoms are deposited. For example, tri-atomic Pd 2 Au clusters exhibit different catalytic activity for electrodeposition order PdÀ PdÀ Au compared to PdÀ AuÀ Pd on the polyaniline (PANI)/Pt matrix. In this work, we utilize density functional theory (DFT) to elucidate the structure and energetics of triatomic Pd m Au n clusters attached to a model PANI support. We provide a rationale for the experimentally observed "ordering effect" in terms of specific covalent interactions between the metal atoms and PANI framework that alter the net stability of the metal catalyst. We find that hydroxyl radical binding energies computed for the model catalytic systems provide a good descriptor for the experimentally measured catalytic activity for n-propanol oxidation. In addition, the good correlation between experiment/theory serves as additional confirmation of our proposed catalytic structures and rationale of the previously unexplained "ordering effect". Our study highlights the important role of the PANI support in determining the activity of uniquely-defined, atomic metal catalysts.

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Polyaniline Electrodes Containing Tri-Atomic Au/Pd Clusters: Effect of Ordering

Cited by 11 publications

References 9 publications

Preparation of a Carbon-Platinum-Polyaniline Support for Atomic Metal Deposition

Preparation of a Carbon-Platinum-Polyaniline Support for Atomic Metal Deposition

Vision of new olfactory sensing array

Quantized Electrodes: Atomic Palladium and Gold in Polyaniline

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