One-step growth of 3-5 nm diameter palladium electrocatalyst in a carbon nanoparticle-chitosan host and characterization for formic acid oxidation

被引：35

作者：

Cheng, Niancai ^{[2
]}

Webster, Richard A. ^{[1
,3
]}

Pan, Mu ^{[2
]}

Mu, Shichun ^{[2
]}

Rassaei, Liza ^{[1
]}

Tsang, Shik Chi ^{[4
]}

Marken, Frank ^{[1
]}

机构：

[1] Univ Bath, Dept Chem, Bath BA2 7AY, Avon, England

[2] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China

[3] Univ Bath, Doctoral Training Ctr Sustainable Chem Technol, Bath BA2 7AY, Avon, England

[4] Univ Oxford, Inorgan Chem Lab, Oxford OX1 3QR, England

来源：

ELECTROCHIMICA ACTA | 2010年 / 55卷 / 22期

基金：

英国工程与自然科学研究理事会;

关键词：

Palladium nanoparticles; Chitosan; Carbon nanoparticles; Carbon dioxide; Nanocomposite; Formic acid; Fuel cell; Screen-printed electrode; Flow cell; Voltammetry; Buffer; Sensor; FUEL-CELL; PD NANOPARTICLES; PARTICLE-SIZE; CATALYSTS; ELECTROOXIDATION; NANOSTRUCTURES; METHANOL; HYDROGENATION; FORMALDEHYDE; NANOTUBES;

D O I：

10.1016/j.electacta.2010.06.014

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

The electrochemical formation of a palladium nanoparticle catalyst composite material has been investigated. A carbon nanoparticle-chitosan host film deposited onto a carbon substrate electrode has been employed to immobilize PdCl2 as catalyst precursor. A one-step electrochemical reduction process gave Pd nanoparticles within the chitosan matrix with different levels of loading, on different carbon substrates, and with a reproducible catalyst particle diameter of ca. 3-5 nm. High activity for formic acid oxidation has been observed in aqueous phosphate buffer medium. The oxidation of formic acid has been investigated as a function of pH and maximum catalyst activity was observed at pH 6. When varying the formic acid concentration, limiting behaviour consistent with a "resistance effect" has been observed. A flow cell system based on a screen-printed carbon electrode has been employed to establish the effect of hydrodynamic conditions on the formic acid oxidation. Both increasing the convective-diffusion mass transport rate and increasing the concentration of formic acid caused the oxidation peak current to converge towards the same "resistance limit". A mechanistic model to explain the resistance effect based on CO2 flux and localized CO2 gas bubble formation at the Pd nanoparticle modified carbon nanoparticle-chitosan host film has been proposed. (C) 2010 Elsevier Ltd. All rights reserved.

引用

页码：6601 / 6610

页数：10

共 46 条

[1] Facile Synthesis of Pd-Cd Nanostructures with High Capacity for Hydrogen Storage [J].

Adams, Brian D. ;

Wu, Guosheng ;

Nigrio, Samantha ;

Chen, Aicheng .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (20) :6930-+

[2]

Adams R. N., 1969, ELECTROCHEMISTRY SOL, P219

[3]

[Anonymous], 1997, CRC HDB CHEM PHYS

[4] Palladium in fuel cell catalysis [J].

Antolini, Ermete .

ENERGY & ENVIRONMENTAL SCIENCE, 2009, 2 (09) :915-931

[5] Nanoparticles as recyclable catalysts: The frontier between homogeneous and heterogeneous catalysis [J].

Astruc, D ;

Lu, F ;

Aranzaes, JR .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (48) :7852-7872

[6] A Facile Preparation of Hollow Palladium Nanosphere Catalysts for Direct Formic Acid Fuel Cell [J].

Bai, Zhengyu ;

Yang, Lin ;

Li, Lei ;

Lv, Jing ;

Wang, Kui ;

Zhang, Jie .

JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (24) :10568-10573

[7]

Bard A.J., 2001, ELECTROCHEMICAL METH, V2nd, P341

[8] Kinetics and mechanism of the electrooxidation of formic acid - Spectroelectrochemical studies in a flow cell [J].

Chen, YX ;

Heinen, M ;

Jusys, Z ;

Behm, RJ .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (06) :981-985

[9]

COMPTON RG, 2007, UNDERSTANDING VOLTAM, P308

[10] Oxidation of glycerol using gold-palladium alloy-supported nanocrystals [J].

Dimitratos, Nikolaos ;

Lopez-Sanchez, Jose Antonio ;

Anthonykutty, Jinto Manjaly ;

Brett, Gemma ;

Carley, Albert F. ;

Tiruvalam, Ram Chandra ;

Herzing, Andrew A. ;

Kiely, Christopher J. ;

Knight, David W. ;

Hutchings, Graham J. .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2009, 11 (25) :4952-4961

← 1 2 3 4 5 →