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Bidirectional modulation interaction between monatomic Pt and Tin+ sites on Ti4O7 for high-efficiency and durable oxygen reduction
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-05-20 , DOI: 10.1016/j.jcat.2022.05.008
Yangjun Luo , Yanwei Wang , Xuetao Qin , Youyuan Wang , Kai Wu , Huijuan Zhang , Li Zhang , Heming Huang , Wu Tian , Yu Wang

Although single atom catalyst (SAC) can maximize the atomic utilization, platinum (Pt)-based SAC is typically inactive to break the O = O bond in oxygen reduction. Herein, the nanoporous Ti4O7 was synthesized while Pt was atomically dispersed on the Ti4O7 surface by a one-step calcination method. The as-prepared Pt/Ti4O7 SAC exhibits a half-wave potential of 0.896 V and a mass activity of 4081.5 A/gPt at 0.9 V with negligible degradation after 20,000 cycles. Meanwhile, it exhibits a Pt utilization efficiency of 0.16 gPt kW−1 in H2/O2 fuel cell and a slight attenuation of the output current density (9.4%) after 120 h. The incorporated monatomic Pt electronically couples with the Tin+ (3 ≤ n < 4) to enhance bilateral electron transfer. The awakened Tin+ active sites synergize with monatomic Pt to moderate the adsorption intensity of O2 and dissociate the O = O bond, opening up a four-electron pathway on the Pt-based SAC.



中文翻译:

Ti4O7 上单原子 Pt 和 Tin+ 位点之间的双向调制相互作用,实现高效持久的氧还原

尽管单原子催化剂 (SAC) 可以最大限度地提高原子利用率,但基于铂 (Pt) 的 SAC 通常不会在氧还原中破坏 O = O 键。在此,通过一步煅烧法合成纳米多孔Ti 4 O 7,同时将Pt原子分散在Ti 4 O 7表面上。所制备的 Pt/Ti 4 O 7 SAC 在 0.9 V 下表现出 0.896 V 的半波电位和 4081.5 A/g Pt的质量活度,在 20,000 次循环后降解可忽略不计。同时,其Pt利用效率为0.16 g Pt kW -1 in H 2 /O 2燃料电池和 120 小时后输出电流密度略有衰减(9.4%)。掺入的单原子 Pt 与 Ti n+ (3 ≤ n < 4) 电子耦合以增强双边电子转移。唤醒的 Ti n+活性位点与单原子 Pt 协同作用以缓和 O 2的吸附强度并解离 O = O 键,从而在 Pt 基 SAC 上开辟一条四电子通路。

更新日期:2022-05-20
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