Synthesis and characterization of n-alkylamine-stabilized palladium nanoparticles for electrochemical oxidation of methane

Zhongping Li; Jie Gao; Xiaoting Xing; Suozhu Wu; Shaomin Shuang; Chuan Dong; Man Chin Paau; Martin M F CHOI

doi:10.1021/jp907745v

Synthesis and characterization of n-alkylamine-stabilized palladium nanoparticles for electrochemical oxidation of methane

Zhongping Li, Jie Gao, Xiaoting Xing, Suozhu Wu, Shaomin Shuang^*, Chuan Dong, Man Chin Paau, Martin M F CHOI

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

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Abstract

Palladium nanoparticles (PdNPs) have been synthesized using n-alkylamines (C_n-NH₂) as stabilizing ligands. The NP size and distribution were controlled by varying the initial mole ratio of PdCl ₂/C_n-NH₂ and carbon chain lengths of C _n-NH₂ including hexylamine (C₆-NH₂), dodecylamine (C₁₂-NH₂), and octadecylamine (C ₁₈-NH₂). The average PdNP sizes were 20 ± 2.0, 6.0 ± 0.8, 5.6 ± 0.8, 6.5 ± 0.9, and 5.2 ± 0.8 nm prepared with 1:7 PdC_l2/C₆-NH₂, 1:7 PdC _l2/C₁₂-NH₂, 1:7 PdC_l2/C ₁₈-NH₂, 1:5 PdC_l2/C₁₈-NH ₂, and 1:9 PdC_l2/C₁₈-NH₂, respectively. The particle size decreased with the increase in the carbon chain length of C_n-NH₂. The as-synthesized n-alkylamine stabilized PdNPs (Cn-NH₂-PdNPs) were fully characterized by transmission electron microscopy, X-ray powder diffraction, Uv-visible absorption spectroscopy, infrared (IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), proton nuclear magnetic resonance (¹H NMR) spectroscopy, thermogravimetric analysis, graphite furnace atomic absorption spectrometry, and mass spectrometry. The interaction of C₁₈-NH ₂ with PdNPs was verified by IR, XPS, and ¹H NMR spectra, demonstrating that the amine functionalities were successfully linked to the Pd core surfaces. The PdNPs are soluble and stable in apolar solvents such as benzene, chloroform, n-hexane, and toluene. The electrochemical reactions between CH₄ and C_n-NH₂-PdNPs on Pd electrodes were studied by cyclic voltammetry and chronoamperometry. These PdNPs reacted readily and produced good response to CH₄ at ambient conditions. The sensitivity to CH₄ depends on the PdNPs prepared from various n-alkyl chain lengths of C_n-NH₂ and also the mole ratio of PdCl₂/Cn-NH₂. It was determined that PdNPs synthesized from 1:7 PdC_l2/C₁₈-NH₂ displayed the best electrocatalytic oxidization of CH₄. The C₁₈-NH ₂-PdNP (5.6 nm) modified Pd electrode could be used repeatedly and had a stable and reproducible response to CH₄.

Original language	English
Pages (from-to)	723-733
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	114
Issue number	2
DOIs	https://doi.org/10.1021/jp907745v
Publication status	Published - 21 Jan 2010

Scopus Subject Areas

Electronic, Optical and Magnetic Materials
Energy(all)
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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@article{9ab12d5f54fd46b5831aeae3662a73f8,

title = "Synthesis and characterization of n-alkylamine-stabilized palladium nanoparticles for electrochemical oxidation of methane",

abstract = "Palladium nanoparticles (PdNPs) have been synthesized using n-alkylamines (Cn-NH2) as stabilizing ligands. The NP size and distribution were controlled by varying the initial mole ratio of PdCl 2/Cn-NH2 and carbon chain lengths of C n-NH2 including hexylamine (C6-NH2), dodecylamine (C12-NH2), and octadecylamine (C 18-NH2). The average PdNP sizes were 20 ± 2.0, 6.0 ± 0.8, 5.6 ± 0.8, 6.5 ± 0.9, and 5.2 ± 0.8 nm prepared with 1:7 PdCl2/C6-NH2, 1:7 PdC l2/C12-NH2, 1:7 PdCl2/C 18-NH2, 1:5 PdCl2/C18-NH 2, and 1:9 PdCl2/C18-NH2, respectively. The particle size decreased with the increase in the carbon chain length of Cn-NH2. The as-synthesized n-alkylamine stabilized PdNPs (Cn-NH2-PdNPs) were fully characterized by transmission electron microscopy, X-ray powder diffraction, Uv-visible absorption spectroscopy, infrared (IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), proton nuclear magnetic resonance (1H NMR) spectroscopy, thermogravimetric analysis, graphite furnace atomic absorption spectrometry, and mass spectrometry. The interaction of C18-NH 2 with PdNPs was verified by IR, XPS, and 1H NMR spectra, demonstrating that the amine functionalities were successfully linked to the Pd core surfaces. The PdNPs are soluble and stable in apolar solvents such as benzene, chloroform, n-hexane, and toluene. The electrochemical reactions between CH4 and Cn-NH2-PdNPs on Pd electrodes were studied by cyclic voltammetry and chronoamperometry. These PdNPs reacted readily and produced good response to CH4 at ambient conditions. The sensitivity to CH4 depends on the PdNPs prepared from various n-alkyl chain lengths of Cn-NH2 and also the mole ratio of PdCl2/Cn-NH2. It was determined that PdNPs synthesized from 1:7 PdCl2/C18-NH2 displayed the best electrocatalytic oxidization of CH4. The C18-NH 2-PdNP (5.6 nm) modified Pd electrode could be used repeatedly and had a stable and reproducible response to CH4.",

author = "Zhongping Li and Jie Gao and Xiaoting Xing and Suozhu Wu and Shaomin Shuang and Chuan Dong and Paau, {Man Chin} and CHOI, {Martin M F}",

year = "2010",

month = jan,

day = "21",

doi = "10.1021/jp907745v",

language = "English",

volume = "114",

pages = "723--733",

journal = "Journal of Physical Chemistry C",

issn = "1932-7447",

publisher = "American Chemical Society",

number = "2",

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TY - JOUR

T1 - Synthesis and characterization of n-alkylamine-stabilized palladium nanoparticles for electrochemical oxidation of methane

