催化作用
电化学
氟
碳纤维
氧气
旋转圆盘电极
兴奋剂
化学
动力学
电化学能量转换
电极
化学工程
材料科学
无机化学
物理化学
有机化学
光电子学
物理
量子力学
复合数
工程类
复合材料
循环伏安法
作者
Jinhui Liang,Lecheng Liang,Binwen Zeng,Binbin Feng,Li Du,Xiaoyi Qiu,Yian Wang,Huiyu Song,Shijun Liao,Minhua Shao,Zhiming Cui
标识
DOI:10.1002/anie.202412825
摘要
It is well‐established that Pt‐based catalysts suffer from the unfavorable linear scaling relationship (LSR) between *OOH and *OH (ΔG(*OOH) = ΔG(*OH) + 3.2 ± 0.2 eV) for the oxygen reduction reaction (ORR), resulting in a great challenge to significantly reduced ORR overpotentials. Herein, we propose a universal and feasible strategy of fluorine‐doped carbon supports, which optimize interfacial microenvironment of Pt‐based catalysts and thus significantly enhance their reactive kinetics. The introduction of C‐F bonds not only weakens the *OH binding energy, but also stabilizes the *OOH intermediate, resulting in a break of LSR. Furthermore, fluorine‐doped carbon constructs a local super‐hydrophobic interface that facilitates the diffusion of H2O and the mass transfer of O2. Electrochemical tests show that the F‐doped carbon‐supported Pt catalysts exhibit over 2‐fold higher mass activities than those without F modification. More importantly, those catalysts also demonstrate excellent stability in both rotating disk electrode (RDE) and membrane electrode assembly (MEA) tests. This study not only validates the feasibility of tuning the electrocatalytic microenvironment to improve mass transport and to break the scaling relationship, but also provides a universal catalyst design paradigm for other gas‐involving electrocatalytic reactions.
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