Ultrathin Carbon Coating and Defect Engineering Promote RuO2 as an Efficient Catalyst for Acidic Oxygen Evolution Reaction with Super-High Durability,Advanced Energy Materials

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Ultrathin Carbon Coating and Defect Engineering Promote RuO2 as an Efficient Catalyst for Acidic Oxygen Evolution Reaction with Super-High Durability
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-04-22 , DOI: 10.1002/aenm.202300152
Haohao Yan ₁ , Zhongqing Jiang ₂ , Binglu Deng ₃ , Yongjie Wang ₄ , Zhong‐Jie Jiang ₁

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Developing acid-stable electrocatalysts with high activity for the oxygen evolution reaction (OER) is of paramount importance for many energy-related technologies. This work reports that ultrathin nitrogen-doped carbon coated oxygen-vacancy (Vo·) rich RuO₂ nanoparticles on carbon nanotubes (CNTs) (NC@Vo·-RuO₂/CNTs-350), synthesized through the controlled calcination in air, is an efficient acid-stable electrocatalyst for the OER. It only needs an overpotential of 170.0 mV to drive 10.0 mA cm⁻² and shows excellent stability with no distinguishable activity loss observed for >900 h. Its mass activity is >110 times higher than the commercial RuO₂. In particular, an electrolyzer assembled with this catalyst shows a record-low cell voltage of 1.45 V to deliver 10.0 mA cm⁻² and exhibits a low performance drop for >1000 h. The NC@Vo·-RuO₂/CNTs-350 also shows super-high catalytic activities and excellent stabilities for OER in neutral and alkaline media. DFT calculations indicate that its high catalytic activity mainly arises from the strong electronic coupling between RuO₂ and NC/CNTs, which increases the oxidation state and catalytic activity of Ru at the active site and improves the stabilities of lattice oxygen and surface Ru during the OER processes. The presence of Vo· can strengthen the electronic coupling between RuO₂ and NC/CNTs.

中文翻译：

超薄碳涂层和缺陷工程促进RuO2作为具有超高耐久性的酸性析氧反应的高效催化剂

为析氧反应 (OER) 开发具有高活性的酸稳定电催化剂对于许多能源相关技术而言至关重要。这项工作报道了在碳纳米管 (CNT) 上超薄氮掺杂碳包覆氧空位 (Vo·) 富 RuO ₂纳米粒子 (NC@Vo·-RuO ₂ /CNTs-350)，通过在空气中的受控煅烧合成，是一种高效的酸稳定 OER 电催化剂。它仅需要 170.0 mV 的过电势即可驱动 10.0 mA cm ^-2并显示出出色的稳定性，在 >900 小时内没有观察到明显的活性损失。其质量活性比商业 RuO _{2高 >110 倍}. 特别是，用这种催化剂组装的电解槽显示出创纪录的低电池电压 1.45 V 以提供 10.0 mA cm ^-2并且表现出低性能下降 >1000 小时。NC@Vo·-RuO ₂ /CNTs-350 在中性和碱性介质中也表现出超高的催化活性和优异的 OER 稳定性。DFT计算表明其高催化活性主要源于RuO ₂与NC/CNTs之间的强电子耦合，提高了Ru在活性位点的氧化态和催化活性，提高了OER过程中晶格氧和表面Ru的稳定性过程。Vo·的存在可以加强RuO ₂和NC/CNTs之间的电子耦合。

更新日期：2023-04-22

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