期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 113, 期 10, 页码 2579-2584出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1516945113
关键词
solar fuel; CO2 reduction; water splitting; photochemistry; Fischer-Tropsch
资金
- National Science Foundation [CHE-1301332]
- Robert A. Welch Foundation [Y-1301]
- University of Texas at Arlington Center for Renewable Science and Technology (CREST)
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1301332] Funding Source: National Science Foundation
A one-step, gas-phase photothermocatalytic process for the synthesis of hydrocarbons, including liquid alkanes, aromatics, and oxygenates, with carbon numbers (C-n) up to C-13, from CO2 and water is demonstrated in a flow photoreactor operating at elevated temperatures (180-200 degrees C) and pressures (1-6 bar) using a 5% cobalt on TiO2 catalyst and under UV irradiation. A parametric study of temperature, pressure, and partial pressure ratio revealed that temperatures in excess of 160 degrees C are needed to obtain the higher C-n products in quantity and that the product distribution shifts toward higher C-n products with increasing pressure. In the best run so far, over 13% by mass of the products were C-5+ hydrocarbons and some of these, i.e., octane, are drop-in replacements for existing liquid hydrocarbons fuels. Dioxygen was detected in yields ranging between 64% and 150%. In principle, this tandem photochemical-thermochemical process, fitted with a photocatalyst better matched to the solar spectrum, could provide a cheap and direct method to produce liquid hydrocarbons from CO2 and water via a solar process which uses concentrated sunlight for both photochemical excitation to generate high-energy intermediates and heat to drive important thermochemical carbonchain-forming reactions.
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