Deep Electronic State Regulation through Unidirectional Cascade Electron Transfer Induced by Dual Junction Boosting Electrocatalysis Performance.
Adv Sci (Weinh)
; 10(31): e2304063, 2023 Nov.
Article
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| MEDLINE
| ID: mdl-37712192
ABSTRACT
Unidirectional cascade electron transfer induced by multi-junctions is essential for deep electronic state regulation of the catalytic active sites, while this advanced concept has rarely been investigated in the field of electrocatalysis. In the present work, a dual junction heterostructure (FePc/L-R/CN) is designed by anchoring iron phthalocyanine (FePc)/MXene (L-Ti3 C2 -R, RâOH or F) heterojunction on g-C3 N4 nanosheet substrates for electrocatalysis. The unidirectional cascade electron transfer (g-C3 N4 â L-Ti3 C2 -R â FePc) induced by the dual junction of FePc/L-Ti3 C2 -R and L-Ti3 C2 -R/g-C3 N4 makes the Fe center electron-rich and therefore facilitates the adsorption of O2 in the oxygen reduction reaction (ORR). Moreover, the electron transfer between FePc and MXene is facilitated by the axial FeâO coordination interaction of Fe with the OH in alkalized MXene nanosheets (L-Ti3 C2 -OH). As a result, FePc/L-OH/CN exhibits an impressive ORR activity with a half-wave potential (E1/2 ) of 0.92 V, which is superior over the catalysts with a single junction and the state-of-the-art Pt/C (E1/2 = 0.85 V). This work provides a broad idea for deep regulation of electronic state by the unidirectional cascade multi-step charge transfer and can be extended to other proton-coupled electron transfer processes.
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01-internacional
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MEDLINE
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En
Revista:
Adv Sci (Weinh)
Año:
2023
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Article