Photocatalytic reduction of CO2 under supercritical CO 2 conditions: Effect of pressure, temperature, and solvent on catalytic efficiency

Hajime Kawanami, David Grills, Takayuki Ishizaka, Maya Chatterjee, Akira Suzuki

Research output: Contribution to journalArticle

4 Citations (Scopus)

Abstract

The photocatalytic reduction of CO2 to CO in single-phase, high-pressure mixtures of supercritical CO2 and N,N-dimethylformamide (DMF), using fac-ReCl(bpy)(CO)3 as a catalyst in the presence of triethanolamine as a sacrificial electron donor has been investigated. The catalytic efficiency was found to be strongly influenced by both the CO 2 and DMF concentrations. For example, the turnover number (TON) for CO formation increases linearly with CO2 pressure up to 60 at 17.8 MPa/60 C. It also increases dramatically as the [DMF] is increased from 3.8 to 6.3 M, and then remains almost constant with further increases in [DMF]. This resulted in an optimized TON of 62 at 17.8 MPa CO2/60 C and [DMF] = 6.3 M, and an initial turnover frequency (TOF) of ∼56 h-1 at 17.8 MPa CO2/60 C and [DMF] = 11.4 M. These values are 5× and 2.3× higher, respectively than those obtained under biphasic low-pressure conditions (0.1 MPa CO2), demonstrating that significant improvements in catalytic performance are possible through the use of high concentrations of CO2. Manipulation of the incident light intensity led to further improvements in both TON (up to 72 under low light levels) and TOF (up to 117 h-1 under the highest light level investigated).

Original languageEnglish
Pages (from-to)93-97
Number of pages5
JournalJournal of CO2 Utilization
Volume3-4
DOIs
Publication statusPublished - 2013

Fingerprint

Dimethylformamide
Carbon Monoxide
turnover
temperature
Temperature
Triethanolamine
light intensity
low pressure
catalyst
effect
electron
Catalysts
Electrons

Keywords

  • Photocatalytic CO reduction
  • Rhenium catalyst
  • Supercritical CO
  • Turnover frequency
  • Turnover number

ASJC Scopus subject areas

  • Chemical Engineering (miscellaneous)
  • Process Chemistry and Technology
  • Waste Management and Disposal

Cite this

Photocatalytic reduction of CO2 under supercritical CO 2 conditions : Effect of pressure, temperature, and solvent on catalytic efficiency. / Kawanami, Hajime; Grills, David; Ishizaka, Takayuki; Chatterjee, Maya; Suzuki, Akira.

In: Journal of CO2 Utilization, Vol. 3-4, 2013, p. 93-97.

Research output: Contribution to journalArticle

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AB - The photocatalytic reduction of CO2 to CO in single-phase, high-pressure mixtures of supercritical CO2 and N,N-dimethylformamide (DMF), using fac-ReCl(bpy)(CO)3 as a catalyst in the presence of triethanolamine as a sacrificial electron donor has been investigated. The catalytic efficiency was found to be strongly influenced by both the CO 2 and DMF concentrations. For example, the turnover number (TON) for CO formation increases linearly with CO2 pressure up to 60 at 17.8 MPa/60 C. It also increases dramatically as the [DMF] is increased from 3.8 to 6.3 M, and then remains almost constant with further increases in [DMF]. This resulted in an optimized TON of 62 at 17.8 MPa CO2/60 C and [DMF] = 6.3 M, and an initial turnover frequency (TOF) of ∼56 h-1 at 17.8 MPa CO2/60 C and [DMF] = 11.4 M. These values are 5× and 2.3× higher, respectively than those obtained under biphasic low-pressure conditions (0.1 MPa CO2), demonstrating that significant improvements in catalytic performance are possible through the use of high concentrations of CO2. Manipulation of the incident light intensity led to further improvements in both TON (up to 72 under low light levels) and TOF (up to 117 h-1 under the highest light level investigated).

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