材料科学
无定形固体
电催化剂
掺杂剂
化学工程
催化作用
纳米材料
钝化
溶解
纳米技术
兴奋剂
物理化学
结晶学
有机化学
光电子学
电化学
化学
图层(电子)
电极
工程类
作者
Zixi Lyu,Junlin Cai,Xia‐Guang Zhang,Huiqi Li,Huiping Huang,Shupeng Wang,Tianyu Li,Qiuxiang Wang,Zhaoxiong Xie,Shuifen Xie
标识
DOI:10.1002/adma.202314252
摘要
Abstract The activity‐stability trade‐off relationship of oxygen reduction reaction (ORR) is a tricky issue that strikes the electrocatalyst population and hinders the widespread application of fuel cells. Here neoteric biphase Pd nanosheets that are structured with ultrathin two‐dimensional crystalline Pd inner cores and ≈1 nm thin atomic‐hybrid RhO x /Pd amorphous skins, named c/a‐Pd@PdRh NSs, for disentangling this trade‐off dilemma for alkaline ORR are developed. The superthin amorphous skins significantly amplify the quantity of flexibly low‐coordinated atoms for electrocatalysis. An in situ selected oxidation of the top‐surface Rh dopants creates atomically hybrid RhO x /Pd disorder surfaces. Detailed energy spectra and theoretical simulation confirm that these RhO x /Pd interfaces can arouse a surface charge redistribution, causing significant electron deficiency and lowered d ‐band center for surface Pd. Meanwhile, anticorrosive Rh/RhO x species can thermodynamically passivate the neighboring Pd atoms from oxidative dissolution. Thanks to these amplified interfacial effects, the biphase c/a‐Pd@PdRh NSs simultaneously exhibit a superhigh ORR activity (5.92 A mg −1 , 22.8 times that of Pt/C) and an outstanding long‐lasting stability after 100k cycles of accelerated durability test, showcasing unprecedented electrocatalysts for breaking the activity‐stability trade‐off relationship of ORR. This work paves a bran‐new strategy for designing high‐performance electrocatalysts through creating modulated amorphous skins on low‐dimensional nanomaterials.
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