期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 112, 期 22, 页码 6882-6886出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1507063112
关键词
CO2-to-CO conversion; contemporary energy challenges; electrochemistry; catalysis; solar fuels
资金
- Societe d'acceleration du transfert de technologies Ile-de-France Innov [054]
Substitution of the four paraphenyl hydrogens of iron tetraphenylporphyrin by trimethylammonio groups provides a water-soluble molecule able to catalyze the electrochemical conversion of carbon dioxide into carbon monoxide. The reaction, performed in pH-neutral water, forms quasi-exclusively carbon monoxide with very little production of hydrogen, despite partial equilibration of CO2 with carbonic acid-a low pKa acid. This selective molecular catalyst is endowed with a good stability and a high turnover frequency. On this basis, prescribed composition of CO-H-2 mixtures can be obtained by adjusting the pH of the solution, optionally adding an electroinactive buffer. The development of these strategies will be greatly facilitated by the fact that one operates in water. The same applies for the association of the cathode compartment with a proton-producing anode by means of a suitable separator.
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