Temperature and pH Affect the Sorption and Transformation of Dissolved Organic Carbon by Birnessite

IF 2.9 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

ACS Earth and Space Chemistry Pub Date : 2024-09-19 DOI:10.1021/acsearthspacechem.4c00125

Oluwadunsin Oyetunji, Dane Lamb, Oliver A. H. Jones, Suresh Subashchandrabose, Edward D. Burton

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Abstract

Soil mineralogy plays a vital role in carbon storage. Birnessite is a widely occurring manganese oxide mineral. Despite its widespread occurrence, studies of the interactions between natural soil organic carbon and manganese oxide minerals are rare. This study investigated the influence of triclinic birnessite on the transformation of vermicompost-derived dissolved organic carbon (DOC) at different pHs (4 and 8) and temperatures (25 and 50 °C). Enhanced adsorption and transformation of DOC, particularly at pH 4 and 50 °C, were observed. The use of SUVA₂₅₄ and fluorescence spectroscopy showed that DOC sorption caused an increase in carbon aromaticity, with the highest degree observed at pH 4 at 50 °C. In particular, X-ray photoelectron spectroscopy and near-edge X-ray absorption fine structure C 1s characterization showed an 8-fold increase in aromaticity at 50 °C compared to the unreacted DOC, with esterification and/or etherification reactions also occurring at pH 4. The impact of DOC sorption on birnessite stability and transformations was also assessed via X-ray absorption near-edge structure spectroscopy, which revealed that reacted and unreacted triclinic birnessite showed modest changes to Mn II, III, and IV. Manganese K-edge extended X-ray absorption fine structure spectroscopy showed the increased formation of hexagonal birnessite at pH 4, the formation of manganite at pH 4 and 8, 50 °C, and the formation of up to 6% ramsdellite at pH 8, 25 °C. This study provides new insights into the role of birnessite in soil carbon storage and manganese mineral transformations under environmentally relevant conditions.

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温度和 pH 值影响桦木岩对溶解有机碳的吸附和转化

土壤矿物学在碳储存中起着至关重要的作用。黝帘石是一种广泛存在的氧化锰矿物。尽管它广泛存在，但有关天然土壤有机碳与氧化锰矿物之间相互作用的研究却很少见。本研究调查了三棱沸石在不同 pH 值（4 和 8）和温度（25 和 50 °C）下对蛭石堆肥衍生的溶解有机碳（DOC）转化的影响。观察到 DOC 的吸附和转化能力增强，尤其是在 pH 值为 4 和 50 °C 时。使用 SUVA254 和荧光光谱分析表明，DOC 的吸附会导致碳芳香度的增加，在 pH 值为 4、温度为 50 ℃ 时，碳芳香度最高。特别是，X 射线光电子能谱和近边 X 射线吸收精细结构 C 1s 表征显示，与未反应的 DOC 相比，50 °C 时的芳香度增加了 8 倍，pH 值为 4 时也发生了酯化和/或醚化反应。DOC 吸附对桦木酸盐稳定性和转化的影响也通过 X 射线吸收近边结构能谱进行了评估，结果显示，已反应和未反应的三斜桦木酸盐对锰Ⅱ、锰Ⅲ和锰Ⅳ的变化不大。锰 K 边扩展 X 射线吸收精细结构光谱显示，pH 值为 4 时，六方桦锰矿的形成增加；pH 值为 4 和 8、50 °C 时，锰矿形成；pH 值为 8、25 °C 时，锰矿形成率高达 6%。这项研究为了解桦锰酸盐在环境相关条件下土壤碳储存和锰矿物转化中的作用提供了新的视角。

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来源期刊

ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology

CiteScore

5.30

自引率

11.80%

发文量

249

期刊介绍： The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.