A Combined Theoretical and Experimental Approach for Platinum Catalyzed 1,2-Propanediol Aqueous Phase Reforming

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Abstract

Decomposition pathways of 1,2-propanediol (1,2-PDO) on platinum were investigated by means of experiments and quantum-mechanical calculations. Different reaction paths on a Pt(111) model surface were computationally screened. Gas and liquid phase products distribution for aqueous phase reforming of 1,2-PDO solutions was experimentally analyzed. A mechanistic approach was used to trace the preferred paths according to calculated activation barriers of the elementary steps; in this way, the presence or absence of some hypothesized intermediates in the experiments was computationally rationalized. Hydroxyacetone was demonstrated to be among the most favored decomposition products. The competition between C-H, O-H, and C-C bond cleavages was investigated, revealing that shortening of the carbon chain occurs most likely via decarbonylation steps. (Figure Presented).
Lingua originaleEnglish
pagine (da-a)14636-14648
Numero di pagine13
RivistaJOURNAL OF PHYSICAL CHEMISTRY. C
Volume121
Stato di pubblicazionePublished - 2017

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Propylene Glycol
Reforming reactions
Platinum
platinum
Decomposition
decomposition
products
cleavage
liquid phases
Carbon
Gases
Experiments
Chemical activation
activation
vapor phases
carbon
Liquids
acetol

All Science Journal Classification (ASJC) codes

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

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title = "A Combined Theoretical and Experimental Approach for Platinum Catalyzed 1,2-Propanediol Aqueous Phase Reforming",
abstract = "Decomposition pathways of 1,2-propanediol (1,2-PDO) on platinum were investigated by means of experiments and quantum-mechanical calculations. Different reaction paths on a Pt(111) model surface were computationally screened. Gas and liquid phase products distribution for aqueous phase reforming of 1,2-PDO solutions was experimentally analyzed. A mechanistic approach was used to trace the preferred paths according to calculated activation barriers of the elementary steps; in this way, the presence or absence of some hypothesized intermediates in the experiments was computationally rationalized. Hydroxyacetone was demonstrated to be among the most favored decomposition products. The competition between C-H, O-H, and C-C bond cleavages was investigated, revealing that shortening of the carbon chain occurs most likely via decarbonylation steps. (Figure Presented).",
author = "Dario Duca and Francesco Ferrante and Antonio Prestianni and Remedios Cortese and Roberto Schimmenti and Murzin, {Dmitry Yu.} and Lidia Godina",
year = "2017",
language = "English",
volume = "121",
pages = "14636--14648",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",

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TY - JOUR

T1 - A Combined Theoretical and Experimental Approach for Platinum Catalyzed 1,2-Propanediol Aqueous Phase Reforming

AU - Duca, Dario

AU - Ferrante, Francesco

AU - Prestianni, Antonio

AU - Cortese, Remedios

AU - Schimmenti, Roberto

AU - Murzin, Dmitry Yu.

AU - Godina, Lidia

PY - 2017

Y1 - 2017

N2 - Decomposition pathways of 1,2-propanediol (1,2-PDO) on platinum were investigated by means of experiments and quantum-mechanical calculations. Different reaction paths on a Pt(111) model surface were computationally screened. Gas and liquid phase products distribution for aqueous phase reforming of 1,2-PDO solutions was experimentally analyzed. A mechanistic approach was used to trace the preferred paths according to calculated activation barriers of the elementary steps; in this way, the presence or absence of some hypothesized intermediates in the experiments was computationally rationalized. Hydroxyacetone was demonstrated to be among the most favored decomposition products. The competition between C-H, O-H, and C-C bond cleavages was investigated, revealing that shortening of the carbon chain occurs most likely via decarbonylation steps. (Figure Presented).

AB - Decomposition pathways of 1,2-propanediol (1,2-PDO) on platinum were investigated by means of experiments and quantum-mechanical calculations. Different reaction paths on a Pt(111) model surface were computationally screened. Gas and liquid phase products distribution for aqueous phase reforming of 1,2-PDO solutions was experimentally analyzed. A mechanistic approach was used to trace the preferred paths according to calculated activation barriers of the elementary steps; in this way, the presence or absence of some hypothesized intermediates in the experiments was computationally rationalized. Hydroxyacetone was demonstrated to be among the most favored decomposition products. The competition between C-H, O-H, and C-C bond cleavages was investigated, revealing that shortening of the carbon chain occurs most likely via decarbonylation steps. (Figure Presented).

UR - http://hdl.handle.net/10447/241748

UR - http://pubs.acs.org/journal/jpccck

M3 - Article

VL - 121

SP - 14636

EP - 14648

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

ER -