期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 5, 期 11, 页码 10624-10632出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.7b02606
关键词
Manganese; Sunlight; Nitrate; Superoxide; Mn(III)-pyrophosphate; Nanosheets stacking; Pair distribution function
资金
- National Science Foundation's Environmental Chemical Sciences program [CHE-1610728]
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
Recent findings have showed the environmental abundance of soluble Mn(III)-complexes (e.g., Mn-siderophore and Mn(III)-pyrophosphate (Mn(III)-PP)). Specifically, Mn(III)PP is of emerging interest in understanding Mn redox cycling and phosphorus cycling in catalysis and environmental systems. Curiously, however, further oxidation of Mn(III)-PP and consequent formation of a MnO2 solid phase have not been considered yet. Here, using photochemically-assisted fast oxidation of Mn2+ (aq) by the reaction with superoxide, generated from nitrate photolysis, we report the role of PP in formation of disordered delta-MnO2 nanosheets and changes in their stacking and structures. With increasing PP concentrations from 0.3 to 2 mM, (delta-MnO2 nanosheets showed better stacking (thicker) layers and an alteration from hexagonal to orthogonal structure (more Mn(III) in layers). We found that the amount of Mn(III)-PP complex and the formation rate of delta-MnO2 nanosheets under the different PP concentrations affected both their layer structures and stacking behaviors. These findings open a new possibility of using photochemically-assisted green chemistry to control the properties of disordered (delta-MnO2 birnessite nanosheets for use in more effective catalytic reactions, such as water oxidation, and suggest the importance of Mn(III)-PP complexes for the formation of (delta-MnO2 nanosheets in nature.
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