摘要
Addressing the bottlenecks of catalytic efficiency and cost in clean energy conversion and electrochemical synthesis is critical for low-carbon technology advancement. Herein, we design an iron single atom supported on an inverse opal-structured carbon support (Fe-N-C io ), featuring unique hierarchical pores (micropores, mesopores, macropores) and an interlayer-confined microenvironment that synergistically enhances mass transfer and modulates the electronic structure of Fe-N 4 active sites. We demonstrate that the confined microenvironment in bilayer graphene downshifts the Fe d -band center, weakening the binding strength of oxygen intermediates, favoring O–O bond cleavage and reducing the rate-determining step energy barrier (O* → OH*). Consequently, Fe-N-C io outperforms commercial Pt/C, achieving a half-wave potential ( E 1 / 2 ) of 0.91 V with only 7.87 mV decay after 100,000 cycles. In practical device applications, the aqueous zinc-air batteries (A-ZABs) assembled with Fe-N-C io achieve stable operation for over 1200 h, with a voltage gap change of only 20 mV. The quasi-solid-state zinc-air batteries (QSS-ZABs) exhibit an OCV of 1.48 V, a large peak power density of up to 207.73 mW cm −2 , and also cycling durability for 160 h. In chlor-alkali electrolysis systems, the Fe-N-C io ||RuO 2 chlor-alkali flow cell operates at 1.66 V (80 °C, 300 mA cm −2 ) with stable performance for over 110 h. This work validates the application potential of Fe-N-C io in energy conversion and industrial electrochemistry, while systematically elucidating the regulatory mechanism of the interlayer-constrained microenvironment on single-atom catalyst’s performance, which provides a paradigm for designing high-efficiency non-precious metal catalysts. Interlayer-confined Fe-N 4 sites optimize electronic modulation, and the hierarchical porous carbon accelerates mass transport, thus enhancing the oxygen reduction reaction. Download: Download high-res image (351KB) Download: Download full-size image
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