Tailoring the Grain Boundary Chemistry of Polymeric Carbon Nitride for Enhanced Solar Hydrogen Production and CO2 Reduction

Photocatalytic water splitting is a promising and clean way to mimic plant photosynthesis in a sustainable manner. Improvements of the quantum efficiency and optical absorption in the relevant range are necessary steps to approach practicality. Herein, we reported that these issues can be readily ad...

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Published inAngewandte Chemie International Edition Vol. 58; no. 11; pp. 3433 - 3437
Main Authors Zhang, Guigang, Li, Guosheng, Heil, Tobias, Zafeiratos, Spiros, Lai, Feili, Savateev, Aleksandr, Antonietti, Markus, Wang, Xinchen
Format Journal Article
LanguageEnglish
Published Weinheim Wiley Subscription Services, Inc 11.03.2019
EditionInternational ed. in English
Subjects
Carbon
Carbon dioxide
carbon dioxide reduction
Carbon nitride
Chemical reduction
Grain boundaries
Hydrogen production
Localization
Molten salts
Organic chemistry
Oxidation
photocatalysis
Photosynthesis
polymeric carbon nitride
Potassium chloride
Potassium phosphate
Potassium phosphates
Quantum efficiency
Sodium chloride
Solar energy
Water splitting
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Summary:Photocatalytic water splitting is a promising and clean way to mimic plant photosynthesis in a sustainable manner. Improvements of the quantum efficiency and optical absorption in the relevant range are necessary steps to approach practicality. Herein, we reported that these issues can be readily addressed when 5‐aminotetrazole, a monomer with high nitrogen content, is used for the synthesis of carbon nitride. The molten salt mixture NaCl/KCl is used as a high‐temperature solvent to tailor the grain boundary structure and chemistry. Visible light quantum efficiency for H2 production of 0.65 could be obtained in the presence of K2HPO4 as a double layer modifier. This value is very high, considering that this number depends on light to charge couple conversion, charge localization, as well as a successful oxidation and reduction reaction. Polymeric carbon nitride with enhanced optical absorption and photocatalytic activities is synthesized via a one‐pot ionothermal polymerization of 5‐aminotetrazole in eutectic NaCl/KCl. This approach allows control of the polymerization process and tailoring of the grain boundary structure and catalytic properties.
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ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.201811938