Activation of Novel Copper-Carbon Catalysts Using Temperature-Programmed Mass Spectometry

Elizabeth Dawson, Gary Midgley, Philip A. Barnes

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

An entirely new method of preparing metal-carbon catalysts is reported in which the metal is present as small crystallites distributed in a three-dimensional array throughout the bulk of the carbon matrix. The metal particles are linked by a network of pores which exposes virtually all of the metal surface to the gas phase. By virtue of their structure, these new materials exhibit a remarkable resistance to sintering, even near the melting point of the metal. While many catalytically important metals can be incorporated into our materials, this paper concentrates on the structure of one of the copper-carbon systems. These are made by the reduction of a copper(II) cellulose precursor to produce a copper(0) cellulose material, followed by thermal degradation of the cellulose and activation of the resulting carbon to produce the pore network. New techniques, using a temperature-programmed gas-flow micro-reactor linked to an on-line mass spectrometer, are used to investigate the nature of the critical activation process. The resulting pore structure is studied and a mechanism is proposed to explain the catalytic effect of the copper particles on the formation of the pore network. Poisoning experiments demonstrate that access to the active sites is determined by the pore size, thus giving a measure of size selectivity. Using temperature- programmed oxidation with on-line MS it was demonstrated that the pores can be widened in a controlled manner, so reducing any diffusion-induced limitation on reaction rates. This offers the possibility of designing a catalyst with a specified balance between the conflicting requirements for size selectivity and high reaction rates.

LanguageEnglish
Pages349-353
Number of pages5
JournalJournal of the Chemical Society, Faraday Transactions
Volume88
Issue number3
DOIs
Publication statusPublished - 1992
Externally publishedYes

Fingerprint

Copper
Carbon
Metals
Chemical activation
activation
porosity
catalysts
copper
Catalysts
carbon
cellulose
Cellulose
metals
Temperature
Reaction rates
temperature
reaction kinetics
selectivity
Catalyst selectivity
poisoning

Cite this

@article{7efe98cf2f4141fa8f23f3d06e057279,
title = "Activation of Novel Copper-Carbon Catalysts Using Temperature-Programmed Mass Spectometry",
abstract = "An entirely new method of preparing metal-carbon catalysts is reported in which the metal is present as small crystallites distributed in a three-dimensional array throughout the bulk of the carbon matrix. The metal particles are linked by a network of pores which exposes virtually all of the metal surface to the gas phase. By virtue of their structure, these new materials exhibit a remarkable resistance to sintering, even near the melting point of the metal. While many catalytically important metals can be incorporated into our materials, this paper concentrates on the structure of one of the copper-carbon systems. These are made by the reduction of a copper(II) cellulose precursor to produce a copper(0) cellulose material, followed by thermal degradation of the cellulose and activation of the resulting carbon to produce the pore network. New techniques, using a temperature-programmed gas-flow micro-reactor linked to an on-line mass spectrometer, are used to investigate the nature of the critical activation process. The resulting pore structure is studied and a mechanism is proposed to explain the catalytic effect of the copper particles on the formation of the pore network. Poisoning experiments demonstrate that access to the active sites is determined by the pore size, thus giving a measure of size selectivity. Using temperature- programmed oxidation with on-line MS it was demonstrated that the pores can be widened in a controlled manner, so reducing any diffusion-induced limitation on reaction rates. This offers the possibility of designing a catalyst with a specified balance between the conflicting requirements for size selectivity and high reaction rates.",
author = "Elizabeth Dawson and Gary Midgley and Barnes, {Philip A.}",
year = "1992",
doi = "10.1039/FT9928800349",
language = "English",
volume = "88",
pages = "349--353",
journal = "Physical Chemistry Chemical Physics",
issn = "1463-9076",
publisher = "Royal Society of Chemistry",
number = "3",

}

Activation of Novel Copper-Carbon Catalysts Using Temperature-Programmed Mass Spectometry. / Dawson, Elizabeth; Midgley, Gary; Barnes, Philip A.

In: Journal of the Chemical Society, Faraday Transactions, Vol. 88, No. 3, 1992, p. 349-353.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Activation of Novel Copper-Carbon Catalysts Using Temperature-Programmed Mass Spectometry

AU - Dawson, Elizabeth

AU - Midgley, Gary

AU - Barnes, Philip A.

PY - 1992

Y1 - 1992

N2 - An entirely new method of preparing metal-carbon catalysts is reported in which the metal is present as small crystallites distributed in a three-dimensional array throughout the bulk of the carbon matrix. The metal particles are linked by a network of pores which exposes virtually all of the metal surface to the gas phase. By virtue of their structure, these new materials exhibit a remarkable resistance to sintering, even near the melting point of the metal. While many catalytically important metals can be incorporated into our materials, this paper concentrates on the structure of one of the copper-carbon systems. These are made by the reduction of a copper(II) cellulose precursor to produce a copper(0) cellulose material, followed by thermal degradation of the cellulose and activation of the resulting carbon to produce the pore network. New techniques, using a temperature-programmed gas-flow micro-reactor linked to an on-line mass spectrometer, are used to investigate the nature of the critical activation process. The resulting pore structure is studied and a mechanism is proposed to explain the catalytic effect of the copper particles on the formation of the pore network. Poisoning experiments demonstrate that access to the active sites is determined by the pore size, thus giving a measure of size selectivity. Using temperature- programmed oxidation with on-line MS it was demonstrated that the pores can be widened in a controlled manner, so reducing any diffusion-induced limitation on reaction rates. This offers the possibility of designing a catalyst with a specified balance between the conflicting requirements for size selectivity and high reaction rates.

AB - An entirely new method of preparing metal-carbon catalysts is reported in which the metal is present as small crystallites distributed in a three-dimensional array throughout the bulk of the carbon matrix. The metal particles are linked by a network of pores which exposes virtually all of the metal surface to the gas phase. By virtue of their structure, these new materials exhibit a remarkable resistance to sintering, even near the melting point of the metal. While many catalytically important metals can be incorporated into our materials, this paper concentrates on the structure of one of the copper-carbon systems. These are made by the reduction of a copper(II) cellulose precursor to produce a copper(0) cellulose material, followed by thermal degradation of the cellulose and activation of the resulting carbon to produce the pore network. New techniques, using a temperature-programmed gas-flow micro-reactor linked to an on-line mass spectrometer, are used to investigate the nature of the critical activation process. The resulting pore structure is studied and a mechanism is proposed to explain the catalytic effect of the copper particles on the formation of the pore network. Poisoning experiments demonstrate that access to the active sites is determined by the pore size, thus giving a measure of size selectivity. Using temperature- programmed oxidation with on-line MS it was demonstrated that the pores can be widened in a controlled manner, so reducing any diffusion-induced limitation on reaction rates. This offers the possibility of designing a catalyst with a specified balance between the conflicting requirements for size selectivity and high reaction rates.

UR - http://www.scopus.com/inward/record.url?scp=0013148025&partnerID=8YFLogxK

U2 - 10.1039/FT9928800349

DO - 10.1039/FT9928800349

M3 - Article

VL - 88

SP - 349

EP - 353

JO - Physical Chemistry Chemical Physics

T2 - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

SN - 1463-9076

IS - 3

ER -