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Author Spotlight: Unlocking the World of Intrinsically Disordered Regions with Cellular Sensing and Responses
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Structural-Insensitive Descriptors Ns,p Based on M-N4-OH Active Entity for Predicting and Enhancing ORR Activity in

Huan Li1, Liyuan Yang1, Wanying Wang1,2

  • 1College of Electronic Information and Optical Engineering, Nankai University, Tianjin, 300350, China.

Small (Weinheim an Der Bergstrasse, Germany)
|April 24, 2025
PubMed
Summary

Researchers explored how s- and p-orbitals impact oxygen reduction reaction (ORR) catalysts. They found these orbitals, not d-orbitals, show a volcano relationship, guiding the design of better ORR catalysts.

Keywords:
DFT calculationsoxygen reduction reactionpyramidal coordination entitys‐ and p‐orbitalstransition metal catalysts

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • Developing high-performance oxygen reduction reaction (ORR) catalysts is crucial for energy technologies.
  • Understanding the electronic structure's role in ORR catalysis, particularly the influence of s- and p-orbitals, remains a challenge.

Purpose of the Study:

  • To investigate the role of delocalized s- and p-orbital electrons in ORR activity using a from active unit to bulk catalyst (FAUC) design strategy.
  • To establish a descriptor for predicting ORR catalyst performance based on s- and p-orbital contributions.

Main Methods:

  • Density functional theory (DFT) calculations were performed on six M-N4-OH (M = V, Cr, Mn, Fe, Co, Ni) catalyst systems.
  • Analysis focused on the relationship between s- and p-orbital electron delocalization (Ns,p) and ORR activity.
  • Structure-activity relationships were explored by modifying M-O and M-N bond lengths.

Main Results:

  • Delocalized electrons in s- and p-orbitals (Ns,p) exhibit a significant volcano relationship with ORR activity, outperforming d-orbitals in predictive capability.
  • Shorter M-O and M-N bond lengths were found to increase Ns,p, enhancing ORR performance.
  • Modification of Co-N4-OH-C catalysts by doping and loading shortened Co-N bonds, increasing Ns,p and improving ORR activity.

Conclusions:

  • The Ns,p descriptor is rational and universally applicable across various 3d transition metals for predicting ORR catalyst performance.
  • This study provides novel insights for designing high-performance ORR catalysts by focusing on s- and p-orbital contributions.