Tuci Giulia, Rossin Andrea, Zhang Xiong, Truong-Phuoc Lai, Berretti Enrico, Liu Yuefeng, Pham-Huu Cuong, Ali Sajjad, Jan Faheem, Poggini Lorenzo, Giambastiani Giuliano
Institute of Chemistry of OrganoMetallic Compounds, ICCOM-CNR and Consorzio INSTM, Via Madonna del Piano, 10, 50019, Sesto F.no, Florence, Italy.
Institute of Chemistry and Processes for Energy, Environment and Health (ICPEES), ECPM, UMR 7515, CNRS-University of Strasbourg, 25 rue Becquerel, 67087, Strasbourg Cedex 02, France.
Chemistry. 2023 Jul 26;29(42):e202301036. doi: 10.1002/chem.202301036. Epub 2023 Jun 16.
Hydrogen peroxide (H O ) electrosynthesis via the 2e Oxygen Reduction Reaction (ORR) represents a highly challenging, environmentally friendly and cost-effective alternative to the current anthraquinone-based technology. Various lightweight element hetero-doped carbon nanostructures are promising and cheap metal-free electrocatalysts for H O synthesis, particularly those containing O-functionalities. The exact role of O-containing functional groups as electroactive sites for the process remains debated if not highly controversial. Herein, we have reported on the covalent exohedral functionalization of the outer surface of extra-pure multi-walled carbon nanotubes (MWCNTs) with discrete O-functional groups as a unique approach to prepare selective electrocatalysts for the process. This kind of decoration has added fundamental tiles to the puzzling structure/reactivity relationship of O-containing carbon-based catalysts for ORR, clearing doubts on the controversial role of hydroxyl/phenol groups as key functionalities for the design of more performing 2e ORR electrocatalysts.
通过2e氧还原反应（ORR）进行过氧化氢（H₂O₂）的电合成是一种极具挑战性、环境友好且具有成本效益的替代当前蒽醌基技术的方法。各种轻质元素杂化的碳纳米结构是用于H₂O₂合成的有前景且廉价的无金属电催化剂，特别是那些含有O-官能团的结构。含O官能团作为该过程的电活性位点的确切作用即使没有高度争议，也仍存在争议。在此，我们报道了用离散的O-官能团对超纯多壁碳纳米管（MWCNT）外表面进行共价外表面功能化，这是一种制备该过程选择性电催化剂的独特方法。这种修饰为含O碳基ORR催化剂令人困惑的结构/反应性关系增添了基本要素，消除了关于羟基/酚基作为设计性能更优的2e ORR电催化剂的关键官能团的争议性作用的疑虑。