AU - Li, Zhongping

AU - Gao, Jie

AU - Xing, Xiaoting

AU - Wu, Suozhu

AU - Shuang, Shaomin

AU - Dong, Chuan

AU - Paau, Man Chin

AU - CHOI, Martin M F

PY - 2010/1/21

Y1 - 2010/1/21

N2 - Palladium nanoparticles (PdNPs) have been synthesized using n-alkylamines (Cn-NH2) as stabilizing ligands. The NP size and distribution were controlled by varying the initial mole ratio of PdCl 2/Cn-NH2 and carbon chain lengths of C n-NH2 including hexylamine (C6-NH2), dodecylamine (C12-NH2), and octadecylamine (C 18-NH2). The average PdNP sizes were 20 ± 2.0, 6.0 ± 0.8, 5.6 ± 0.8, 6.5 ± 0.9, and 5.2 ± 0.8 nm prepared with 1:7 PdCl2/C6-NH2, 1:7 PdC l2/C12-NH2, 1:7 PdCl2/C 18-NH2, 1:5 PdCl2/C18-NH 2, and 1:9 PdCl2/C18-NH2, respectively. The particle size decreased with the increase in the carbon chain length of Cn-NH2. The as-synthesized n-alkylamine stabilized PdNPs (Cn-NH2-PdNPs) were fully characterized by transmission electron microscopy, X-ray powder diffraction, Uv-visible absorption spectroscopy, infrared (IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), proton nuclear magnetic resonance (1H NMR) spectroscopy, thermogravimetric analysis, graphite furnace atomic absorption spectrometry, and mass spectrometry. The interaction of C18-NH 2 with PdNPs was verified by IR, XPS, and 1H NMR spectra, demonstrating that the amine functionalities were successfully linked to the Pd core surfaces. The PdNPs are soluble and stable in apolar solvents such as benzene, chloroform, n-hexane, and toluene. The electrochemical reactions between CH4 and Cn-NH2-PdNPs on Pd electrodes were studied by cyclic voltammetry and chronoamperometry. These PdNPs reacted readily and produced good response to CH4 at ambient conditions. The sensitivity to CH4 depends on the PdNPs prepared from various n-alkyl chain lengths of Cn-NH2 and also the mole ratio of PdCl2/Cn-NH2. It was determined that PdNPs synthesized from 1:7 PdCl2/C18-NH2 displayed the best electrocatalytic oxidization of CH4. The C18-NH 2-PdNP (5.6 nm) modified Pd electrode could be used repeatedly and had a stable and reproducible response to CH4.

AB - Palladium nanoparticles (PdNPs) have been synthesized using n-alkylamines (Cn-NH2) as stabilizing ligands. The NP size and distribution were controlled by varying the initial mole ratio of PdCl 2/Cn-NH2 and carbon chain lengths of C n-NH2 including hexylamine (C6-NH2), dodecylamine (C12-NH2), and octadecylamine (C 18-NH2). The average PdNP sizes were 20 ± 2.0, 6.0 ± 0.8, 5.6 ± 0.8, 6.5 ± 0.9, and 5.2 ± 0.8 nm prepared with 1:7 PdCl2/C6-NH2, 1:7 PdC l2/C12-NH2, 1:7 PdCl2/C 18-NH2, 1:5 PdCl2/C18-NH 2, and 1:9 PdCl2/C18-NH2, respectively. The particle size decreased with the increase in the carbon chain length of Cn-NH2. The as-synthesized n-alkylamine stabilized PdNPs (Cn-NH2-PdNPs) were fully characterized by transmission electron microscopy, X-ray powder diffraction, Uv-visible absorption spectroscopy, infrared (IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), proton nuclear magnetic resonance (1H NMR) spectroscopy, thermogravimetric analysis, graphite furnace atomic absorption spectrometry, and mass spectrometry. The interaction of C18-NH 2 with PdNPs was verified by IR, XPS, and 1H NMR spectra, demonstrating that the amine functionalities were successfully linked to the Pd core surfaces. The PdNPs are soluble and stable in apolar solvents such as benzene, chloroform, n-hexane, and toluene. The electrochemical reactions between CH4 and Cn-NH2-PdNPs on Pd electrodes were studied by cyclic voltammetry and chronoamperometry. These PdNPs reacted readily and produced good response to CH4 at ambient conditions. The sensitivity to CH4 depends on the PdNPs prepared from various n-alkyl chain lengths of Cn-NH2 and also the mole ratio of PdCl2/Cn-NH2. It was determined that PdNPs synthesized from 1:7 PdCl2/C18-NH2 displayed the best electrocatalytic oxidization of CH4. The C18-NH 2-PdNP (5.6 nm) modified Pd electrode could be used repeatedly and had a stable and reproducible response to CH4.

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U2 - 10.1021/jp907745v

DO - 10.1021/jp907745v

M3 - Article

AN - SCOPUS:75249102292

SN - 1932-7447

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JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

IS - 2

ER -

Synthesis and characterization of n-alkylamine-stabilized palladium nanoparticles for electrochemical oxidation of methane

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