Low-Pressure Plasma Synthesis of Ni/C Nanocatalysts from Solid Precursors

Influence of the Plasma Chemistry on the Morphology and Chemical State

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

Nanocatalyst materials based on metal nanoparticles (NPs) deposited on mesoporous carbon substrates are widely used in catalysis and energy storage; however, conventional wet-chemical deposition methods based on the reduction of metal salts are not always the best choice when looking for a process ensuring easy scalability and low environmental impact. Moreover, additional surface functionalization steps, such as the addition of nitrogen- or oxygen-containing groups, are more and more explored to increase the activity or the chemical stability of catalysts. In this work, we investigate a new methodology for the fabrication of nickel/carbon nanocatalysts relying on a low-pressure radio frequency plasma treatment of solid (powder) precursors. A mesoporous carbon xerogel is used as support for nickel NPs synthesized through the decomposition of an organometallic nickel precursor in a plasma discharge. Different plasma treatment conditions and chemical environments are applied by varying the plasma power and the gas mixture injected into the plasma chamber (Ar, N2, NH3, and O2). The nucleation kinetics of nickel NPs, their morphology evolution, and chemical state were fully characterized by combining analytical techniques such as in situ optical emission spectroscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Results indicate that the plasma chemistry and conditions strongly influence the organometallic compound decomposition as well as the size and the oxidation state of the homogeneously dispersed nickel NPs. We compare the organometallic precursor degradation efficiency for each plasma by defining a rational “activation power” associated with each plasma chemistry. Moreover, simultaneous carbon substrate functionalization is obtained through plasma treatment, which demonstrates the high versatility of the plasma fabrication for developing green and efficient catalysts and energy materials.
langue originaleAnglais
Pages (de - à)265-273
Nombre de pages9
journalACS Applied Nano Materials
Volume1
Numéro de publication1
Les DOIs
étatPublié - janv. 2018

Empreinte digitale

Plasmas
Nickel
Carbon
Organometallics
Nanoparticles
Organometallic Compounds
Plasma Gases
Decomposition
Fabrication
Optical emission spectroscopy
Xerogels
Catalysts
Metal nanoparticles
Chemical stability
Substrates
Gas mixtures
Powders
Energy storage
Catalysis
Environmental impact

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title = "Low-Pressure Plasma Synthesis of Ni/C Nanocatalysts from Solid Precursors: Influence of the Plasma Chemistry on the Morphology and Chemical State",
abstract = "Nanocatalyst materials based on metal nanoparticles (NPs) deposited on mesoporous carbon substrates are widely used in catalysis and energy storage; however, conventional wet-chemical deposition methods based on the reduction of metal salts are not always the best choice when looking for a process ensuring easy scalability and low environmental impact. Moreover, additional surface functionalization steps, such as the addition of nitrogen- or oxygen-containing groups, are more and more explored to increase the activity or the chemical stability of catalysts. In this work, we investigate a new methodology for the fabrication of nickel/carbon nanocatalysts relying on a low-pressure radio frequency plasma treatment of solid (powder) precursors. A mesoporous carbon xerogel is used as support for nickel NPs synthesized through the decomposition of an organometallic nickel precursor in a plasma discharge. Different plasma treatment conditions and chemical environments are applied by varying the plasma power and the gas mixture injected into the plasma chamber (Ar, N2, NH3, and O2). The nucleation kinetics of nickel NPs, their morphology evolution, and chemical state were fully characterized by combining analytical techniques such as in situ optical emission spectroscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Results indicate that the plasma chemistry and conditions strongly influence the organometallic compound decomposition as well as the size and the oxidation state of the homogeneously dispersed nickel NPs. We compare the organometallic precursor degradation efficiency for each plasma by defining a rational “activation power” associated with each plasma chemistry. Moreover, simultaneous carbon substrate functionalization is obtained through plasma treatment, which demonstrates the high versatility of the plasma fabrication for developing green and efficient catalysts and energy materials.",
keywords = "low-pressure plasma, nanocatalysts, nickel nanoparticles, optical emission spectroscopy, organometal, photoelectron spectroscopy, surface functionalization",
author = "Emile Haye and Yan Busby and {Da Silva Pires}, Mathieu and Florian Bocchese and Nathalie Job and Laurent Houssiau and Jean-Jacques Pireaux",
year = "2018",
month = "1",
doi = "10.1021/acsanm.7b00125",
language = "English",
volume = "1",
pages = "265--273",
journal = "ACS Applied Nano Materials",
publisher = "American Chemical Society",
number = "1",

