Journal
ENERGY STORAGE MATERIALS
Volume 42, Issue -, Pages 118-128Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2021.07.027
Keywords
Iminodiacetonitrile; Organometallic coordination polymer; PdNi/Ni@carbon nanosheets; Bifunctional electrocatalyst; Rechargeable Zn-Air batteries
Funding
- National Natural Science Foundation of China [22072067, 21875112]
- National and Local Joint Engineering Research Center of Biomedical Functional Materials
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Postgraduate Research & Practice Innovation Program of Jiangsu Province [KYCX21_1326]
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By utilizing the molecular structure of IDAN, a novel PdNi/Ni@N-C bifunctional electrocatalyst was developed, showing outstanding performance in ORR and OER, out-performing commercial benchmarks.
Developing highly-active, stable and conducive 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 dsp(2) hybridization, while the amino ligands tend to form a high spin tetrahedral complex with M2+ by sp(3) 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.
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