Robust Binding between Carbon Nitride Nanosheets and a Binuclear Ruthenium(II) Complex Enabling Durable, Selective CO2 Reduction under Visible Light in Aqueous Solution

Ryo Kuriki; Muneaki Yamamoto; Kimitaka Higuchi; Yuta Yamamoto; Masato Akatsuka; Daling Lu; Shinya Yagi; Tomoko Yoshida; Osamu Ishitani; Kazuhiko Maeda

doi:10.1002/anie.201701627

Robust Binding between Carbon Nitride Nanosheets and a Binuclear Ruthenium(II) Complex Enabling Durable, Selective CO₂ Reduction under Visible Light in Aqueous Solution

Angew Chem Int Ed Engl. 2017 Apr 18;56(17):4867-4871. doi: 10.1002/anie.201701627.

Authors

Affiliations

¹ Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo, 152-8550, Japan.
² Advanced Research Institute for Natural Science and Technology, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka, 558-8585, Japan.
³ Institute of Materials and Systems for Sustainability, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, 464-8603, Japan.
⁴ Suzukakedai Materials Analysis Division, Technical Department, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan.

PMID: 28387039
DOI: 10.1002/anie.201701627

Abstract

Carbon nitride nanosheets (NS-C₃ N₄ ) were found to undergo robust binding with a binuclear ruthenium(II) complex (RuRu') even in basic aqueous solution. A hybrid material consisting of NS-C₃ N₄ (further modified with nanoparticulate Ag) and RuRu' promoted the photocatalytic reduction of CO₂ to formate in aqueous media, in conjunction with high selectivity (approximately 98 %) and a good turnover number (>2000 with respect to the loaded Ru complex). These represent the highest values yet reported for a powder-based photocatalytic system during CO₂ reduction under visible light in an aqueous environment. We also assessed the desorption of RuRu' from the Ag/C₃ N₄ surface, a factor that can contribute to a loss of activity. It was determined that desorption is not induced by salt additives, pH changes, or photoirradiation, which partly explains the high photocatalytic performance of this material.

Keywords: CO2 fixation; artificial photosynthesis; carbon nitride; formate; heterogeneous photocatalysis.

Publication types

Research Support, Non-U.S. Gov't