2026-09-07 東北大学
図1.（a）本研究で前駆体として使用したRuターピリジル錯体。（b）ボトムアップ合成手法によりOCFが得られる様子。(c)得られたRu-OCFのHAADF-STEM像。
＜関連情報＞
- https://www.tohoku.ac.jp/japanese/2026/09/press20260907-01-ruthenium.html
- https://onlinelibrary.wiley.com/doi/10.1002/anie.6197340
ポリピリジル配位モチーフを前駆体とした、高密度ルテニウム単原子触媒に向けた秩序だった炭素骨格の構築 Polypyridyl Coordination Motifs as Precursors for Ordered Carbonaceous Frameworks Toward High-Density Ru Single-Atom Catalysts
Koki Chida, Tan-Hao Shi, Takeharu Yoshii, Yuichiro Hayasaka, Yu Gao, Hao Zhang, Nikolay Kosinov, Shigehisa Akine, Kazuhide Kamiya, Kaining Li, Yoshifumi Kondo, Yasutaka Kuwahara …
Angewandte Chemie International Edition Published: 03 September 2026
DOI:https://doi.org/10.1002/anie.6197340
ABSTRACT
Achieving high-density single-atom catalysts (SACs) remains a fundamental challenge, particularly for precious metals such as Ru that readily aggregate under synthetic and catalytic conditions. Here, we report a rational precursor design strategy for fabricating high-density Ru SACs via direct carbonization, yielding ordered carbonaceous frameworks (Ru-OCFs) with high Ru loadings of up to 11.0 wt%. By expanding the scope of precursors for OCF synthesis beyond conventional macrocyclic coordination motifs to coordinatively flexible polypyridyl ligands, we show that Ru-terpyridine crystals with thermally polymerizable ethynyl units serve as effective precursors for immobilizing single-atomic Ru species within three-dimensional porous carbon frameworks, without metal aggregation or post-synthetic treatments. The resulting Ru-OCFs retain the ordered structure and coordination environment of the precursor crystals while simultaneously developing microporosity with high specific surface areas of up to 670 m2 g−1. As a proof of concept, the high-density isolated Ru sites in Ru-OCFs enable enhanced catalytic activity in liquid-phase CO2 hydrogenation, achieving a high formic acid productivity of up to 19 mmol gcat−1 h−1, outperforming representative nanoparticle catalysts.
