Electrocatalytic, Kinetic, and Mechanism Insights into the Oxygen-Reduction Catalyzed Based on the Biomass-Derived FeO x @N-Doped Porous Carbon Composites

• Published in: Small (Weinheim an der Bergstrasse, Germany) Vol. 17; no. 19; p. e2007326
• Main Authors: Lu, Zhiwei, Chen, Jinpeng, Wang, WenLi, Li, Wenjin, Sun, Mengmeng, Wang, Yanying, Wang, Xianxiang, Ye, Jianshan, Rao, Hanbing
• Format: Journal Article
• Language: English
• Published: Germany 01.05.2021
• Subjects: Fe N co-doped; electrocatalysts; oxygen reduction reaction; biomass derivative; density function theory
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202007326

A valid strategy for amplifying the oxygen reduction reaction (ORR) efficiency of non-noble electrocatalyst in both alkaline and acid electrolytes by decorated with a layer of biomass derivative nitrogen-doped carbon (NPC) is proposed. Herein, a top-down strategy for the generally fabricating NPC matrix decorated with trace of metal oxides nanoparticles (FeO NPs) by a dual-template assisted high-temperature pyrolysis process is reported. A high-activity FeO /FeNC (namely Hemin/NPC-900) ORR electrocatalyst is prepared via simply carbonizing the admixture of Mg (OH) (CO ) and NaCl as dual-templates, melamine and acorn shells as nitrogen and carbon source, hemin as a natural iron and nitrogen source, respectively. Owing to its unique 3D porous construction, large BET areas (819.1 m ∙g ), and evenly dispersed active sites (FeN , CN, and FeO parts), the optimized Hemin/NPC-900 catalyst displays comparable ORR catalytic activities, remarkable survivability to methanol, and preferable long-term stability in both alkali and acid electrolyte compared with benchmark Pt/C. More importantly, density function theory computations certify that the interaction between Fe O nanoparticles and arm-GN (graphitic N at armchair edge) active sites can effectually promote ORR electrocatalytic performance by a lower overpotential of 0.81 eV. Accordingly, the research provides some insight into design of low-cost non-precious metal ORR catalysts in theory and practice.