Abstract Ionic modulation, in particular that by hydrogen intercalation, has become a powerful method to tune the material’s properties in recent years. Though the SrFeOx system is akin to SrCoOx that can be protonated to the HSrCoO2.5 phase, it remains a challenge for the hydrogenation of SrFeO2.5. In this work, starting from the perovskite SrFeO3-δ, we achieved the hydrogen intercalation and obtained a stable hydrogenated brownmillerite phase HSrFeO2.5 via Pt-catalyzed H-spillover at room temperature. The results indicate that the hydrogenation process is accompanied by the simultaneous oxygen ionic release, i.e., the perovskite SrFeO3-δ is the prerequisite of the hydrogen-induced phase transition. Then, by realization of the hydrogenation, the complete phase transition cycle among the perovskite SrFeO3-δ, brownmillerite SrFeO2.5 and the hydrogenated HSrFeO2.5 phase, are finished. Upon hydrogenation, SrFeO3-δ exhibits a remarkable 9.4% lattice expansion, and its electronic state undergoes a multi-step evolution, transforming from pristine helical antiferromagnetic insulator to a bad metal, and eventually returning to an antiferromagnetic insulator. Moreover, based on the obtained results we also successfully fabricated the microscale patterns with varied surface morphology and electric conductivity that can be used to construct electronic devices. This work provides a different pathway to modulate the properties of correlated and functional materials.
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