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Coupled Manganese Redox Cycling and Organic Carbon Degradation on Mineral Surfaces

机译:含有矿物表面上的锰氧化还原循环与有机碳劣化

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摘要

Minerals, natural organic matter (NOM), and divalent manganese (Mn(Ⅱ)) often coexist in suboxic/oxic environment. Multiple adsorption and oxidation processes occur in this ternary system, which are coupled to affect the fate of both OM and Mn therein and alter their chemical reactivity toward metals and other pollutants. However, the details about the coupling are poorly known although much has been gained for the binary systems. We determined the mutual influence of surface catalyzed Mn(Ⅱ) oxidation and humic acid (HA) adsorption and oxidation in a Fe(Ⅲ) oxide (goethite)-HA-Mn(Ⅱ) system at pH 5-8. The presence of Mn(Ⅱ) substantially increased HA adsorption whereas HA greatly impaired the extent and rate of Mn(Ⅱ) oxidation by O_2 on goethite surfaces. The impacts were more pronounced at higher pH. Mn(Ⅱ) oxidation produced β-MnOOH, γ-MnOOH, and Mn_3O_4 which in turn oxidized HA, producing small organic acids. The presence of HA markedly altered the composition of Mn(Ⅱ) oxidation products by inhibiting the formation of β-MnOOH while favoring the production of γ-MnOOH and Mn(Ⅱ) adsorbed on the HA-mineral assemblage. Nonconducting γ-Al_2O_3 exhibited similar but weaker effects than semiconducting goethite in the above processes. Our results suggest that similar to Mn-oxidizing microorganisms, mineral surfaces can drive the coupling of the Mn redox cycle with NOM oxidative degradation under suboxic/oxic and circumneutral/alkaline conditions.
机译:矿物质,天然有机物(NOM)和二价锰(Mn(Ⅱ))经常在解释/氧环境中共存。在该三元系统中发生多种吸附和氧化过程,其耦合以影响OM和Mn的命运,并改变其对金属和其他污染物的化学反应性。然而,耦合的细节是众所周知的,尽管二元系统已经获得了太多。我们确定在pH5-8处的Fe(Ⅲ)氧化物(甲酸酯)-Ha-Mn(Ⅱ)系统中的表面催化的Mn(Ⅱ)氧化和腐殖酸(HA)吸附和氧化的相互影响。 Mn(Ⅱ)的存在基本上增加了HA吸附,而HA大大损害了O_2对甲石表面上的Mn(Ⅱ)氧化的程度和速率。影响更高的pH值更加明显。 Mn(Ⅱ)氧化产生β-mnooh,γ-mnooh和mn_3O_4,其又氧化HA,产生小有机酸。 HA的存在明显改变Mn(Ⅱ)氧化产物的组合物,抑制β-Mnooh的形成,同时有利于吸附在Ha-矿物组合上的γ-mnooh和Mn(Ⅱ)的产生。非导电γ-Al_2O_3表现出与上述过程中的半导体聚乙烯相似但较弱的效果。我们的研究结果表明,类似于Mn氧化微生物,矿物表面可以在解冻/氧化和血管/碱性条件下将Mn氧化还原循环与NOM氧化降解驱动。

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  • 来源
    《Environmental Science & Technology》 |2020年第14期|8801-8810|共10页
  • 作者单位

    Department of Ecosystem Science and Management University of Wyoming Wyoming 82071 United States College of Resource and Environment Qingdao Agricultural University Qingdao Shandong 266109 China;

    Department of Ecosystem Science and Management University of Wyoming Wyoming 82071 United States College of Resource and Environment Qingdao Agricultural University Qingdao Shandong 266109 China;

    Department of Ecosystem Science and Management University of Wyoming Wyoming 82071 United States;

    Department of Ecosystem Science and Management University of Wyoming Wyoming 82071 United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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