兴奋剂
系列(地层学)
电荷(物理)
Atom(片上系统)
酒
分布(数学)
材料科学
化学物理
化学
原子物理学
光电子学
物理
有机化学
数学
计算机科学
古生物学
量子力学
生物
嵌入式系统
数学分析
作者
Liu Huang,Rui Lü,Wenchang Zhang,Yikang Fan,Yuanxin Du,Kun Ni,Jianglin Ye,Manzhou Zhu
标识
DOI:10.1002/anie.202412964
摘要
High efficiently photocatalytic CO2 reduction (CO2RR) into liquid fuels in pure water system remains challenged. Iron polyphthalocyanine (FePPc) with strong light harvesting, unique Fe‐N4 structure, abundant pores, and good stability could serve as a promising catalyst for CO2 photoreduction. To further improve the catalytic efficiency, herein, symmetry‐breaking Fe sites are constructed by coupling with atomically precise M1Ag24 (M=Ag, Au, Pt) series clusters. Especially, the introduction of Pt1Ag24 causes the most asymmetric charge distribution of Fe in FePPc (followed by Au1Ag24 and Ag25), leading to the favorable CO2 adsorption and activation. In addition, Pt1Ag24‐FePPc exhibits the most effective photogenerated carriers transfer and separation. As a result, Pt1Ag24‐FePPc shows the methanol/ethanol yield of 48.55/32.97 μmol·gcat−1·h−1 in H2O‐CO2 system under visible light irradiation, ~ 1.65/1.25‐fold, 1.83/1.37‐fold, and 3.6/1.61‐fold higher than that of Au1Ag24‐FePPc, Ag25‐FePPc, and FePPc, respectively. This work provides a concept for precisely construction and regulation symmetry‐breaking sites of cluster‐based catalysts for effective CO2 conversion.
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