Nanoscale Surface Activation via Reticular Chemistry for Reactive H₂S Sequestration Surpassing 1500 mg_H2S g^-1 under Ambient Conditions.

Abstract

Efficient removal of H₂S from industrial emissions and the environment is crucial for safeguarding human health and ecosystems. Conventional metal oxide-based materials for H₂S sequestration trap sulfur species in solid matrices but suffer from low uptake capacity (<65 mg_H2S g^-1) and require elevated operating conditions due to limited active sites and kinetic barriers. Herein, we achieve efficient H₂S sequestration under ambient conditions by chemically activating metal oxide surfaces using reticular chemistry to enhance solid-gas reactions. This approach integrates a metal oxide core with a metal-organic framework (MOF) layer, forming a surface-activated interfacial nanoreactor (SAIN). The MOF facilitates H₂S transfer to the functional interface while activating the metal oxide surface for enhanced reactivity. SAIN achieves a higher H₂S sequestration of up to 1524 mg_H2S g^-1 across a wide concentration range with nearly 100% efficiency. It demonstrates a >23-fold improvement over standalone metal oxide and/or MOF platforms, higher than emerging materials by up to 508-fold in H₂S uptake and 24-fold in sequestration rate. Mechanistic studies reveal that interfacial electron migration and electronic hybridization weaken metal-oxygen bonds, enhancing their interactions with H₂S and promoting efficient reactive sequestration. Our "activate-react-lock" strategy offers valuable insights for designing functional interfaces to activate nanomaterial surfaces for diverse environmental, chemical, and energy applications.