Redox Cycling Driven Transformation of Layered Manganese Oxides to Tunnel Structures

Jung, Haesung; Taillefert, Martial; Sun, Jingying; Wang, Qian; Borkiewicz, Olaf J.; Liu, Pan; Yang, Lufeng; Chen, Shuo; Chen, Hailong; Tang, Yuanzhi

doi:10.1021/jacs.9b12266

Redox Cycling Driven Transformation of Layered Manganese Oxides to Tunnel Structures

Journal Article · Wed Jan 08 00:00:00 EST 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b12266· OSTI ID:1755664

Jung, Haesung ^[1]; ^[1]; Sun, Jingying ^[2]; Wang, Qian ^[1]; Borkiewicz, Olaf J. ^[3]; Liu, Pan ^[1]; Yang, Lufeng ^[1]; Chen, Shuo ^[1]; ^[1]; ^[1]

Georgia Inst. of Technology, Atlanta, GA (United States)
Univ. of Houston, TX (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Mn oxides are among the most ubiquitous minerals on Earth and play critical roles in numerous elemental cycles in biotic/abiotic loops as the key redox center. Yet, it has long puzzled geochemists why the laboratory synthesis of todorokite, a tunnel-structured Mn oxide, is extremely difficult while it is the dominant form over other tunneled phases in low-temperature natural environments. This study employs a novel electrochemical method to mimic the cyclic redox reactions occurring over long geological time scales in an accelerated manner. The results revealed that the kinetics and electron flux of the cyclic redox reaction are key to the layer-to-tunnel structure transformation of Mn oxides, provided new insights for natural biotic and abiotic redox reactions, and explained the dominance of todorokite in nature.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1755664

Alternate ID(s):: OSTI ID: 1689990

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 5 Vol. 142; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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