Iminodiacetonitrile induce-synthesis of two-dimensional PdNi/Ni@carbon nanosheets with uniform dispersion and strong interface bonding as an effective bifunctional eletrocatalyst in air-cathode

Zhijuan Li, Hao Li, Meng Li, Jinrui Hu, Yuanyuan Liu, Dongmei Sun, Gengtao Fu*, Yawen Tang

*Corresponding author for this work

Research output: Contribution to journalJournal articlepeer-review

Abstract

Developing highly-active, stable and conductive bifunctional electrocatalysts towards both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is a key step for rechargeable Zn-air batteries. From unique molecular structure of iminodiacetonitrile (IDAN), herein we design and build a novel organometallic coordination polymer (OCP) for the synthesis of hierarchical N-doped carbon nanosheets anchored PdNi/Ni hybrids (PdNi/Ni@N-C). The cyano ligands in IDAN can form a low spin planar tetragonal complex with M2+ (M=Pd and Ni) by dsp2 hybridization, while the amino ligands tend to form a high spin tetrahedral complex with M2+ by sp3 hybridization, which not only induce the formation of 2D carbon nanosheets, but also strengthen metal-carbon interaction after the pyrolysis. The optimized PdNi/Ni@N-C can function as an outstanding bifunctional electrocatalyst, presenting a positive half-wave potential of 0.89 V towards ORR and a low overpotential of 360 mV at 10 mA cm−2 towards OER, out-performing commercial precious-metal benchmarks. Theoretical calculations are performed to analyze the alloying effects of PdNi and identify the potential active sites for ORR/OER. Furthermore, the PdNi/Ni@N-C as an air-cathode can enable rechargeable liquid and flexible all-solid-state Zn–air batteries to achieve higher power density and longer cycle life than costly Pd/C+RuO2-driven batteries. This work offers a potential molecular design strategy for the development of efficient electrocatalysts for energy storage and conversion.

Original languageEnglish
JournalEnergy Storage Materials
Volume42
Pages (from-to)118-128
ISSN2405-8297
DOIs
Publication statusPublished - 2021

Keywords

  • Bifunctional electrocatalyst
  • Iminodiacetonitrile
  • Organometallic coordination polymer
  • PdNi/Ni@carbon nanosheets
  • Rechargeable Zn-Air batteries

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