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@ARTICLE{Ayalew:422544,
author = {Ayalew, Eyasu and Janssens, Koen and De Wael, Karolien},
title = {{U}nraveling the {R}eactivity of {M}inium toward
{B}icarbonate and the {R}ole of {L}ead {O}xides {T}herein},
journal = {Analytical chemistry},
volume = {88},
number = {3},
issn = {1520-6882},
address = {Columbus, Ohio},
publisher = {American Chemical Society},
reportid = {PUBDB-2019-02230},
pages = {1564 - 1569},
year = {2016},
note = {© American Chemical Society; Post referee fulltext in
progress 2; Embargo 12 months from publication},
abstract = {Understanding the reactivity of (semiconductor) pigments
provides vital information on how to improve conservation
strategies for works of art to avoid rapid degradation of
the pigments. This study focuses on the photoactivity of
minium (Pb$_3$O$_4$), a semiconductor pigment that gives
rise to strong discoloration phenomena upon exposure to
various environmental conditions. For demonstrating its
photoactivity, an electrochemical setup with a
minium-modified graphite electrode (C|Pb$_3$O$_4$) was used.
It is confirmed that minium is a p-type semiconductor that
is photoactive during illumination and becomes inactive in
the dark. Raman measurements confirm the formation of
degradation products. The photoactivity of a semiconductor
pigment is partly defined by the presence of lead oxide
(PbO) impurities; these introduce new states in the original
band gap. It will be experimentally evidenced that the
presence of PbO particles in minium leads to an upward shift
of the valence band that reduces the band gap. Thus, upon
photoexcitation, the electron/hole separation is more easily
initialized. The PbO/Pb$_3$O$_4$ composite electrodes
demonstrate a higher reductive photocurrent compared to the
photocurrent registered at pure PbO or Pb$_3$O$_4$-modified
electrodes. Upon exposure to light with energy close to and
above the band gap, electrons are excited from the valence
band to the conduction band to initialize the reduction of
Pb(IV) to Pb(II), resulting in the initial formation of PbO.
However, in the presence of bicarbonate ions, a
significantly higher photoreduction current is recorded
because the PbO reacts further to form hydrocerussite.
Therefore, the presence of bicarbonates in the environment
stimulates the photodecomposition process of minium and
plays an important role in the degradation process.},
cin = {DOOR},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G3 - PETRA III (POF3-622)},
pid = {G:(DE-HGF)POF3-6G3},
experiment = {EXP:(DE-H253)P-P06-20150101},
typ = {PUB:(DE-HGF)36 / PUB:(DE-HGF)16},
pubmed = {pmid:26720157},
UT = {WOS:000369471100014},
doi = {10.1021/acs.analchem.5b02503},
url = {https://bib-pubdb1.desy.de/record/422544},
}