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Enhanced oxygen reduction performance of nitrogen and sulfur Co-doped graphene oxide by immobilized ionic liquid
Chemical Engineering Science ( IF 4.1 ) Pub Date : 2021-02-23 , DOI: 10.1016/j.ces.2021.116544
Wenlin Zhang , Yongkang Zhang , Yandong Li , Shuangcheng Yang , Lu-Hua Zhang , Fengshou Yu

The development of robust metal-free catalysts for electrochemical oxygen reduction reaction (ORR) is a great challenge due to the large energy barriers for the intermediate *OO formation. In this work, an ionic liquid (IL) modified N/S co-doped graphene oxide (IL-SNG) was synthesized and explored as a metal-free ORR catalyst in alkaline conditions. Compared to the electrode without IL modification (SNG), the onset and half-wave potentials of IL-SNG were positively shifted by 130 and 110 mV, respectively. The IL and co-doping effects enable IL-SNG a comparable activity to that of Pt/C catalyst in alkaline solution. In addition to impressive activity, IL-SNG exhibits a superior tolerance to methanol and excellent long-term stability over Pt/C under the identical conditions, enabling it a potential candidate for ORR in alkaline conditions. DFT calculation shows that IL enhances O2 adsorption and stabilizes the high-energy *OO intermediate by forming ion pairs and therefore boosts the catalytic activity.



中文翻译:

固定化离子液体提高氮和硫共掺杂氧化石墨烯的氧还原性能

由于中间体* OO-具有较大的能垒,因此开发用于电化学氧还原反应(ORR)的耐用的无金属催化剂是一项巨大的挑战编队。在这项工作中,合成了一种离子液体(IL)改性的N / S共掺杂氧化石墨烯(IL-SNG),并在碱性条件下用作无金属的ORR催化剂。与没有IL修饰(SNG)的电极相比,IL-SNG的起始和半波电势分别正向偏移130和110 mV。IL和共掺杂效应使IL-SNG具有与碱性溶液中Pt / C催化剂相当的活性。除了令人印象深刻的活性外,IL-SNG在相同条件下还具有优于Pt / C的甲醇耐受性和出色的长期稳定性,使其成为碱性条件下ORR的潜在候选者。DFT计算表明IL增强Ò 2吸附并稳定高能* OO - 通过形成离子对形成中间体,因此提高了催化活性。

更新日期:2021-03-04
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