Advanced

Surface Properties of Nanocrystalline PbS Films Deposited at the Water-Oil Interface: A Study of Atmospheric Aging

Cant, David J. H.; Syres, Karen L.; Lunt, Patrick J. B.; Radtke, Hanna; Treacy, Jon; Thomas, P. John; Lewis, Edward A.; Haigh, Sarah J.; O'Brien, Paul and Schulte, Karina LU , et al. (2015) In Langmuir 31(4). p.1445-1453
Abstract
Nanocrystalline thin films of PbS are obtained in a straightforward reaction by precipitation at the interface between toluene (containing a Pb precursor) and water (containing Na2S). Lead thiobiuret [Pb(SON(CN(i)Pr-2)(2))(2)] and lead diethyldithiocarbamate [Pb(S2CNEt2)(2)] precursors are used. The films are characterized by X-ray diffraction and electron microscopy, revealing typical particle sizes of 10-40 nm and preferred (200) orientation. Synchrotron-excited depth-profiling X-ray photoelectron spectroscopy (XPS) is used to determine the depth-dependent chemical composition as a function of surface aging in air for periods of up to 9 months. The as-synthesized films show a 1:1 Pb/S composition. Initial degradation occurs to form lead... (More)
Nanocrystalline thin films of PbS are obtained in a straightforward reaction by precipitation at the interface between toluene (containing a Pb precursor) and water (containing Na2S). Lead thiobiuret [Pb(SON(CN(i)Pr-2)(2))(2)] and lead diethyldithiocarbamate [Pb(S2CNEt2)(2)] precursors are used. The films are characterized by X-ray diffraction and electron microscopy, revealing typical particle sizes of 10-40 nm and preferred (200) orientation. Synchrotron-excited depth-profiling X-ray photoelectron spectroscopy (XPS) is used to determine the depth-dependent chemical composition as a function of surface aging in air for periods of up to 9 months. The as-synthesized films show a 1:1 Pb/S composition. Initial degradation occurs to form lead hydroxide and small quantities of surface-adsorbed -SH species. A lead-deficient Pb1-xS phase is produced as the aging proceeds. Oxidation of the sulfur occurs later to form sulfite and sulfate products that are highly localized at the surface layers of the nanocrystals. These species show logarithmic growth kinetics, demonstrating that the sulfite/sulfate layer acts to passivate the nanocrystals. Our results demonstrate that the initial reaction of the PbS nanocrystals (forming lead hydroxide) is incongruent. The results are discussed in the context of the use of PbS nanocrystals as light-harvesting elements in next-generation solar technology. (Less)
Please use this url to cite or link to this publication:
author
, et al. (More)
(Less)
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Langmuir
volume
31
issue
4
pages
1445 - 1453
publisher
The American Chemical Society
external identifiers
  • wos:000349059200026
  • scopus:84922245204
ISSN
0743-7463
DOI
10.1021/la504779h
language
English
LU publication?
yes
id
51a195dd-8c26-484b-ab5a-9e403136ed55 (old id 5175920)
date added to LUP
2015-03-25 13:19:55
date last changed
2017-09-17 03:00:40
@article{51a195dd-8c26-484b-ab5a-9e403136ed55,
  abstract     = {Nanocrystalline thin films of PbS are obtained in a straightforward reaction by precipitation at the interface between toluene (containing a Pb precursor) and water (containing Na2S). Lead thiobiuret [Pb(SON(CN(i)Pr-2)(2))(2)] and lead diethyldithiocarbamate [Pb(S2CNEt2)(2)] precursors are used. The films are characterized by X-ray diffraction and electron microscopy, revealing typical particle sizes of 10-40 nm and preferred (200) orientation. Synchrotron-excited depth-profiling X-ray photoelectron spectroscopy (XPS) is used to determine the depth-dependent chemical composition as a function of surface aging in air for periods of up to 9 months. The as-synthesized films show a 1:1 Pb/S composition. Initial degradation occurs to form lead hydroxide and small quantities of surface-adsorbed -SH species. A lead-deficient Pb1-xS phase is produced as the aging proceeds. Oxidation of the sulfur occurs later to form sulfite and sulfate products that are highly localized at the surface layers of the nanocrystals. These species show logarithmic growth kinetics, demonstrating that the sulfite/sulfate layer acts to passivate the nanocrystals. Our results demonstrate that the initial reaction of the PbS nanocrystals (forming lead hydroxide) is incongruent. The results are discussed in the context of the use of PbS nanocrystals as light-harvesting elements in next-generation solar technology.},
  author       = {Cant, David J. H. and Syres, Karen L. and Lunt, Patrick J. B. and Radtke, Hanna and Treacy, Jon and Thomas, P. John and Lewis, Edward A. and Haigh, Sarah J. and O'Brien, Paul and Schulte, Karina and Bondino, Federica and Magnano, Elena and Flavell, Wendy R.},
  issn         = {0743-7463},
  language     = {eng},
  number       = {4},
  pages        = {1445--1453},
  publisher    = {The American Chemical Society},
  series       = {Langmuir},
  title        = {Surface Properties of Nanocrystalline PbS Films Deposited at the Water-Oil Interface: A Study of Atmospheric Aging},
  url          = {http://dx.doi.org/10.1021/la504779h},
  volume       = {31},
  year         = {2015},
}