反键分子轨道
电催化剂
脱质子化
氢氧化物
镍
甲醇
催化作用
化学
光化学
无机化学
氧化态
物理化学
电化学
原子轨道
电子
有机化学
电极
物理
离子
量子力学
作者
Junhua Li,Chao Wu,Zhen Wang,Hecheng Meng,Qi Zhang,Y.J. Tang,Anqi Zou,Yihe Zhang,Haoyin Zhong,Shibo Xi,Junmin Xue,Xiaopeng Wang,Jiagang Wu
标识
DOI:10.1002/anie.202404730
摘要
The anodic methanol oxidation reaction (MOR) plays a crucial role in coupling with the cathodic hydrogen evolution reaction (HER) and enables the sustainable production of the high‐valued formate. Nickel‐based hydroxide (Ni(OH)2) as MOR electrocatalyst has attracted enormous attention. However, the key factor determining the intrinsic catalytic activity remains unknown, which significantly hinders the further development of Ni(OH)2 electrocatalyst. Here, we found that the dx2‐y2 electronic state within antibonding bands plays a decisive role in the whole MOR process. The onset potential depends on the deprotonation ability (Ni2+ to Ni3+), which was closely related to the band center of dx2‐y2 orbital. The closer of dx2‐y2 orbital to the Fermi level showed the stronger the deprotonation ability. Meanwhile, in the high potential region, the broadening of dx2‐y2 orbital would facilitate the electron transfer from methanol to catalysts (Ni3+ to Ni2+), further enhancing the catalytic properties. Our work for the first time clarifies the intrinsic relationship between dx2‐y2 electronic state and the MOR activities, which adds a new layer of understanding to the methanol electrooxidation research scene.
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