Nanoscale Surface Activation via Reticular Chemistry for Reactive H2S Sequestration Surpassing 1500 mgH2S g–1 under Ambient Conditions

Nanoscale Surface Activation via Reticular Chemistry for Reactive H2S Sequestration Surpassing 1500 mgH2S g–1 under Ambient Conditions

ACS Nano

10.1021/acsnano.5c14225

https://doi.org/10.1021/acsnano.5c14225

Li Shiuan Ng, Jun Jing Teh, Zhi Zhong Ang, Veronica Pereira, Sankar Das, Brynne Shu Ni Tan, Hiang Kwee Lee

03 November 2025

Ng, L. S., Teh, J. J., Ang, Z. Z., Pereira, V., Das, S., Tan, B. S. N., & Lee, H. K. (2025). Nanoscale Surface Activation via Reticular Chemistry for Reactive H 2 S Sequestration Surpassing 1500 mg H2S g –1 under Ambient Conditions. ACS Nano, 19(45), 39349–39361. https://doi.org/10.1021/acsnano.5c14225

Efficient H2S removal 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 mgH2S·g⁻¹) and require elevated operating conditions due to limited active sites and kinetic barriers. Herein, we achieve efficient H2S sequestration at ambient conditions by chemically activating metal oxide surfaces using reticular chemistry to enhance solid-gas reactions. This approach integrates 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 higher H2S sequestration of up to 1524 mgH2S·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 and 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.

Publisher Copyright

This research / project is supported by the Agency for Science, Technology and Research - Manufacturing, Trade, and Connectivity Individual Research Grant
Grant Reference no. : MTC IRG M23M6c0098

This research / project is supported by the Agency for Science, Technology and Research - Advanced Manufacturing and Engineering (AME) Young Individual Research Grant
Grant Reference no. : AME YIRG A2084c0158

This research / project is supported by the Ministry of Education, Singapore - Academic Research Fund Tier 1
Grant Reference no. : RS13/20

This research / project is supported by the Ministry of Education, Singapore - Academic Research Fund Tier 1
Grant Reference no. : RG4/21

This research / project is supported by the National University of Singapore - Center of Hydrogen Innovation
Grant Reference no. : CHI-P2022-05

This research / project is supported by the Nanyang Technological University - Start-up grants
Grant Reference no. :

This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsnano.5c14225.

https://oar.a-star.edu.sg/communities-collections/articles/22994

1936-0851
1936-086X

Institute of Materials Research and Engineering