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Water oxidation electrocatalysis using ruthenium coordination oligomers adsorbed on multiwalled carbon nanotubes
Nature Chemistry ( IF 21.8 ) Pub Date : 2020-09-28 , DOI: 10.1038/s41557-020-0548-7
Md Asmaul Hoque , Marcos Gil-Sepulcre , Adiran de Aguirre , Johannes A. A. W. Elemans , Dooshaye Moonshiram , Roc Matheu , Yuanyuan Shi , Jordi Benet-Buchholz , Xavier Sala , Marc Malfois , Eduardo Solano , Joohyun Lim , Alba Garzón-Manjón , Christina Scheu , Mario Lanza , Feliu Maseras , Carolina Gimbert-Suriñach , Antoni Llobet

Photoelectrochemical cells that utilize water as a source of electrons are one of the most attractive solutions for the replacement of fossil fuels by clean and sustainable solar fuels. To achieve this, heterogeneous water oxidation catalysis needs to be mastered and properly understood. The search continues for a catalyst that is stable at the surface of electro(photo)anodes and can efficiently perform this reaction at the desired neutral pH. Here, we show how oligomeric Ru complexes can be anchored on the surfaces of graphitic materials through CH–π interactions between the auxiliary ligands bonded to Ru and the hexagonal rings of the graphitic surfaces, providing control of their molecular coverage. These hybrid molecular materials behave as molecular electroanodes that catalyse water oxidation to dioxygen at pH 7 with high current densities. This strategy for the anchoring of molecular catalysts on graphitic surfaces can potentially be extended to other transition metals and other catalytic reactions.



中文翻译:

钌配位低聚物吸附在多壁碳纳米管上的水氧化电催化

利用水作为电子源的光电化学电池是用清洁,可持续的太阳能替代化石燃料的最有吸引力的解决方案之一。为此,需要掌握并正确理解多相水氧化催化。继续寻找在电(光)阳极表面稳定并且可以在所需的中性pH下有效地进行该反应的催化剂。在这里,我们展示了如何通过CH– π将低聚Ru络合物固定在石墨材料的表面上与Ru结合的辅助配体与石墨表面的六角环之间的相互作用,提供了对其分子覆盖率的控制。这些杂化分子材料表现为分子阳极,可在高电流密度下在pH 7时催化水氧化为双氧。这种将分子催化剂锚定在石墨表面上的策略可以潜在地扩展到其他过渡金属和其他催化反应。

更新日期:2020-10-19
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