Atomically dispersed metal-nitrogen-carbon materials (AD-MNCs) are considered the most promising non-precious catalysts for the oxygen reduction reaction (ORR), but it remains a major challenge for simultaneously achieving high intrinsic activity, fast mass transport, and effective utilization of the active sites within a single catalyst. Here, an AD-MNCs consisting of defect-rich Fe-N₃ sites dispersed with axially coordinated Te atoms on porous carbon frameworks (Fe₁Te₁-900) is designed. The local charge densities and energy band structures of the neighboring Fe and Te atoms in FeN₃-Te are rearranged to facilitate the catalytic conversion of the O-intermediates. Meanwhile, the negative shift of the d-band center in FeN₃-Te reduces the energy barrier limit for effective desorption of the final OH^* intermediate. In the electrochemical evaluation, Fe₁Te₁-900 presents a more positive onset potential and half-wave potentials of 1.03 and 0.89 V versus the reversible hydrogen electrode, respectively. Furthermore, the liquid zinc-air batteries assembled with Fe₁Te₁-900 exhibited excellent performances compared to commercial Pt/C. This work opens up new ideas for the development of high-performance ORR electrocatalysts for applications in various energy conversion and storage technologies.

中文翻译：

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设计 Te 调制 Fe 单原子催化剂的局部原子环境以实现高效 O2 还原


原子分散的金属-氮-碳材料 （AD-MNCs） 被认为是氧还原反应 （ORR） 最有前途的非贵金属催化剂，但要在单个催化剂中同时实现高本征活性、快速质量传递和有效利用活性位点仍然是一个重大挑战。在这里，设计了一种由多孔碳框架 （Fe₁Te 1-900） 上与轴向配位 Te 原子分散的富含缺陷的 Fe-N₃ 位点组成的 AD-MNC。FeN_3-Te 中相邻 Fe 和 Te 原子的局部电荷密度和能带结构被重新排列，以促进 O 中间体的催化转化。同时，FeN_3-Te 中 d 带中心的负移降低了最终 ^OH* 中间体有效解吸的能垒极限。在电化学评估中，与可逆氢电极相比，Fe₁Te 1-900 分别具有 1.03 V 和 0.89 V 的正起始电位和半波电位。此外，与商用 Pt/C 相比，用 Fe₁Te 1-900 组装的液态锌空气电池表现出优异的性能。这项工作为开发用于各种能量转换和存储技术的高性能 ORR 电催化剂开辟了新思路。