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Title: Engineering efficient bifunctional electrocatalysts for rechargeable zinc–air batteries by confining Fe–Co–Ni nanoalloys in nitrogen-doped carbon nanotube@nanosheet frameworks

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/d0ta09580j· OSTI ID:1767949

Developing precious-metal-free bifunctional oxygen reduction and evolution reaction (ORR/OER) electrocatalysts is of great significance for several key energy conversion and storage systems, yet remains a formidable challenge. In this work, we systematically designed Fe–Co–Ni trimetallic nanoalloys encapsulated in nitrogen-doped carbon nanotube@nanosheet frameworks (FeCoNi-NC) for application as effective bifunctional ORR/OER electrocatalysts. The rational structural design of FeCoNi-NC provides hierarchical porosity coupled with greatly increased effective electrochemical specific area for exposing abundant active sites and enhanced mass-transfer capability toward the ORR/OER. Experimental observations and theoretical calculations confirmed that Fe–Co–Ni nanoalloys interacting with pyridinic nitrogen-rich carbon synergistically optimized the adsorption/desorption free energies of oxygen intermediates, thus significantly enhancing the intrinsic ORR/OER activity. Consequently, FeCoNi-NC exhibits remarkable bifunctionality for the ORR (half-wave potential of 0.89 V) and OER (1.54 V at 10 mA cm–2) with ΔE = 0.65 V, and even outperforms Pt/C–RuO2 benchmarks. Moreover, the corresponding zinc–air battery shows large power density (315.2 mW cm–2), high capacity (803.78 mA h g–1 at 100 mA cm–2) and excellent cycling durability (over 100 hours at 50 mA cm–2), further testifying its practical applications. This work demonstrates an effective pathway to highly active non-precious-metal bifunctional catalysts toward sustainable energy technologies.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Natural Science Foundation of Jiangxi Province; China Postdoctoral Science Foundation; National Postdoctoral Program for Innovative Talents
Grant/Contract Number:
AC02-76SF00515; 51763018; 21704038; 52073137; 51761135114; 20192BCB23001; 20202ZDB01009; 2018M632599; BX201700112
OSTI ID:
1767949
Journal Information:
Journal of Materials Chemistry. A, Vol. 8, Issue 48; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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