Microscopic identification of a bimolecular reaction intermediate

Hiroshi Uetsuka; Akira Sasahara; Akira Yamakata; Hiroshi Onishi

doi:10.1021/jp026253r

Microscopic identification of a bimolecular reaction intermediate

Hiroshi Uetsuka, Akira Sasahara, Akira Yamakata, Hiroshi Onishi

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

18 Citations (Scopus)

Abstract

How a molecule impinging from an ambient phase attaches to and reacts with a preadsorbed reactant was studied by scanning tunneling microscopy (STM). A carboxylate (RCOO^-) chemisorbed on a TiO₂(110) surface was exchanged by another carboxylate (R′COO^-) via an S_N2-like mechanism when the RCOO^--covered TiO₂ surface was exposed to R′COOH vapor at room temperature or below. An R′COOH impinging from the gas phase was temporarily bound to a preadsorbed RCOO^- yielding a bimolecular intermediate. The trapped R′COOH was inserted into the monolayer and dissociated to produce an adsorbed R′COO^-. One of the carboxylates (RCOO^- or R′COO^-) was then pushed out of the monolayer to restore the intermediate and released to the vapor phase. The individual reaction steps were resolved using time-lapse imaging.

Original language	English
Pages (from-to)	11549-11552
Number of pages	4
Journal	Journal of Physical Chemistry B
Volume	106
Issue number	44
DOIs	https://doi.org/10.1021/jp026253r
Publication status	Published - Nov 7 2002
Externally published	Yes

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Surfaces, Coatings and Films
Materials Chemistry

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10.1021/jp026253r

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abstract = "How a molecule impinging from an ambient phase attaches to and reacts with a preadsorbed reactant was studied by scanning tunneling microscopy (STM). A carboxylate (RCOO-) chemisorbed on a TiO2(110) surface was exchanged by another carboxylate (R′COO-) via an SN2-like mechanism when the RCOO--covered TiO2 surface was exposed to R′COOH vapor at room temperature or below. An R′COOH impinging from the gas phase was temporarily bound to a preadsorbed RCOO- yielding a bimolecular intermediate. The trapped R′COOH was inserted into the monolayer and dissociated to produce an adsorbed R′COO-. One of the carboxylates (RCOO- or R′COO-) was then pushed out of the monolayer to restore the intermediate and released to the vapor phase. The individual reaction steps were resolved using time-lapse imaging.",

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T1 - Microscopic identification of a bimolecular reaction intermediate

AU - Uetsuka, Hiroshi

AU - Sasahara, Akira

AU - Yamakata, Akira

AU - Onishi, Hiroshi

PY - 2002/11/7

Y1 - 2002/11/7

N2 - How a molecule impinging from an ambient phase attaches to and reacts with a preadsorbed reactant was studied by scanning tunneling microscopy (STM). A carboxylate (RCOO-) chemisorbed on a TiO2(110) surface was exchanged by another carboxylate (R′COO-) via an SN2-like mechanism when the RCOO--covered TiO2 surface was exposed to R′COOH vapor at room temperature or below. An R′COOH impinging from the gas phase was temporarily bound to a preadsorbed RCOO- yielding a bimolecular intermediate. The trapped R′COOH was inserted into the monolayer and dissociated to produce an adsorbed R′COO-. One of the carboxylates (RCOO- or R′COO-) was then pushed out of the monolayer to restore the intermediate and released to the vapor phase. The individual reaction steps were resolved using time-lapse imaging.

AB - How a molecule impinging from an ambient phase attaches to and reacts with a preadsorbed reactant was studied by scanning tunneling microscopy (STM). A carboxylate (RCOO-) chemisorbed on a TiO2(110) surface was exchanged by another carboxylate (R′COO-) via an SN2-like mechanism when the RCOO--covered TiO2 surface was exposed to R′COOH vapor at room temperature or below. An R′COOH impinging from the gas phase was temporarily bound to a preadsorbed RCOO- yielding a bimolecular intermediate. The trapped R′COOH was inserted into the monolayer and dissociated to produce an adsorbed R′COO-. One of the carboxylates (RCOO- or R′COO-) was then pushed out of the monolayer to restore the intermediate and released to the vapor phase. The individual reaction steps were resolved using time-lapse imaging.

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Microscopic identification of a bimolecular reaction intermediate

Abstract

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