Electroactive Nanoporous Metal Oxides and Chalcogenides by Chemical Design

Christopher H. Hendon; Keith T. Butler; Alex M. Ganose; Yuriy Román-Leshkov; David O. Scanlon; Geoffrey A. Ozin; Aron Walsh

doi:10.1021/acs.chemmater.7b00464

Electroactive Nanoporous Metal Oxides and Chalcogenides by Chemical Design

Christopher H. Hendon, Keith T. Butler, Alex M. Ganose, Yuriy Román-Leshkov, David O. Scanlon, Geoffrey A. Ozin, Aron Walsh

Department of Physics

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

The archetypal silica- and aluminosilicate-based zeolite-type materials are renowned for wide-ranging applications in heterogeneous catalysis, gas-separation and ion-exchange. Their compositional space can be expanded to include nanoporous metal chalcogenides, exemplified by germanium and tin sulfides and selenides. By comparison with the properties of bulk metal dichalcogenides and their 2D derivatives, these open-framework analogues may be viewed as three-dimensional semiconductors filled with nanometer voids. Applications exist in a range of molecule size and shape discriminating devices. However, what is the electronic structure of nanoporous metal chalcogenides? Herein, materials modeling is used to describe the properties of a homologous series of nanoporous metal chalcogenides denoted np-MX₂, where M = Si, Ge, Sn, Pb, and X = O, S, Se, Te, with Sodalite, LTA and aluminum chromium phosphate-1 structure types. Depending on the choice of metal and anion their properties can be tuned from insulators to semiconductors to metals with additional modification achieved through doping, solid solutions, and inclusion (with fullerene, quantum dots, and hole transport materials). These systems form the basis of a new branch of semiconductor nanochemistry in three dimensions.

Original language	English
Pages (from-to)	3663-3670
Number of pages	8
Journal	Chemistry of Materials
Volume	29
Issue number	8
DOIs	https://doi.org/10.1021/acs.chemmater.7b00464
State	Published - 25 Apr 2017

Bibliographical note

Funding Information:
A.W., K.T.B., and C.H.H. are supported by the Royal Society, the EPSRC (Grant EP/M009580/1) and the ERC (Grant 277757). D.O.S. and A.W. acknowledge membership of the Materials Design Network. A.M.G. acknowledges Diamond Light Source for the cosponsorship of a studentship on the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science (EP/L015862/1). GAO is a Government of Canada Research Chair in Materials Chemistry and Nanochemistry. He deeply appreciates the strong and sustained support of his research from the Natural Sciences and Engineering Research Council of Canada. This work benefitted from access to the ARCHER, through the UK High Performance Computing Consortium, which is funded by EPSRC Grant EP/L000202, and access to XSEDE Grant Number AC-1053575.

Publisher Copyright:
© 2017 American Chemical Society.

Access to Document

10.1021/acs.chemmater.7b00464

Cite this

@article{f157443add28464d94ea572471f1edc3,

title = "Electroactive Nanoporous Metal Oxides and Chalcogenides by Chemical Design",

abstract = "The archetypal silica- and aluminosilicate-based zeolite-type materials are renowned for wide-ranging applications in heterogeneous catalysis, gas-separation and ion-exchange. Their compositional space can be expanded to include nanoporous metal chalcogenides, exemplified by germanium and tin sulfides and selenides. By comparison with the properties of bulk metal dichalcogenides and their 2D derivatives, these open-framework analogues may be viewed as three-dimensional semiconductors filled with nanometer voids. Applications exist in a range of molecule size and shape discriminating devices. However, what is the electronic structure of nanoporous metal chalcogenides? Herein, materials modeling is used to describe the properties of a homologous series of nanoporous metal chalcogenides denoted np-MX2, where M = Si, Ge, Sn, Pb, and X = O, S, Se, Te, with Sodalite, LTA and aluminum chromium phosphate-1 structure types. Depending on the choice of metal and anion their properties can be tuned from insulators to semiconductors to metals with additional modification achieved through doping, solid solutions, and inclusion (with fullerene, quantum dots, and hole transport materials). These systems form the basis of a new branch of semiconductor nanochemistry in three dimensions.",

author = "Hendon, {Christopher H.} and Butler, {Keith T.} and Ganose, {Alex M.} and Yuriy Rom{\'a}n-Leshkov and Scanlon, {David O.} and Ozin, {Geoffrey A.} and Aron Walsh",

