材料科学
电催化剂
电化学
催化作用
化学工程
质子交换膜燃料电池
碳纤维
纳米技术
无机化学
电极
复合数
物理化学
复合材料
化学
有机化学
工程类
作者
Jesús Barrio,Angus Pedersen,Saurav Ch. Sarma,Alexander Bagger,Mengjun Gong,Silvia Favero,Zhao Chang-xin,Ricardo García-Serres,Alain Li,Qiang Zhang,Frédéric Jaouen,Frédéric Maillard,Anthony Kucernak,Ifan E. L. Stephens,Maria‐Magdalena Titirici
标识
DOI:10.1002/adma.202211022
摘要
Atomic Fe in N-doped carbon (FeNC) electrocatalysts for oxygen (O2 ) reduction at the cathode of proton exchange membrane fuel cells are the most promising alternative to platinum-group-metal catalysts. Despite recent progress on atomic FeNC O2 reduction, their controlled synthesis and stability for practical applications remain challenging. A two-step synthesis approach has recently led to significant advances in terms of Fe-loading and mass activity; however, the Fe utilization remains low owing to the difficulty of building scaffolds with sufficient porosity that electrochemically exposes the active sites. Herein, this issue is addressed by coordinating Fe in a highly porous nitrogen-doped carbon support (≈3295 m2 g-1 ), prepared by pyrolysis of inexpensive 2,4,6-triaminopyrimidine and a Mg2+ salt active site template and porogen. Upon Fe coordination, a high electrochemical active site density of 2.54 × 1019 sites gFeNC-1 and a record 52% FeNx electrochemical utilization based on in situ nitrite stripping are achieved. The Fe single atoms are characterized pre- and post-electrochemical accelerated stress testing by aberration-corrected high-angle annular dark field scanning transmission electron microscopy, showing no Fe clustering. Moreover, ex situ X-ray absorption spectroscopy and low-temperature Mössbauer spectroscopy suggest the presence of penta-coordinated Fe sites, which are further studied by density functional theory calculations.
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