Orbital Occupancy Modulation to Optimize Intermediate Absorption for Efficient Electrocatalysts in Water Electrolysis and Zinc-Ethanol-Air Battery
學年 112
學期 2
出版（發表）日期 2024-03-04
作品名稱 Orbital Occupancy Modulation to Optimize Intermediate Absorption for Efficient Electrocatalysts in Water Electrolysis and Zinc-Ethanol-Air Battery
作品名稱（其他語言）
著者 Yanting Ye; Jinchang Xu; Xiulan Li; Yongqi Jian; Fangyan Xie; Jian Chen; Yanshuo Jin; Xiang Yu; Ming-Hsien Lee; Nan Wang; Shuhui Sun; Hui Meng
單位
出版者
著錄名稱、卷期、頁數 Advanced Materials 36(23), 2312618
摘要 Spin engineering is a promising way to modulate the interaction between the metal d-orbital and the intermediates and thus enhance the catalytic kinetics. Herein, an innovative strategy is reported to modulate the spin state of Co by regulating its coordinating environment. o-c-CoSe2-Ni is prepared as pre-catalyst, then in situ electrochemical impedance spectroscopy (EIS) and in situ Raman spectroscopy are employed to prove phase transition, and CoOOH/Co3O4 is formed on the surface as active sites. In hybrid water electrolysis, the voltage has a negative shift, and in zinc–ethanol–air battery, the charging voltage is lowered and the cycling stability is greatly increased. Coordinated atom substitution and crystalline symmetry change are combined to regulate the absorption ability of reaction intermediates with balanced optimal adsorption. Coordinated atom substitution weakens the adsorption while the crystalline symmetry change strengthens the adsorption. Importantly, the tetrahedral sites are introduced by Ni doping which enables the co-existence of four-coordinated sites and six-coordination sites in o-c-CoSe2-Ni. The dz2 + dx2-y2 orbital occupancy decreases after the atomic substitution, while increases after replacing the CoSe6-Oh field with CoSe6-Oh/CoSe4-Td. This work explores a new direction for the preparation of efficient catalysts for water electrolysis and innovative zinc–ethanol–air battery.
關鍵字
語言 en_US
ISSN 1521-4095; 0935-9648
期刊性質 國外
收錄於 SCI
產學合作
通訊作者
審稿制度 否
國別 USA
公開徵稿
出版型式 ,電子版
相關連結

機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/127548 )