Continuous time-resolved X-ray diffraction of the biocatalyzed reduction of Mn oxide

Timothy B. Fischer, Peter J. Heaney, Je Hun Jang, Daniel E. Ross, Susan Louise Brantley, Jeffrey E. Post, Ming Tien

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

Here we report the first continuous time-resolved X-ray diffraction analysis of a biologically mediated mineral reaction. We incubated total membrane (TM) fractions of the facultative anaerobe Shewanella oneidensis in an anoxic environmental reaction cell with formate (as electron donor via formate dehydrogenase) and powdered birnessite, a layered Mn3+,4+ oxide common to many soils. Using both synchrotron and conventional X-ray sources, we irradiated the reaction mixtures for up to two weeks and observed bioreduction and dissolution of birnessite and the concomitant precipitation of rhodochrosite [Mn2+CO3] and hausmannite [Mn2+ Mn23+O4]. The high time resolution of these experiments documented systematic changes in crystal structure during the breakdown of birnessite and the emergence of nanocarystalline rhodochrosite. In addition, the relative abundances of birnessite and rhodochrosite were quantified over time for different concentrations of TM fraction, allowing for the determination of rate equations that govern this bioreaction. Importantly, constant irradiation for two weeks did not stop the enzymatic reaction, suggesting that enzymes may be more resilient than whole cells when exposed to X-ray radiation.

Original languageEnglish (US)
Pages (from-to)1929-1932
Number of pages4
JournalAmerican Mineralogist
Volume93
Issue number11-12
DOIs
StatePublished - Nov 1 2008

Fingerprint

birnessite
rhodochrosite
Oxides
X-ray diffraction
oxide
X ray diffraction
formic acid
oxides
formates
diffraction
anaerobes
x rays
Formate Dehydrogenases
membrane
membranes
Membranes
X rays
dehydrogenases
cells
Synchrotrons

All Science Journal Classification (ASJC) codes

  • Geophysics
  • Geochemistry and Petrology

Cite this

Fischer, Timothy B. ; Heaney, Peter J. ; Jang, Je Hun ; Ross, Daniel E. ; Brantley, Susan Louise ; Post, Jeffrey E. ; Tien, Ming. / Continuous time-resolved X-ray diffraction of the biocatalyzed reduction of Mn oxide. In: American Mineralogist. 2008 ; Vol. 93, No. 11-12. pp. 1929-1932.
@article{1812b6f8e3c84cea9f6142b4d6da506f,
title = "Continuous time-resolved X-ray diffraction of the biocatalyzed reduction of Mn oxide",
abstract = "Here we report the first continuous time-resolved X-ray diffraction analysis of a biologically mediated mineral reaction. We incubated total membrane (TM) fractions of the facultative anaerobe Shewanella oneidensis in an anoxic environmental reaction cell with formate (as electron donor via formate dehydrogenase) and powdered birnessite, a layered Mn3+,4+ oxide common to many soils. Using both synchrotron and conventional X-ray sources, we irradiated the reaction mixtures for up to two weeks and observed bioreduction and dissolution of birnessite and the concomitant precipitation of rhodochrosite [Mn2+CO3] and hausmannite [Mn2+ Mn23+O4]. The high time resolution of these experiments documented systematic changes in crystal structure during the breakdown of birnessite and the emergence of nanocarystalline rhodochrosite. In addition, the relative abundances of birnessite and rhodochrosite were quantified over time for different concentrations of TM fraction, allowing for the determination of rate equations that govern this bioreaction. Importantly, constant irradiation for two weeks did not stop the enzymatic reaction, suggesting that enzymes may be more resilient than whole cells when exposed to X-ray radiation.",
author = "Fischer, {Timothy B.} and Heaney, {Peter J.} and Jang, {Je Hun} and Ross, {Daniel E.} and Brantley, {Susan Louise} and Post, {Jeffrey E.} and Ming Tien",
year = "2008",
month = "11",
day = "1",
doi = "10.2138/am.2008.3038",
language = "English (US)",
volume = "93",
pages = "1929--1932",
journal = "American Mineralogist",
issn = "0003-004X",
publisher = "Mineralogical Society of America",
number = "11-12",

}

Continuous time-resolved X-ray diffraction of the biocatalyzed reduction of Mn oxide. / Fischer, Timothy B.; Heaney, Peter J.; Jang, Je Hun; Ross, Daniel E.; Brantley, Susan Louise; Post, Jeffrey E.; Tien, Ming.

In: American Mineralogist, Vol. 93, No. 11-12, 01.11.2008, p. 1929-1932.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Continuous time-resolved X-ray diffraction of the biocatalyzed reduction of Mn oxide

AU - Fischer, Timothy B.

AU - Heaney, Peter J.

AU - Jang, Je Hun

AU - Ross, Daniel E.

AU - Brantley, Susan Louise

AU - Post, Jeffrey E.

AU - Tien, Ming

PY - 2008/11/1

Y1 - 2008/11/1

N2 - Here we report the first continuous time-resolved X-ray diffraction analysis of a biologically mediated mineral reaction. We incubated total membrane (TM) fractions of the facultative anaerobe Shewanella oneidensis in an anoxic environmental reaction cell with formate (as electron donor via formate dehydrogenase) and powdered birnessite, a layered Mn3+,4+ oxide common to many soils. Using both synchrotron and conventional X-ray sources, we irradiated the reaction mixtures for up to two weeks and observed bioreduction and dissolution of birnessite and the concomitant precipitation of rhodochrosite [Mn2+CO3] and hausmannite [Mn2+ Mn23+O4]. The high time resolution of these experiments documented systematic changes in crystal structure during the breakdown of birnessite and the emergence of nanocarystalline rhodochrosite. In addition, the relative abundances of birnessite and rhodochrosite were quantified over time for different concentrations of TM fraction, allowing for the determination of rate equations that govern this bioreaction. Importantly, constant irradiation for two weeks did not stop the enzymatic reaction, suggesting that enzymes may be more resilient than whole cells when exposed to X-ray radiation.

AB - Here we report the first continuous time-resolved X-ray diffraction analysis of a biologically mediated mineral reaction. We incubated total membrane (TM) fractions of the facultative anaerobe Shewanella oneidensis in an anoxic environmental reaction cell with formate (as electron donor via formate dehydrogenase) and powdered birnessite, a layered Mn3+,4+ oxide common to many soils. Using both synchrotron and conventional X-ray sources, we irradiated the reaction mixtures for up to two weeks and observed bioreduction and dissolution of birnessite and the concomitant precipitation of rhodochrosite [Mn2+CO3] and hausmannite [Mn2+ Mn23+O4]. The high time resolution of these experiments documented systematic changes in crystal structure during the breakdown of birnessite and the emergence of nanocarystalline rhodochrosite. In addition, the relative abundances of birnessite and rhodochrosite were quantified over time for different concentrations of TM fraction, allowing for the determination of rate equations that govern this bioreaction. Importantly, constant irradiation for two weeks did not stop the enzymatic reaction, suggesting that enzymes may be more resilient than whole cells when exposed to X-ray radiation.

UR - http://www.scopus.com/inward/record.url?scp=58049113686&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=58049113686&partnerID=8YFLogxK

U2 - 10.2138/am.2008.3038

DO - 10.2138/am.2008.3038

M3 - Article

AN - SCOPUS:58049113686

VL - 93

SP - 1929

EP - 1932

JO - American Mineralogist

JF - American Mineralogist

SN - 0003-004X

IS - 11-12

ER -