An active site pre-anchoring and post-exposure strategy in Fe(CN)64-@PPy derived Fe/S/N-doped carbon electrocatalyst for high performance oxygen reduction reaction and zinc-air batteries

电催化剂 催化作用 聚合 材料科学 色散(光学) 化学工程 无机化学 化学 电化学 聚合物 有机化学 电极 物理化学 复合材料 冶金 光学 物理 工程类
作者
Zuoxu Xiao,Yanling Wu,Shoufu Cao,Wei Yan,Baotong Chen,Tao Xing,Zhi Li,Xiaoqing Lü,Yanli Chen,Kang Wang,Jianzhuang Jiang
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:413: 127395-127395 被引量:45
标识
DOI:10.1016/j.cej.2020.127395
摘要

A novel “active site pre-anchoring and post-exposure” strategy is developed for the synthesis of highly active Fe/3S/N-C ORR electrocatalyst. In the synthesis of Fe/3S/N-C, the Fe(CN)64-@PPy precursors with highly dispersion of Fe active species were initially created by pre-anchoring Fe(CN)64- into polypyrrole (PPy) matrixes through electrostatic interactions depending on the cation radicals generated on the PPy chains during pyrrole monomer polymerization. The Fe(CN)64-@PPy then suffered pyrolysis treatment in the presence of sublimed sulfur activator that ensures a larger specific area and thus effective exposure of Fe and N active sites in Fe/3S/N-C. Depending on highly efficient dispersion of Fe3C and Fe-Nx active species, the resultant Fe/3S/N-C electrocatalyst displays 20 mV higher onset potential (0.99 V) and 50 mV higher half-wave potential (0.89 V) than those of a commercial Pt/C catalyst in an alkaline medium. This, combined with high current density (–5.71 mA cm−2) and excellent durability (larger than 95% retention after 20000 s), are one of the best performance among non-precious metal ORR electrocatalysts reported thus far. In addition, Fe/3S/N-C employed as the cathode material for zinc-air battery, shows excellent durability and superior peak power density to Pt/C. A series of control experiments combined with DFT theoretical analysis demonstrated that the Fe3C nanoparticles boost the activity of Fe-Nx species in Fe/3S/N-C, meanwhile the coexistence of Fe3C and Fe-Nx active species increased the HOMO energy level and O2 adsorption energy of the catalyst. These result in improved ORR performance.
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