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Ultrastrong Anion Affinity of Anionic Clay Induced by Its Inherent Nanoconfinement

机译:阴离子粘土诱导其固有纳米罚法的超空心阴离子亲和力

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摘要

Layered double hydroxide (LDH), the only anionic clay in the environment, plays a key role in natural ion transportation. The ion retention effect of LDHs was traditionally attributed to ion exchange with low affinity. Here, we demonstrated an ultrastrong interaction between anions and LDHs induced by their inherent nanoconfinement using chromium ore processing residue (COPR) that contained several Cr(Ⅵ)-bonded LDHs as a probe. Hydrocalumite (Ca/Al-Cl LDH) was verified as the primary phase for Cr(Ⅵ) retention through two types of interactions such as ion exchange and Cr-Ca coordination. More significantly, the confined spacing between two layers of hydrocalumite provided spatial restriction and shielding effects to the intercalated Cr(Ⅵ), which enhanced Cr-Ca coordination by shortening the bonding distance and modulating the binding angle to achieve the lowest bonding energy. Such enhancement boosted Cr(Ⅵ) affinity up to 3.2 × 10~5 mL/g, which was 1-3 orders of magnitudes higher than ion exchange. The universality of this mechanism was verified using another Mg/Al-Cl LDH and various anions. This study broke the traditional awareness of low ion affinities of LDHs limited by single ion exchange and disclosed an essential mechanism for unexpected ion retention effects of anionic clays in nature.
机译:分层双氢氧化物(LDH)是环境中唯一的阴离子粘土,在天然离子运输中起着关键作用。 LDH的离子保持效果传统上归因于具有低亲和力的离子交换。在这里,我们在含有铬矿石加工残基(COPR)作为探针中含有几种Cr(Ⅵ) - 粘合的LDH的固有纳米细胞诱导的阴离子和LDH之间的超空间相互作用。通过两种类型的相互作用如离子交换和CR-CA配位验证氢化合物(Ca / Al-Cl LDH)作为Cr(Ⅵ)保留的初级相。更重要的是,两层含水离子的限制间隔为插入的Cr(ⅵ)提供了空间限制和屏蔽效果,通过缩短粘合距离并调节结合角来实现最低粘合能量来增强CR-CA协调。这种增强增强Cr(ⅵ)亲和力可达3.2×10〜5ml / g,其比离子交换高出1-3个级。使用另一种Mg / Al-Cl LDH和各种阴离子来验证该机制的普遍性。该研究严重对单离子交换限制的LDH的低离子亲和性的传统意识,并公开了阴离子粘土意外的离子保留效应的基本机制。

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  • 来源
    《Environmental Science & Technology》 |2021年第2期|930-940|共11页
  • 作者单位

    Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling School of Environment and Energy and Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of Technology Guangzhou Guangdong 510006 P. R China;

    Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling School of Environment and Energy South China University of Technology Guangzhou Guangdong 510006 P. R. China;

    Jiangsu Academy of Science and Technology for Development Nanjing Jiangsu 210042 P. R. China;

    Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling School of Environment and Energy and Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of Technology Guangzhou Guangdong 510006 P. R China;

    Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling School of Environment and Energy and Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of Technology Guangzhou Guangdong 510006 P. R. China;

    Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling School of Environment and Energy and Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of Technology Guangzhou Guangdong 510006 P. R. China;

    Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling School of Environment and Energy and Guangdong Engineering and Technology Research Center for Environmental Nanomaterials South China University of Technology Guangzhou Guangdong 510006 P. R. China;

    School of Metallurgy and Environment Central South University Changsha 410083 P. R China;

    School of Metallurgy and Environment Central South University Changsha 410083 P. R. China;

  • 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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