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T1 - Low-Pressure Plasma Synthesis of Ni/C Nanocatalysts from Solid Precursors

T2 - Influence of the Plasma Chemistry on the Morphology and Chemical State

AU - Haye, Emile

AU - Busby, Yan

AU - Da Silva Pires, Mathieu

AU - Bocchese, Florian

AU - Job, Nathalie

AU - Houssiau, Laurent

AU - Pireaux, Jean-Jacques

PY - 2018/1

Y1 - 2018/1

N2 - Nanocatalyst materials based on metal nanoparticles (NPs) deposited on mesoporous carbon substrates are widely used in catalysis and energy storage; however, conventional wet-chemical deposition methods based on the reduction of metal salts are not always the best choice when looking for a process ensuring easy scalability and low environmental impact. Moreover, additional surface functionalization steps, such as the addition of nitrogen- or oxygen-containing groups, are more and more explored to increase the activity or the chemical stability of catalysts. In this work, we investigate a new methodology for the fabrication of nickel/carbon nanocatalysts relying on a low-pressure radio frequency plasma treatment of solid (powder) precursors. A mesoporous carbon xerogel is used as support for nickel NPs synthesized through the decomposition of an organometallic nickel precursor in a plasma discharge. Different plasma treatment conditions and chemical environments are applied by varying the plasma power and the gas mixture injected into the plasma chamber (Ar, N2, NH3, and O2). The nucleation kinetics of nickel NPs, their morphology evolution, and chemical state were fully characterized by combining analytical techniques such as in situ optical emission spectroscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Results indicate that the plasma chemistry and conditions strongly influence the organometallic compound decomposition as well as the size and the oxidation state of the homogeneously dispersed nickel NPs. We compare the organometallic precursor degradation efficiency for each plasma by defining a rational “activation power” associated with each plasma chemistry. Moreover, simultaneous carbon substrate functionalization is obtained through plasma treatment, which demonstrates the high versatility of the plasma fabrication for developing green and efficient catalysts and energy materials.

AB - Nanocatalyst materials based on metal nanoparticles (NPs) deposited on mesoporous carbon substrates are widely used in catalysis and energy storage; however, conventional wet-chemical deposition methods based on the reduction of metal salts are not always the best choice when looking for a process ensuring easy scalability and low environmental impact. Moreover, additional surface functionalization steps, such as the addition of nitrogen- or oxygen-containing groups, are more and more explored to increase the activity or the chemical stability of catalysts. In this work, we investigate a new methodology for the fabrication of nickel/carbon nanocatalysts relying on a low-pressure radio frequency plasma treatment of solid (powder) precursors. A mesoporous carbon xerogel is used as support for nickel NPs synthesized through the decomposition of an organometallic nickel precursor in a plasma discharge. Different plasma treatment conditions and chemical environments are applied by varying the plasma power and the gas mixture injected into the plasma chamber (Ar, N2, NH3, and O2). The nucleation kinetics of nickel NPs, their morphology evolution, and chemical state were fully characterized by combining analytical techniques such as in situ optical emission spectroscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Results indicate that the plasma chemistry and conditions strongly influence the organometallic compound decomposition as well as the size and the oxidation state of the homogeneously dispersed nickel NPs. We compare the organometallic precursor degradation efficiency for each plasma by defining a rational “activation power” associated with each plasma chemistry. Moreover, simultaneous carbon substrate functionalization is obtained through plasma treatment, which demonstrates the high versatility of the plasma fabrication for developing green and efficient catalysts and energy materials.

KW - low-pressure plasma

KW - nanocatalysts

KW - nickel nanoparticles

KW - optical emission spectroscopy

KW - organometal

KW - photoelectron spectroscopy

KW - surface functionalization

UR - http://pubs.acs.org/doi/10.1021/acsanm.7b00125

UR - http://www.mendeley.com/research/lowpressure-plasma-synthesis-nic-nanocatalysts-solid-precursors-influence-plasma-chemistry-morpholog

U2 - 10.1021/acsanm.7b00125

DO - 10.1021/acsanm.7b00125

M3 - Article

VL - 1

SP - 265

EP - 273

JO - ACS Applied Nano Materials

JF - ACS Applied Nano Materials

IS - 1

ER -