P掺杂提高Fe–N–C催化剂中Fe–Nx活性基团的氧还原催化活性

Fe–N–C材料是一类有前景的非贵金属氧还原催化剂。为了在酸性介质中取代Pt/C催化剂，需要大幅度地改善其氧还原催化活性。

近日，香港科技大学邵敏华教授和华盛顿州立大学林跃河教授等人在Science China Materials上发表研究论文，提出一种通过P原子掺杂的方法来调节单原子Fe–N–C材料中Fe–N_x活性位点的活性。优化得到的材料在0.1 mol L⁻¹ HClO₄溶液中表现出优异的氧还原性能，其半波电位为0.858 V(比没有P掺杂的Fe–N–C材料高23 mV)。密度泛函理论计算表明，P掺杂能降低限制步骤的热力学过电位，从而提高其氧还原催化活性。

图1  FeN₄C, FeN₄CP1, and FeN₄CP3中 Fe–N₄位点的ORR过程：（a）计算模型；（b）自由能图。

该研究成果最近发表于Science China Materials, 2019, doi: 10.1007/s40843-019-1207-y。

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