Cascaded orbital-oriented hybridization of intermetallic Pd3Pb boosts electrocatalysis of Li-O2 battery

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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Author(s)

  • Yin Zhou
  • Kun Yin
  • Lu Tao
  • Yiju Li
  • Hao Tan
  • Yong Yang
  • Shaojun Guo

Detail(s)

Original languageEnglish
Article numbere2301439120
Journal / PublicationProceedings of the National Academy of Sciences of the United States of America
Volume120
Issue number25
Online published12 Jun 2023
Publication statusPublished - 20 Jun 2023

Link(s)

Abstract

Catalysts with a refined electronic structure are highly desirable for promoting the oxygen evolution reaction (OER) kinetics and reduce the charge overpotentials for lithium-oxygen (Li-O2) batteries. However, bridging the orbital interactions inside the catalyst with external orbital coupling between catalysts and intermediates for reinforcing OER catalytic activities remains a grand challenge. Herein, we report a cascaded orbital-oriented hybridization, namely alloying hybridization in intermetallic Pd3Pb followed by intermolecular orbital hybridization between low-energy Pd atom and reaction intermediates, for greatly enhancing the OER electrocatalytic activity in Li-O2 battery. The oriented orbital hybridization in two axes between Pb and Pd first lowers the d band energy level of Pd atoms in the intermetallic Pd3Pb; during the charging process, the low-lying 4dxz/yz and 4dz2 orbital of the Pd further hybridizes with 2π* and 5σ orbitals of lithium superoxide (LiO2) (key reaction intermediate), eventually leading to lower energy levels of antibonding and, thus, weakened orbital interaction toward LiO2. As a consequence, the cascaded orbital-oriented hybridization in intermetallic Pd3Pb considerably decreases the activation energy and accelerates the OER kinetics. The Pd3Pb-based Li-O2 batteries exhibit a low OER overpotential of 0.45 V and superior cycle stability of 175 cycles at a fixed capacity of 1,000 mAh g-1, which is among the best in the reported catalysts. The present work opens up a way for designing sophisticated Li-O2 batteries at the orbital level. © 2023 the Author(s). Published by PNAS.

Research Area(s)

  • energy barrier, intermetallic, lithium–oxygen batteries, orbital hybridization

Citation Format(s)

Cascaded orbital-oriented hybridization of intermetallic Pd3Pb boosts electrocatalysis of Li-O2 battery. / Zhou, Yin; Gu, Qianfeng; Yin, Kun et al.
In: Proceedings of the National Academy of Sciences of the United States of America, Vol. 120, No. 25, e2301439120, 20.06.2023.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

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