note = "Funding Information: A.W., K.T.B., and C.H.H. are supported by the Royal Society, the EPSRC (Grant EP/M009580/1) and the ERC (Grant 277757). D.O.S. and A.W. acknowledge membership of the Materials Design Network. A.M.G. acknowledges Diamond Light Source for the cosponsorship of a studentship on the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science (EP/L015862/1). GAO is a Government of Canada Research Chair in Materials Chemistry and Nanochemistry. He deeply appreciates the strong and sustained support of his research from the Natural Sciences and Engineering Research Council of Canada. This work benefitted from access to the ARCHER, through the UK High Performance Computing Consortium, which is funded by EPSRC Grant EP/L000202, and access to XSEDE Grant Number AC-1053575. Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

year = "2017",

month = apr,

day = "25",

doi = "10.1021/acs.chemmater.7b00464",

language = "English",

volume = "29",

pages = "3663--3670",

journal = "Chemistry of Materials",

issn = "0897-4756",

publisher = "American Chemical Society",

number = "8",

}

TY - JOUR

T1 - Electroactive Nanoporous Metal Oxides and Chalcogenides by Chemical Design

AU - Hendon, Christopher H.

AU - Butler, Keith T.

AU - Ganose, Alex M.

AU - Román-Leshkov, Yuriy

AU - Scanlon, David O.

AU - Ozin, Geoffrey A.

AU - Walsh, Aron

N1 - Funding Information: A.W., K.T.B., and C.H.H. are supported by the Royal Society, the EPSRC (Grant EP/M009580/1) and the ERC (Grant 277757). D.O.S. and A.W. acknowledge membership of the Materials Design Network. A.M.G. acknowledges Diamond Light Source for the cosponsorship of a studentship on the EPSRC Centre for Doctoral Training in Molecular Modelling and Materials Science (EP/L015862/1). GAO is a Government of Canada Research Chair in Materials Chemistry and Nanochemistry. He deeply appreciates the strong and sustained support of his research from the Natural Sciences and Engineering Research Council of Canada. This work benefitted from access to the ARCHER, through the UK High Performance Computing Consortium, which is funded by EPSRC Grant EP/L000202, and access to XSEDE Grant Number AC-1053575. Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/4/25

Y1 - 2017/4/25

N2 - The archetypal silica- and aluminosilicate-based zeolite-type materials are renowned for wide-ranging applications in heterogeneous catalysis, gas-separation and ion-exchange. Their compositional space can be expanded to include nanoporous metal chalcogenides, exemplified by germanium and tin sulfides and selenides. By comparison with the properties of bulk metal dichalcogenides and their 2D derivatives, these open-framework analogues may be viewed as three-dimensional semiconductors filled with nanometer voids. Applications exist in a range of molecule size and shape discriminating devices. However, what is the electronic structure of nanoporous metal chalcogenides? Herein, materials modeling is used to describe the properties of a homologous series of nanoporous metal chalcogenides denoted np-MX2, where M = Si, Ge, Sn, Pb, and X = O, S, Se, Te, with Sodalite, LTA and aluminum chromium phosphate-1 structure types. Depending on the choice of metal and anion their properties can be tuned from insulators to semiconductors to metals with additional modification achieved through doping, solid solutions, and inclusion (with fullerene, quantum dots, and hole transport materials). These systems form the basis of a new branch of semiconductor nanochemistry in three dimensions.

AB - The archetypal silica- and aluminosilicate-based zeolite-type materials are renowned for wide-ranging applications in heterogeneous catalysis, gas-separation and ion-exchange. Their compositional space can be expanded to include nanoporous metal chalcogenides, exemplified by germanium and tin sulfides and selenides. By comparison with the properties of bulk metal dichalcogenides and their 2D derivatives, these open-framework analogues may be viewed as three-dimensional semiconductors filled with nanometer voids. Applications exist in a range of molecule size and shape discriminating devices. However, what is the electronic structure of nanoporous metal chalcogenides? Herein, materials modeling is used to describe the properties of a homologous series of nanoporous metal chalcogenides denoted np-MX2, where M = Si, Ge, Sn, Pb, and X = O, S, Se, Te, with Sodalite, LTA and aluminum chromium phosphate-1 structure types. Depending on the choice of metal and anion their properties can be tuned from insulators to semiconductors to metals with additional modification achieved through doping, solid solutions, and inclusion (with fullerene, quantum dots, and hole transport materials). These systems form the basis of a new branch of semiconductor nanochemistry in three dimensions.

UR - http://www.scopus.com/inward/record.url?scp=85018661766&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.7b00464

DO - 10.1021/acs.chemmater.7b00464

M3 - Article

AN - SCOPUS:85018661766

SN - 0897-4756

VL - 29

SP - 3663

EP - 3670

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 8

ER -

Electroactive Nanoporous Metal Oxides and Chalcogenides by Chemical Design

Abstract

Bibliographical note

Access to Document

Fingerprint

Cite this