Synergistic modulation of d‐Band Center in δ‐MnO2 viaTungsten Doping and Oxygen Defects for BoostedAqueous Magnesium‐Ion Storage Performance

影响因子：12.0

DOI码：10.1002/cnl2.70144

发表刊物：Carbon Neutralization

关键字：Aqueous magnesium‐ion batteries; D‐band center; Doping and defect; Electronic structure; δ‐MnO2

摘要：Poor inherent conductivity, sluggish reaction kinetics, and structural instability have widely limited the use of layered δ‐MnO2 in aqueous magnesium‐ion storage. Inspired by the d‐band center (εd) theory, this study synthesizes oxygen defective W‐doped δ‐MnO2 (Od‐WMO) with a tailored d‐band center through a two‐step hydrothermal‐calcination method to address the above bottlenecks. The results of theoretical calculation demonstrate that synergistic modulation mechanism of tungsten doping andoxygen defects not only promotes the upward shift of the εd of Mn, significantly enhancing the adsorption capacity for Mg2+, but also simultaneously strengthens Mn‐O bonds, thereby markedly improving structural stability. Moreover, the synergistic modulation effect of the two also dramatically narrows the band gap, lowers the migration energy barrier, as well as speeds up the dynamics of charge transport/ion diffusion. As expected, Od‐WMO demonstrates outstanding structural durability andremarkable storage capacity (185.2 mAh g−1 at 0.1 A g−1). Moreover, 3,4,9,10‐perylenetetracarboxylic diimide (PTCDI) as anodeto assembled Od‐WMO//PTCDI full cell also exhibit a stable working state. This study uncovers the synergistic modulation mechanism of doping and defect engineering on MnO2's εd, makes up for the limitation in current research that focuses solelyon individual regulatory effects of doping or defects. It provides valuable insights for the rational design of high‐performance electrode materials for AMIBs and other electrochemical energy storage systems via d‐band center engineering.

合写作者：Zhang Yifu,Zhang Shaoqing,Zhou Zhenhua,Zhao Hongxin,Liu Xin

论文类型：期刊论文

通讯作者：Wang Yang*,Meng Changgong*,Huang Chi*

论文编号：e70144

卷号：5

页面范围：e70144, 2026

是否译文：否

发布期刊链接：https://doi.org/10.1002/cnl2.70144