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Regulating single-atom Mn sites by precisely axial pyridinic-nitrogen coordination to stabilize the oxygen reduction
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2023-02-13 , DOI: 10.1016/j.jechem.2023.01.048
Yuan Qin , Chaozhong Guo , Zihao Ou , Chuanlan Xu , Qi Lan , Rong Jin , Yao Liu , Yingchun Niu , Quan Xu , Yujun Si , Honglin Li

Designing single-atom catalysts for oxygen reduction reaction (ORR) are fashionable but challenging to boost the zinc-air battery performance. Significantly enhanced ORR activity by manganese (Mn) single-atom catalysts can be achieved by accurately regulating the coordination number of isolated Mn atoms. Theoretical calculations indicate that the single Mn-N5 sites possess lower free energy barrier and higher oxygen adsorption performance than single Mn-N4 sites to accelerate the ORR kinetics. Target to it, here we synthesize an atomically dispersed Mn-N5 catalyst by precisely axial coordination of pyridinic-N doped into two-dimensional (2D) porous nanocarbon sheets (∼3.56 nm thickness), which reveals outstanding catalytic activity and ultrahigh stability for the ORR in zinc-air battery owing to the inhomogeneous charge distribution of Mn-N5 sites compared to the conventional single-site Mn-N4 catalyst and Pt/C. This work gives a new strategy for in situ regulating the electronic structure of metal single-atoms and further promoting the overall ORR performance in energy systems.



中文翻译:

通过精确轴向吡啶-氮配位调节单原子 Mn 位置以稳定氧还原

设计用于氧还原反应 (ORR) 的单原子催化剂很流行,但要提高锌空气电池的性能却具有挑战性。通过精确调节孤立的 Mn 原子的配位数,可以显着提高锰 (Mn) 单原子催化剂的 ORR 活性。理论计算表明,与单个Mn-N 4位点相比,单个Mn-N 5位点具有更低的自由能垒和更高的氧吸附性能,从而加速了ORR动力学。针对它,这里我们合成了一个原子分散的Mn-N 5通过将吡啶-N 掺杂到二维 (2D) 多孔纳米碳片(~3.56 nm 厚度)中的精确轴向配位催化剂,由于电荷分布不均匀,显示出锌空气电池中 ORR 的出色催化活性和超高稳定性与传统单中心 Mn-N 4催化剂和 Pt/C相比, Mn-N 5位点。这项工作为原位调节金属单原子的电子结构并进一步提升能源系统的整体 ORR 性能提供了新的策略。

更新日期:2023-02-13
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