Polyoxometalate-mediated electron transfer-oxygen transfer oxidation of cellulose and hemicellulose to synthesis gas

Bidyut Bikash Sarma, Ronny Neumann

Research output: Contribution to journalArticle

40 Citations (Scopus)

Abstract

Terrestrial plants contain ∼70% hemicellulose and cellulose that are a significant renewable bioresource with potential as an alternative to petroleum feedstock for carbon-based fuels. The efficient and selective deconstruction of carbohydrates to their basic components, carbon monoxide and hydrogen, so called synthesis gas, is an important key step towards the realization of this potential, because the formation of liquid hydrocarbon fuels from synthesis gas are known technologies. Here we show that by using a polyoxometalate as an electron transfer-oxygen transfer catalyst, carbon monoxide is formed by cleavage of all the carbon-carbon bonds through dehydration of initially formed formic acid. In this oxidation-reduction reaction, the hydrogen atoms are stored on the polyoxometalate as protons and electrons, and can be electrochemically released from the polyoxometalate as hydrogen. Together, synthesis gas is formed. In a hydrogen economy scenario, this method can also be used to convert carbon monoxide to hydrogen.

Original languageEnglish
Article number4621
JournalNature Communications
Volume5
DOIs
Publication statusPublished - Aug 1 2014

Fingerprint

synthesis gas
Synthesis gas
cellulose
Cellulose
Hydrogen
electron transfer
Gases
Electrons
carbon monoxide
Oxygen
Carbon Monoxide
Oxidation
oxidation
oxygen
hydrogen
formic acid
Carbon
carbon
oxidation-reduction reactions
hydrocarbon fuels

ASJC Scopus subject areas

  • Biochemistry, Genetics and Molecular Biology(all)
  • Chemistry(all)
  • Physics and Astronomy(all)
  • Medicine(all)

Cite this

Polyoxometalate-mediated electron transfer-oxygen transfer oxidation of cellulose and hemicellulose to synthesis gas. / Sarma, Bidyut Bikash; Neumann, Ronny.

In: Nature Communications, Vol. 5, 4621, 01.08.2014.

Research output: Contribution to journalArticle

@article{e4008b8039764faa87c47bb897368ee6,
title = "Polyoxometalate-mediated electron transfer-oxygen transfer oxidation of cellulose and hemicellulose to synthesis gas",
abstract = "Terrestrial plants contain ∼70{\%} hemicellulose and cellulose that are a significant renewable bioresource with potential as an alternative to petroleum feedstock for carbon-based fuels. The efficient and selective deconstruction of carbohydrates to their basic components, carbon monoxide and hydrogen, so called synthesis gas, is an important key step towards the realization of this potential, because the formation of liquid hydrocarbon fuels from synthesis gas are known technologies. Here we show that by using a polyoxometalate as an electron transfer-oxygen transfer catalyst, carbon monoxide is formed by cleavage of all the carbon-carbon bonds through dehydration of initially formed formic acid. In this oxidation-reduction reaction, the hydrogen atoms are stored on the polyoxometalate as protons and electrons, and can be electrochemically released from the polyoxometalate as hydrogen. Together, synthesis gas is formed. In a hydrogen economy scenario, this method can also be used to convert carbon monoxide to hydrogen.",
author = "Sarma, {Bidyut Bikash} and Ronny Neumann",
year = "2014",
month = "8",
day = "1",
doi = "10.1038/ncomms5621",
language = "English",
volume = "5",
journal = "Nature Communications",
issn = "2041-1723",
publisher = "Nature Publishing Group",

}

TY - JOUR

T1 - Polyoxometalate-mediated electron transfer-oxygen transfer oxidation of cellulose and hemicellulose to synthesis gas

AU - Sarma, Bidyut Bikash

AU - Neumann, Ronny

PY - 2014/8/1

Y1 - 2014/8/1

N2 - Terrestrial plants contain ∼70% hemicellulose and cellulose that are a significant renewable bioresource with potential as an alternative to petroleum feedstock for carbon-based fuels. The efficient and selective deconstruction of carbohydrates to their basic components, carbon monoxide and hydrogen, so called synthesis gas, is an important key step towards the realization of this potential, because the formation of liquid hydrocarbon fuels from synthesis gas are known technologies. Here we show that by using a polyoxometalate as an electron transfer-oxygen transfer catalyst, carbon monoxide is formed by cleavage of all the carbon-carbon bonds through dehydration of initially formed formic acid. In this oxidation-reduction reaction, the hydrogen atoms are stored on the polyoxometalate as protons and electrons, and can be electrochemically released from the polyoxometalate as hydrogen. Together, synthesis gas is formed. In a hydrogen economy scenario, this method can also be used to convert carbon monoxide to hydrogen.

AB - Terrestrial plants contain ∼70% hemicellulose and cellulose that are a significant renewable bioresource with potential as an alternative to petroleum feedstock for carbon-based fuels. The efficient and selective deconstruction of carbohydrates to their basic components, carbon monoxide and hydrogen, so called synthesis gas, is an important key step towards the realization of this potential, because the formation of liquid hydrocarbon fuels from synthesis gas are known technologies. Here we show that by using a polyoxometalate as an electron transfer-oxygen transfer catalyst, carbon monoxide is formed by cleavage of all the carbon-carbon bonds through dehydration of initially formed formic acid. In this oxidation-reduction reaction, the hydrogen atoms are stored on the polyoxometalate as protons and electrons, and can be electrochemically released from the polyoxometalate as hydrogen. Together, synthesis gas is formed. In a hydrogen economy scenario, this method can also be used to convert carbon monoxide to hydrogen.

UR - http://www.scopus.com/inward/record.url?scp=84905492799&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84905492799&partnerID=8YFLogxK

U2 - 10.1038/ncomms5621

DO - 10.1038/ncomms5621

M3 - Article

C2 - 25082188

AN - SCOPUS:84905492799

VL - 5

JO - Nature Communications

JF - Nature Communications

SN - 2041-1723

M1 - 4621

ER -