Institute of Medical Support Technology , Academy of Military Science of Chinese PLA , Tianjin 300161 , China.
State Key Laboratory of Powder Metallurgy & Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering , Central South University , Changsha 410083 , China.
ACS Appl Mater Interfaces. 2018 Oct 24;10(42):35888-35895. doi: 10.1021/acsami.8b09197. Epub 2018 Oct 12.
It is a challenge to synthesize highly efficient nonprecious metal electrocatalysts with a well-defined nanostructure and rich active species. Herein, through electron engineering and structure manipulation simultaneously, we constructed Fe-embedded pyridinic-N-dominated carbon nanotubes (CNTs) on ordered mesoporous carbon, showing excellent oxygen reduction reaction activity (half-wave potential, 0.85 V) and an overpotential of 420 mV to achieve 10 mA cm for oxygen evolution reaction in alkaline media (potential difference, 0.80 V). Density functional theory calculation indicates those Fe@N clusters improve charge transfer and further promote the electrocatalytic reactivity of the functionalized region in CNTs. Rechargeable Zn-air batteries were assembled, displaying robust charging-discharging cycling performance (over 90 h) with voltage gap of only 0.08 V, much lower than that of the Pt/C + Ir/C electrode (0.29 V). This work presents a highly active nonprecious metal-based bifunctional catalyst toward air electrode for energy conversion.
合成具有明确纳米结构和丰富活性物种的高效非贵金属电催化剂是一项挑战。在此，我们通过电子工程和结构操纵的协同作用，在有序介孔碳上构建了 Fe 嵌入的吡啶-N 为主的碳纳米管（CNTs），在碱性介质中表现出优异的氧还原反应活性（半波电位为 0.85 V）和 420 mV 的过电势即可实现 10 mA cm 的析氧反应（电位差为 0.80 V）。密度泛函理论计算表明，这些 Fe@N 簇提高了电荷转移，并进一步促进了 CNTs 中功能化区域的电催化反应性。组装了可充电的锌空气电池，具有稳健的充放电循环性能（超过 90 h），电压差仅为 0.08 V，远低于 Pt/C + Ir/C 电极（0.29 V）。这项工作提出了一种高效的基于非贵金属的双功能空气电极催化剂，用于能量转换。
