Medium spin FeIII regulating the peroxide selectivity in the heterogeneous oxygen reduction reaction of spin-polarized Fe-TAML complexes
學年 114
學期 1
出版（發表）日期 2025-11-21
作品名稱 Medium spin FeIII regulating the peroxide selectivity in the heterogeneous oxygen reduction reaction of spin-polarized Fe-TAML complexes
作品名稱（其他語言）
著者 Cheng-Han Tso; Chih-Hung Hsu; Jiali Wang; Po-Yi Lin; Huang-Teng Lin; Nozomu Hiraoka; Ming-Kang Tsai; Chih-Hsin Chen; Hao Ming Chen
單位
出版者
著錄名稱、卷期、頁數 Materials Horizons 2025 12 ,p. 9808
摘要 Hydrogen peroxide (H2O2) can be produced cleanly and sustainably using electrosynthesis from the oxygen reduction reaction (ORR) via a 2-electron pathway, as opposed to the conventional anthraquinone technique. However, the rational design protocols for promoting the peroxide selectivity of ORR catalysts are still inadequate. This work synthesized a series of medium FeIII complexes with tetra-amido macrocyclic ligands (Fe-TAMLs) using a simplified two-step procedure. A relationship between peroxide selectivity and the spin polarization of metal centers in these Fe-TAML complex ORR catalysts is revealed. Using X-ray absorption spectroscopy (XAS) and X-ray emission spectroscopy (XES), the spin polarization of metal centers in Fe-TAMLs regulated by the ligand modification was studied. We found that the nitro group-substituted ligand Fe-TAML complex was regulated by its spin-polarization and offered the highest spin state enhancing peroxide selectivity about 55% to 78%. An operando XAS study is employed to verify the stability of the oxidation states and the robustness of the coordination structures of the Fe-TAMLs.
關鍵字
語言 en
ISSN
期刊性質 國外
收錄於 SCI Scopus
產學合作
通訊作者
審稿制度 是
國別 GBR
公開徵稿
出版型式 ,電子版,紙本
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機構典藏連結 ( http://tkuir.lib.tku.edu.tw:8080/dspace/handle/987654321/129194 )