Engineering p–d Orbital Coupling and Vacancy-Rich Structure in Triatomic Iron–Bismuth–Iron Sites for Rechargeable Zinc–Air Batteries DOI

Zhanhao Liang,

Wencai Liu,

Shaojie Jing

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

The rational design of heteroatomic sites with synergistic electronic modulation remains a critical challenge for achieving bifunctional oxygen electrocatalysis in sustainable energy technologies such as fuel cells and metal-air batteries. Herein, triatomic Fe2BiN5 configuration embedded nitrogen-doped carbon (Fe2BiN5/C) atomically dispersed FeN2-BiN-FeN2 vacancy-rich structures is synthesized via pyrolysis etching strategy. architecture endows Fe2BiN5/C exceptional activity, delivering high reduction reaction half-wave potential 0.918 V an evolution overpotential 245 mV at 10 mA cm-2, surpassing Pt/C RuO2. In situ X-ray absorption fine structure Raman spectroscopy reveal dynamic structural during electrocatalysis, where Fe acts the primary active center Bi regulating electron distribution long-range interactions, thereby optimizing adsorption/desorption energetics intermediates. theoretical calculations further elucidate that Bi-induced p-d orbital coupling leads to alteration d-orbitals level, downshift d-band center, weaken binding strength oxygen-based intermediates, reduced barrier electrocatalysis. This work provides understanding site p-block metal modulators transition-metal atoms toward enhanced catalysis.

Language: Английский

Engineering p–d Orbital Coupling and Vacancy-Rich Structure in Triatomic Iron–Bismuth–Iron Sites for Rechargeable Zinc–Air Batteries DOI

Zhanhao Liang,

Wencai Liu,

Shaojie Jing

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

The rational design of heteroatomic sites with synergistic electronic modulation remains a critical challenge for achieving bifunctional oxygen electrocatalysis in sustainable energy technologies such as fuel cells and metal-air batteries. Herein, triatomic Fe2BiN5 configuration embedded nitrogen-doped carbon (Fe2BiN5/C) atomically dispersed FeN2-BiN-FeN2 vacancy-rich structures is synthesized via pyrolysis etching strategy. architecture endows Fe2BiN5/C exceptional activity, delivering high reduction reaction half-wave potential 0.918 V an evolution overpotential 245 mV at 10 mA cm-2, surpassing Pt/C RuO2. In situ X-ray absorption fine structure Raman spectroscopy reveal dynamic structural during electrocatalysis, where Fe acts the primary active center Bi regulating electron distribution long-range interactions, thereby optimizing adsorption/desorption energetics intermediates. theoretical calculations further elucidate that Bi-induced p-d orbital coupling leads to alteration d-orbitals level, downshift d-band center, weaken binding strength oxygen-based intermediates, reduced barrier electrocatalysis. This work provides understanding site p-block metal modulators transition-metal atoms toward enhanced catalysis.

Language: Английский

Citations

0