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1.
Small ; 20(33): e2310637, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38593369

RESUMO

Constructing multiheteroatom coordination structure in carbonaceous substrates demonstrates an effective method to accelerate the oxygen reduction reaction (ORR) of supported single-atom catalyst. Herein, the novel etching route assisted by potassium thiocyanate (KCNS) is developed to convert metal-organic framework to 2D defect-rich porous N,S-co-doped carbon nanosheets for anchoring atomically dispersed iron sites as the high-performance ORR catalysts (Fe-SACs). The well-designed KCNS-assisted etching route can generate spatial confinement template to direct the carbon nanosheet formation, etching condition to form defect-rich structure, and additional sulfur atoms to coordinate iron species. Spectral and microscopy analysis reveals that the iron element in Fe-SACs is highly isolated on carbon nanosheet and anchored by nitrogen and sulfur atoms in unsymmetrical Fe-S1N3 structure. The optimized Fe-SACs with large specific surface area could show remarkable alkaline ORR performances with a high half-wave potential of 0.920 V versus RHE and excellent durability. The rechargeable zinc-air battery assembled with Fe-SACs air electrodes delivers a large power density of 350 mW cm-2 and a stable voltage platform during charge and discharge over more than 1300 h. This work proposes a novel strategy for the preparation of single-atom catalysts with multiheteroatom coordination structure and highly exposed active sites for efficient ORR.

2.
Small ; 19(28): e2301075, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-36978240

RESUMO

Defect chemistry in carbon matrix shows great potential for promoting the oxygen reduction reaction (ORR) of metal single-atom catalysts. Herein, a modified pyrolysis strategy is proposed to tune carbon defects in copper single-atom catalysts (Cu-SACs) to fully understand their positive effect on the ORR activity. The optimized Cu-SACs with controllable carbon defect degree and enhanced active specific surface area can exhibit improved ORR activity with a half-wave potential of 0.897 VRHE , ultrahigh limiting current density of 6.5 mA cm-2 , and superior turnover frequency of 2.23 e site-1 s-1 . The assembled Zn-air batteries based on Cu-SACs can also show well-retained reversibility and voltage platform over 1100 h charge/discharge period. Density functional theory calculations reveal that suitable carbon defects can redistribute charge density of Cu-N4 active sites to weaken the O-O bond in adsorbed OOH* intermediate and thus reduce its dissociation energy. This discovery offers a universal strategy for fabricating superior single-atom catalysts with high-efficiency active sites toward energy-directed applications.

3.
Appl Opt ; 62(8): 1984-1991, 2023 Mar 10.
Artigo em Inglês | MEDLINE | ID: mdl-37133084

RESUMO

A centimeter-sized bearing fault probe based on dual-fiber Bragg grating vibration sensing is proposed. The probe can provide multi-carrier heterodyne vibration measurements based on swept source optical coherence tomography technology and the synchrosqueezed wavelet transform method to obtain a wider vibration frequency response range and collect more accurate vibration data. For the sequential characteristics of bearing vibration signals, we propose a convolutional neural network with long short-term memory and transformer encoder. This method is proven in bearing fault classification under variable working conditions, and the accuracy rate reaches 99.65%.

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