A density functional theory and experimental study of CO 2 interaction with brookite TiO 2

Monique M. Rodriguez, Xihong Peng, Lianjun Liu, Ying Li, Jean Andino

Research output: Contribution to journalArticle

50 Citations (Scopus)

Abstract

The interactions of CO 2 with the (210) surface of brookite TiO 2 were studied using first-principle calculations on cluster and periodic slab systems. Charge and spin density analyses were implemented to determine if charge transfer to the CO 2 molecule occurred and whether this charge transfer was comparable to that seen with the anatase TiO 2 (101) surface. Although the brookite (210) surface provided energetically similar CO 2 interactions as compared to the anatase (101) surface, the brookite surface had negligible charge transfer to the CO 2 molecule. This result suggests that unmodified brookite is not a suitable catalyst for the reduction of CO 2. However, the results also suggest that modification of the brookite surface through the creation of oxygen vacancies may lead to enhancements in CO 2 reduction. The computational results were supported with laboratory data for CO 2 interaction with perfect brookite and oxygen-deficient brookite. The laboratory data, generated using diffuse reflectance Fourier transform infrared spectroscopy, confirms the presence of CO 2 - at significant levels on the oxygen-deficient brookite.

Original languageEnglish (US)
Pages (from-to)19755-19764
Number of pages10
JournalJournal of Physical Chemistry C
Volume116
Issue number37
DOIs
StatePublished - Sep 20 2012

Fingerprint

Carbon Monoxide
Density functional theory
density functional theory
Charge transfer
charge transfer
interactions
anatase
Titanium dioxide
oxygen
Molecules
Oxygen
Oxygen vacancies
Fourier transform infrared spectroscopy
titanium dioxide
molecules
slabs
infrared spectroscopy
reflectance
catalysts
Catalysts

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

A density functional theory and experimental study of CO 2 interaction with brookite TiO 2 . / Rodriguez, Monique M.; Peng, Xihong; Liu, Lianjun; Li, Ying; Andino, Jean.

In: Journal of Physical Chemistry C, Vol. 116, No. 37, 20.09.2012, p. 19755-19764.

Research output: Contribution to journalArticle

@article{b228ee9bf44a4c64a37389f8e9a98085,
title = "A density functional theory and experimental study of CO 2 interaction with brookite TiO 2",
abstract = "The interactions of CO 2 with the (210) surface of brookite TiO 2 were studied using first-principle calculations on cluster and periodic slab systems. Charge and spin density analyses were implemented to determine if charge transfer to the CO 2 molecule occurred and whether this charge transfer was comparable to that seen with the anatase TiO 2 (101) surface. Although the brookite (210) surface provided energetically similar CO 2 interactions as compared to the anatase (101) surface, the brookite surface had negligible charge transfer to the CO 2 molecule. This result suggests that unmodified brookite is not a suitable catalyst for the reduction of CO 2. However, the results also suggest that modification of the brookite surface through the creation of oxygen vacancies may lead to enhancements in CO 2 reduction. The computational results were supported with laboratory data for CO 2 interaction with perfect brookite and oxygen-deficient brookite. The laboratory data, generated using diffuse reflectance Fourier transform infrared spectroscopy, confirms the presence of CO 2 - at significant levels on the oxygen-deficient brookite.",
author = "Rodriguez, {Monique M.} and Xihong Peng and Lianjun Liu and Ying Li and Jean Andino",
year = "2012",
month = "9",
day = "20",
doi = "10.1021/jp302342t",
language = "English (US)",
volume = "116",
pages = "19755--19764",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "37",

}

TY - JOUR

T1 - A density functional theory and experimental study of CO 2 interaction with brookite TiO 2

AU - Rodriguez, Monique M.

AU - Peng, Xihong

AU - Liu, Lianjun

AU - Li, Ying

AU - Andino, Jean

PY - 2012/9/20

Y1 - 2012/9/20

N2 - The interactions of CO 2 with the (210) surface of brookite TiO 2 were studied using first-principle calculations on cluster and periodic slab systems. Charge and spin density analyses were implemented to determine if charge transfer to the CO 2 molecule occurred and whether this charge transfer was comparable to that seen with the anatase TiO 2 (101) surface. Although the brookite (210) surface provided energetically similar CO 2 interactions as compared to the anatase (101) surface, the brookite surface had negligible charge transfer to the CO 2 molecule. This result suggests that unmodified brookite is not a suitable catalyst for the reduction of CO 2. However, the results also suggest that modification of the brookite surface through the creation of oxygen vacancies may lead to enhancements in CO 2 reduction. The computational results were supported with laboratory data for CO 2 interaction with perfect brookite and oxygen-deficient brookite. The laboratory data, generated using diffuse reflectance Fourier transform infrared spectroscopy, confirms the presence of CO 2 - at significant levels on the oxygen-deficient brookite.

AB - The interactions of CO 2 with the (210) surface of brookite TiO 2 were studied using first-principle calculations on cluster and periodic slab systems. Charge and spin density analyses were implemented to determine if charge transfer to the CO 2 molecule occurred and whether this charge transfer was comparable to that seen with the anatase TiO 2 (101) surface. Although the brookite (210) surface provided energetically similar CO 2 interactions as compared to the anatase (101) surface, the brookite surface had negligible charge transfer to the CO 2 molecule. This result suggests that unmodified brookite is not a suitable catalyst for the reduction of CO 2. However, the results also suggest that modification of the brookite surface through the creation of oxygen vacancies may lead to enhancements in CO 2 reduction. The computational results were supported with laboratory data for CO 2 interaction with perfect brookite and oxygen-deficient brookite. The laboratory data, generated using diffuse reflectance Fourier transform infrared spectroscopy, confirms the presence of CO 2 - at significant levels on the oxygen-deficient brookite.

UR - http://www.scopus.com/inward/record.url?scp=84866690469&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84866690469&partnerID=8YFLogxK

U2 - 10.1021/jp302342t

DO - 10.1021/jp302342t

M3 - Article

VL - 116

SP - 19755

EP - 19764

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 37

ER -