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Free keywords:
dual active centers; fenton-like reactions; non-redox catalysis; reyctive oxygen species; single-atom catalysis
Abstract:
A broad range of chemical transformations driven by catalytic processes necessitate the electron transfer between catalyst and substrate. The redox cycle limitation arising from the inequivalent electron donation and acceptance of the involved catalysts, however, generally leads to their deactivation, causing substantial economic losses and environmental risks. Here we provide a “non-redox catalysis” strategy wherein the catalytic units were constructed by atomic Fe and B as dual active sites to create tensile force and electric field, which allowed directional self-decomposition of peroxymonosulfate (PMS) molecules through internal electron transfer to form singlet oxygen, bypassing the need of electron transfer between catalyst and PMS. The proposed catalytic approach with non-redox cycling of catalyst contributed to excellent stability of the active centers, while the generated reactive oxygen species found high efficiency in long-term catalytic pollutant degradation and selective organic oxidation synthesis in aqueous phase. This work offers new avenue for directional substrate conversion, which holds promise to advance the design of alternative catalytic pathways for sustainable energy conversion and valuable chemical production.
