Spin‐state Conversion by Asymmetrical Orbital Hybridization in Ni‐doped Co3O4 to Boost Singlet Oxygen Generation for Microbial Disinfection

• DOI: 10.1002/anie.202318924
• Publication Date: 2024-01-25T16:05:14Z
• Authors: Meilin Duan; Chao Huang; Gong Zhang; Hao Shi; Pengfei Zhang; Limin Li; Tong Xu; Zhen Zhao; Zhujun Fu; Jingrui Han; Yuanhong Xu; Xiaoteng Ding
• Keywords: Disinfection; Oxygen; 0301 basic medicine; 03 medical and health sciences; Singlet Oxygen; Escherichia coli; Nucleic Acid Hybridization; Hybridization, Genetic

AbstractSinglet oxygen (1O2) plays a significant role in environmental and biomedical disinfection fields. Electrocatalytic processes hold great potential for 1O2 generation, but remain challenging. Herein, a facile Ni doping converted spin‐state transition approach is reported for boosting 1O2 production. Magnetic analysis and theoretical calculations reveal that Ni occupied at the octahedral site of Co3O4 can effectively induce a low‐to‐high spin‐state transition. The high‐spin Ni−Co3O4 generate appropriate binding strength and enhance electron transfer between the Co centers with oxygen intermediates, thereby improving the catalytic activity of Ni−Co3O4 for effective generating 1O2. In neutral conditions, 1×106 CFU mL−1 Gram‐negative ESBL‐producing Escherichia coli (E. coli) could be inactivated by Ni−Co3O4 system within 5 min. Further antibacterial mechanisms indicate that 1O2 can lead to cell membrane damage and DNA degradation so as to irreversible cell death. Additionally, the developed Ni−Co3O4 system can effectively inactivate bacteria from wastewater and bioaerosols. This work provides an effective strategy for designing high‐spin electrocatalysis to boost 1O2 generation for disinfection process.