电催化剂
催化作用
化学
可逆氢电极
碳纤维
扫描透射电子显微镜
密度泛函理论
电化学
光化学
选择性
无机化学
材料科学
电极
纳米技术
物理化学
透射电子显微镜
计算化学
工作电极
有机化学
复合数
复合材料
作者
Nan Wang,Xunhua Zhao,Rui Zhang,Saerom Yu,Zachary Levell,Chunyang Wang,Shengqian Ma,Peichao Zou,Lili Han,J. Qin,Lu Ma,Yuanyue Liu,Huolin L. Xin
标识
DOI:10.1021/acscatal.1c05633
摘要
Selective electrochemical two-electron oxygen reduction is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. Herein, we report a high-performance nitrogen-coordinated single-atom Pd electrocatalyst, which is derived from Pd-doped zeolitic imidazolate frameworks (ZIFs) through one-step thermolysis. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with X-ray absorption spectroscopy verifies atomically dispersed Pd atoms on nitrogen-doped carbon (Pd-NC). The single-atom Pd-NC catalyst exhibits excellent electrocatalytic performance for two-electron oxygen reduction to H2O2, which shows ∼95% selectivity toward H2O2 and an unprecedented onset potential of ∼0.8 V versus revisable hydrogen electrode (RHE) in 0.1 M KOH. Density functional theory (DFT) calculations demonstrate that the Pd-N4 catalytic sites thermodynamically prefer *–O bond breaking to O–O bond breaking, corresponding to a high selectivity for H2O2 production. This work provides a deep insight into the understanding of the catalytic process and design of high-performance 2e– ORR catalysts.
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