Deciphering Local Microstrain-Induced Optimization of Asymmetric Fe Single Atomic Sites for Efficient Oxygen Reduction DOI Creative Commons
Peng Zhang,

Siying Huang,

Kuo Chen

и другие.

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Май 26, 2025

Abstract Disrupting the symmetric electron distribution of porphyrin-like Fe single-atom catalysts has been considered as an effective way to harvest high intrinsic activity. Understanding catalytic performance governed by geometric microstrains is highly desirable for further optimization such efficient sites. Here, we decipher crucial role local microstrain in boosting activity and durability asymmetric (Fe–N 3 S 1 ) replacing one N atom with atom. The high-curvature hollow carbon nanosphere substrate introduces 1.3% compressive strain Fe–N bonds 1.5% tensile Fe–S bonds, downshifting d -band center accelerating kinetics *OH reduction. Consequently, curved sites anchored on (FeNS-HNS-20) exhibit negligible current loss, a half-wave potential 0.922 V vs. RHE turnover frequency 6.2 e −1 s site , which are 53 mV more positive 1.7 times that flat Fe–N–S counterpart, respectively. More importantly, multiple operando spectroscopies monitored dynamic strained into sites, mitigating overadsorption intermediates. This work not only sheds new light microstrain-induced enhancement, but also provides plausible direction optimizing via configurations.

Язык: Английский

Deciphering Local Microstrain-Induced Optimization of Asymmetric Fe Single Atomic Sites for Efficient Oxygen Reduction DOI Creative Commons
Peng Zhang,

Siying Huang,

Kuo Chen

и другие.

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Май 26, 2025

Abstract Disrupting the symmetric electron distribution of porphyrin-like Fe single-atom catalysts has been considered as an effective way to harvest high intrinsic activity. Understanding catalytic performance governed by geometric microstrains is highly desirable for further optimization such efficient sites. Here, we decipher crucial role local microstrain in boosting activity and durability asymmetric (Fe–N 3 S 1 ) replacing one N atom with atom. The high-curvature hollow carbon nanosphere substrate introduces 1.3% compressive strain Fe–N bonds 1.5% tensile Fe–S bonds, downshifting d -band center accelerating kinetics *OH reduction. Consequently, curved sites anchored on (FeNS-HNS-20) exhibit negligible current loss, a half-wave potential 0.922 V vs. RHE turnover frequency 6.2 e −1 s site , which are 53 mV more positive 1.7 times that flat Fe–N–S counterpart, respectively. More importantly, multiple operando spectroscopies monitored dynamic strained into sites, mitigating overadsorption intermediates. This work not only sheds new light microstrain-induced enhancement, but also provides plausible direction optimizing via configurations.

Язык: Английский

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