Metal Adsorption Controls Stability of Layered Manganese Oxides

Yang, Peng; Post, Jeffrey E.; Wang, Qian; Xu, Wenqian; Geiss, Roy; McCurdy, Patrick R.; Zhu, Mengqiang

doi:10.1021/acs.est.9b01242

Title: Metal Adsorption Controls Stability of Layered Manganese Oxides

Journal Article · Wed May 22 00:00:00 EDT 2019 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.9b01242· OSTI ID:1559537

Yang, Peng ^[1]; Post, Jeffrey E. ^[2]; Wang, Qian ^[1]; Xu, Wenqian ^[3]; Geiss, Roy ^[4]; McCurdy, Patrick R. ^[4];

^[1]

Univ. of Wyoming, Laramie, WY (United States)
Smithsonian Inst., Washington, DC (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Colorado State Univ., Fort Collins, CO (United States)

Hexagonal birnessite, a typical layered Mn oxide (LMO), can adsorb and oxidize Mn(II) and thereby transform to Mn(III)-rich hexagonal birnessite, triclinic birnessite, and/or tunneled Mn oxides (TMOs), remarkably changing the environmental behavior of Mn oxides. We have determined the effects of co-existing cations on the transformation by incubating Mn(II)-bearing δ-MnO₂ at pH 8 under anoxic conditions for 25 d (dissolved Mn < 11 μM). In the Li⁺, Na⁺ or K⁺ chloride solution, the Mn(II)-bearing δ-MnO₂ first transforms to Mn(III)-rich δ-MnO₂ and/or triclinic birnessite (T-bir) due to the Mn(II)-Mn(IV) comproportionation, most of which eventually transform to a 4 × 4 TMO. In contrast, Mn(III)-rich δ-MnO₂ and T-bir form and persist in the Mg²⁺ or Ca²⁺ chloride solution. Yet, in the presence of surface adsorbed Cu(II), Mn(II)-bearing δ-MnO₂ turns into Mn(III)-rich δ-MnO₂ without forming T-bir or TMOs. The stabilizing power of the cations on the δ-MnO₂ structure positively correlates with their binding strength to δ-MnO₂ (Li⁺, Na⁺ or K⁺ < Mg²⁺ or Ca²⁺ < Cu(II)). Since metal adsorption decreases the surface energy of minerals, our result suggests that the surface energy largely controls the thermodynamic stability of LMOs. Our study implies that the adsorption of divalent metal cations, particularly transition metals, can be a prime cause of the high abundance of LMOs, rather than the more stable TMO phases, in the environment.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Wyoming, Laramie, WY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Experimental Program to Stimulate Competitive Research (EPSCoR)

Grant/Contract Number:: AC02-06CH11357; SC0016272

OSTI ID:: 1559537

Alternate ID(s):: OSTI ID: 1854156

Journal Information:: Environmental Science and Technology, Vol. 53, Issue 13; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 26 works

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