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Manganese(ii) phosphate nanosheet assembly with native out-of-plane Mn centres for electrocatalytic water oxidation.

ABSTRACT: Nature selects Mn-clusters as catalysts for water oxidation, which is a significant reaction in photosynthesis. Thus, it is of critical importance to develop Mn-based superstructures and study their catalytic details for water-splitting-based renewable energy research. Herein, we report a manganese(ii) phosphate nanosheet assembly with asymmetric out-of-plane Mn centers from the transformation of amine-intercalated nanoplates for efficient electrocatalytic water oxidation in neutral aqueous solutions. From structural and computational studies, it is found that the native out-of-plane Mn centers with terminal water ligands are accessible and preferential oxidation sites to form active intermediates for water oxidation. In addition, the asymmetry can stabilize the key MnIII intermediate, as demonstrated by electrochemical and spectrometric studies. This study delivers a convenient strategy to prepare unique nanosheet assemblies for electrocatalysis and fundamental understandings of oxygen evolution chemistry.

SUBMITTER: Liu H

PROVIDER: S-EPMC6333235 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Manganese(ii) phosphate nanosheet assembly with native out-of-plane Mn centres for electrocatalytic water oxidation.

Liu Hongfei H Gao Xueqing X Yao Xiaolong X Chen Mingxing M Zhou Guojun G Qi Jing J Zhao Xueli X Wang Weichao W Zhang Wei W Cao Rui R

Chemical science 20181002 1

Nature selects Mn-clusters as catalysts for water oxidation, which is a significant reaction in photosynthesis. Thus, it is of critical importance to develop Mn-based superstructures and study their catalytic details for water-splitting-based renewable energy research. Herein, we report a manganese(ii) phosphate nanosheet assembly with asymmetric out-of-plane Mn centers from the transformation of amine-intercalated nanoplates for efficient electrocatalytic water oxidation in neutral aqueous solu ...[more]

PMID: 30713630

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Project description:UnlabelledThe mechanisms, key organisms, and geochemical significance of biological low-pH Mn(II) oxidation are largely unexplored. Here, we investigated the structure of indigenous Mn(II)-oxidizing microbial communities in a secondary subsurface Mn oxide deposit influenced by acidic (pH 4.8) metal-rich groundwater in a former uranium mining area. Microbial diversity was highest in the Mn deposit compared to the adjacent soil layers and included the majority of known Mn(II)-oxidizing bacteria (MOB) and two genera of known Mn(II)-oxidizing fungi (MOF). Electron X-ray microanalysis showed that romanechite [(Ba,H2O)2(Mn(4+),Mn(3+))5O10] was conspicuously enriched in the deposit. Canonical correspondence analysis revealed that certain fungal, bacterial, and archaeal groups were firmly associated with the autochthonous Mn oxides. Eight MOB within the Proteobacteria, Actinobacteria, and Bacteroidetes and one MOF strain belonging to Ascomycota were isolated at pH 5.5 or 7.2 from the acidic Mn deposit. Soil-groundwater microcosms demonstrated 2.5-fold-faster Mn(II) depletion in the Mn deposit than adjacent soil layers. No depletion was observed in the abiotic controls, suggesting that biological contribution is the main driver for Mn(II) oxidation at low pH. The composition and species specificity of the native low-pH Mn(II) oxidizers were highly adapted to in situ conditions, and these organisms may play a central role in the fundamental biogeochemical processes (e.g., metal natural attenuation) occurring in the acidic, oligotrophic, and metalliferous subsoil ecosystems.ImportanceThis study provides multiple lines of evidence to show that microbes are the main drivers of Mn(II) oxidation even at acidic pH, offering new insights into Mn biogeochemical cycling. A distinct, highly adapted microbial community inhabits acidic, oligotrophic Mn deposits and mediates biological Mn oxidation. These data highlight the importance of biological processes for Mn biogeochemical cycling and show the potential for new bioremediation strategies aimed at enhancing biological Mn oxidation in low-pH environments for contaminant mitigation.

Dataset Information

Manganese(ii) phosphate nanosheet assembly with native out-of-plane Mn centres for electrocatalytic water oxidation.

Publications

Manganese(ii) phosphate nanosheet assembly with native out-of-plane Mn centres for electrocatalytic water oxidation.

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