Journal of Colloid and Interface Science ( IF 9.9 ) Pub Date : 2020-08-29 , DOI: 10.1016/j.jcis.2020.08.103 Zhe Chen 1 , Dengyu Zhao 1 , Cong Chen 1 , Yuan Xu 1 , Congli Sun 2 , Kangning Zhao 1 , Muhammad Arif Khan 3 , Daixin Ye 1 , Hongbin Zhao 1 , Jianhui Fang 1 , Xueliang Andy Sun 4 , Jiujun Zhang 1
Constructing of single atom catalysts that can stably exist in various energy conversion and storage devices is still in its infancy. Herein, a geometrically optimized three-dimensional hierarchically architectural single atomic FeNC catalyst with fast mass transport and electron transfer is rationally developed by post-molecule pyrolysis assisted with silicon template and reconstructs by ammonia treating. The ammonia-assisted secondary pyrolysis not only compensates for the volatilization of nitrogen species contained in organic precursors but also optimizes the surface structure of FeNC catalyst, thus increasing the content of pyridinic nitrogen and boosting the density of active sites (FeNx) in FeNC samples. In addition, the pyridinic nitrogen adjusts the electronic distribution in Fe 3d active center and promotes the catalytic performances. Therefore, this hollow spherical atomically dispersed FeNC catalyst delivers outstanding oxygen reduction reaction (ORR) activity in pH-universal electrolyte and surpasses the most reported values.
中文翻译:
pH通用原子FeNC催化剂的重建,用于氧还原反应。
稳定地存在于各种能量转换和存储装置中的单原子催化剂的构建仍处于起步阶段。本文通过硅模板辅助分子后热解,合理合成了具有快速传质和电子传递的几何优化的三维层次结构单原子Fe N C催化剂,并通过氨处理进行了重构。氨辅助的二次热解不仅可以补偿有机前体中所含氮的挥发,而且可以优化Fe N C催化剂的表面结构,从而增加吡啶二氮的含量并提高活性位(Fe N x)的密度。在Fe N中C样本。此外,吡啶二氮可调节Fe 3 d活性中心的电子分布并提高催化性能。因此,这种中空球形原子分散的Fe N C催化剂在pH通用型电解质中具有出色的氧还原反应(ORR)活性,并超过了大多数报道的值。