Selective hydroxyl generation for efficient pollutant degradation by electronic structure modulation at Fe sites.

Zhan, Haiyin; Zhou, Ruiren; Wang, Pengfei; Zhou, Qixing · Proc Natl Acad Sci U S A · 2023

basic_science · Level V

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Abstract

Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is an important green oxidant in the field of sewage treatment, and how to improve its activation efficiency and generate free radicals with stronger oxidation performance is a key issue in current research. Herein, we synthesized a Cu-doped α-Fe<sub>2</sub>O<sub>3</sub> catalyst (7% Cu-Fe<sub>2</sub>O<sub>3</sub>) for activation of H<sub>2</sub>O<sub>2</sub> under visible light for degradation of organic pollutants. The introduction of a Cu dopant changed the d-band center of Fe closer to the Fermi level, which enhanced the adsorption and activation of the Fe site for H<sub>2</sub>O<sub>2</sub>, and the cleavage pathway of H<sub>2</sub>O<sub>2</sub> changed from heterolytic cleavage to homolytic cleavage, thereby improving the selectivity of •OH generation. In addition, Cu doping also promoted the light absorption ability of α-Fe<sub>2</sub>O<sub>3</sub> and the separation of hole-electron pairs, which enhanced its photocatalytic activities. Benefiting from the high selectivity of •OH, 7% Cu-Fe<sub>2</sub>O<sub>3</sub> exhibited efficient degradation activities against ciprofloxacin, the degradation rate was 3.6 times as much as that of α-Fe<sub>2</sub>O<sub>3</sub>, and it had good degradation efficiency for a variety of organic pollutants.