过氧化氢
过渡金属
可逆氢电极
氢
化学
金属
密度泛函理论
氧气
碳纤维
无机化学
光化学
材料科学
催化作用
计算化学
物理化学
电化学
有机化学
工作电极
电极
复合材料
复合数
作者
Kun Jiang,Seoin Back,Austin Akey,Chuan Xia,Yongfeng Hu,Wentao Liang,Diane Schaak,Eli Stavitski,Jens K. Nørskov,Samira Siahrostami,Haotian Wang
标识
DOI:10.1038/s41467-019-11992-2
摘要
Shifting electrochemical oxygen reduction towards 2e- pathway to hydrogen peroxide (H2O2), instead of the traditional 4e- to water, becomes increasingly important as a green method for H2O2 generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H2O2 catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm-2 H2O2 current, and a high H2O2 selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e-/4e- ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e-, are responsible for the H2O2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.
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