Suppressing the Pt dissolution still remains a big challenge in improving the long-term stability of Pt-based catalysts in electrochemical energy conversion. In this work, the degradation of Pt nanoparticles is successfully suppressed via weakening the Pt–O dipole effect by adjusting the electronic structure of surface Pt atoms. The specially designed graphitic-N-doped carbon nanosheets with balanced N content and graphitization degree as well as fewer defects are prepared for anchoring Pt nanoparticles to enhance the electronic metal–support interaction. This can accelerate the electron transfer from Pt to substrate, decrease the surface electron density of Pt, and attenuate the Pt–O interaction. As a result, the rate of Pt dissolution decreases by 95% compared to that of commercial Pt/C toward the oxygen reduction reaction and thus the catalytic stability is significantly improved in the electrochemical accelerated durability test. The theoretical simulation shows that the inhibition of surface Pt dissolution is attributed to the enhanced energy barrier in the initial relaxation process.

中文翻译：

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通过电子金属-载体相互作用抑制 Pt 基电催化剂的溶解

抑制 Pt 溶解仍然是提高 Pt 基催化剂在电化学能量转换中的长期稳定性的一大挑战。在这项工作中，通过调整表面 Pt 原子的电子结构来减弱 Pt-O 偶极效应，成功地抑制了 Pt 纳米粒子的降解。特别设计的石墨-N掺杂碳纳米片具有平衡的N含量和石墨化程度以及较少的缺陷，用于锚定Pt纳米颗粒以增强电子金属-载体相互作用。这可以加速电子从 Pt 到衬底的转移，降低 Pt 的表面电子密度，并减弱 Pt-O 相互作用。其结果，与商用 Pt/C 相比，Pt 的溶解速率降低了 95%，用于氧还原反应，因此在电化学加速耐久性试验中催化稳定性显着提高。理论模拟表明，表面 Pt 溶解的抑制归因于初始弛豫过程中增强的能垒。