The role of surface hydroxyls on the radiolysis of gibbsite and boehmite nanoplatelets

Wang, Zheming; Walter, Eric D.; Sassi, Michel; Zhang, Xin; Zhang, Hailin; Li, Xiaohong Shari; Chen, Ying; Cui, Wenwen; Tuladhar, Aashish; Jessamy-Chase, Zizwe A.; Winkelman, Austin D.; Wang, Hong-Fei; Pearce, Carolyn I.; Clark, Sue B.; Rosso, Kevin M.

doi:10.1016/j.jhazmat.2020.122853

The role of surface hydroxyls on the radiolysis of gibbsite and boehmite nanoplatelets

Journal Article · Sun May 24 00:00:00 EDT 2020 · Journal of Hazardous Materials

DOI:https://doi.org/10.1016/j.jhazmat.2020.122853· OSTI ID:1638688

^[1]; ^[2]; ^[1]; Zhang, Xin ^[1]; Zhang, Hailin ^[1]; Li, Xiaohong Shari ^[1]; ^[2]; Cui, Wenwen ^[1]; ^[1]; Jessamy-Chase, Zizwe A. ^[2]; ^[1]; ^[3]; ^[1]; Clark, Sue B. ^[1]; ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Fudan Univ., Shanghai (China)

Understanding mechanistic pathways to radiolytic hydrogen generation by metal oxyhydroxide nanomaterials is challenging because of the difficulties of distinguishing key locations of OH bond scission, from structural interiors to hydroxylated surfaces to physi-sorbed water molecules. In this work we exploited the interface-selectivity of vibrational sum frequency generation (VSFG) to isolate surface versus bulk hydroxyl groups for gibbsite and boehmite nanoplatelets before and after ⁶⁰Co irradiation at dose levels of approximately 7.0 and 29.6 Mrad. While high-resolution microscopy revealed no effect on particle bulk and surface structures, VSFG results clearly indicated up to 83% and 94% radiation-induced surface OH bond scission for gibbsite and boehmite, respectively, a substantially higher proportion than observed for interior OH groups by IR and Raman spectroscopy. Electron paramagnetic spectroscopy revealed that the major radiolysis products bound in the mineral structures are trapped electrons, O, O₂^– and possibly F-centers in gibbsite, and H, O and O₃^– in boehmite, which persist on the time frame of several months. The entrapped radiolysis products appear to be highly stable, enduring re-hydration of particle surfaces, and likely reflect a permanent adjustment in the thermodynamic stabilities of these nanomaterials.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Interfacial Dynamics in Radioactive Environments and Materials (IDREAM); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1638688

Alternate ID(s):: OSTI ID: 1692186

Report Number(s):: PNNL-SA--150311

Journal Information:: Journal of Hazardous Materials, Journal Name: Journal of Hazardous Materials Vol. 398; ISSN 0304-3894

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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The role of surface hydroxyls on the radiolysis of gibbsite and boehmite nanoplatelets

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