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首页> 外文期刊>Environmental Science & Technology >Synergetic Molecular Oxygen Activation and Catalytic Oxidation of Formaldehyde over Defective MIL-88B(Fe) Nanorods at Room Temperature
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Synergetic Molecular Oxygen Activation and Catalytic Oxidation of Formaldehyde over Defective MIL-88B(Fe) Nanorods at Room Temperature

机译：在室温下缺陷MIL-88B（Fe）纳米棒（Fe）甲醛的协同作用分子氧活化和催化氧化

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摘要

Defective MIL-88B(Fe) nanorods are exploited as exemplary iron-bearing metal-organic framework (MOF) catalyst for molecular oxygen (O_2) activation at ambient temperature, triggering effective catalytic oxidation of formaldehyde (HCHO), one of the major indoor air pollutants. Defective MIL-88B(Fe) nanorods, growing along the [001] direction, expose abundant coordinatively unsaturated Fe-sites (Fe-CUSs) along extended hexagonal channels with a diameter of ca. 5 A, larger enough for the diffusion of O_2 (3.46 A) and HCHO (2.7 A). The Lewis acid-base interaction between Fe-CUSs and accessible HCHO accelerates the Fe~Ⅲ/Fe~Ⅱ cycle, catalyzing Fenton-like O_2 activation to produce reactive oxidative species (ROSs), including superoxide radicals (•O_2~-), hydroxyl radicals (•OH), and singlet oxygen (~1O_2). Consequently, adsorbed HCHO can be oxidized into CO_2 with a considerable mineralization efficiency (over 80%) and exceptional recyclability (4 runs, 48 h). Dioxymethylene (CH_2OO), formate (HCOO~-) species, and formyl radicals (•CHO) are recorded as the main reaction intermediates during HCHO oxidation. HCHO, H_2O, and O_2 are captured and activated by abundant Fe~Ⅲ/Fe~Ⅱ-CUSs as acid/base and redox sites, triggering synergetic ROS generation and HCHO oxidation, involving cooperative acid-base and redox catalysis processes. This study will bring new insights into exploiting novel MOF catalysts for efficient O_2 activation and reliable indoor air purification at ambient temperature.
机译：有缺陷的MIL-88b（Fe）纳米棒被利用为用于在环境温度下的用于分子氧（O_2）活化的示例性耐铁金属 - 有机骨架（MOF）催化剂，引发有效的甲醛（HCHO）的有效催化氧化，其中一个主要的室内空气污染物。有缺陷的MIL-88b（Fe）纳米棒，沿着[001]方向生长，沿着直径的延伸的六边形通道暴露丰富的坐标不饱和的Fe-sita（Fe-cuss）。 5 a，足以扩散O_2（3.46a）和Hcho（2.7a）。 Fe-Cuss和Accessible Hcho之间的Lewis酸碱相互作用加速了Fe〜Ⅲ/ Fe〜Ⅱ循环，催化Fenton样O_2活化以产生反应性氧化物种（罗斯），包括超氧基自由基（•O_2〜 - ），羟基自由基（•哦）和单线氧（〜1O_2）。因此，吸附的Hcho可以被氧化成具有相当大的矿化效率（超过80％）和特殊再循环性（4次，48小时）。二恶英亚甲基（CH_2OO），甲酸盐（HCOO〜 - ）物种和甲酰基自由基（•CHO）被记录为HCHO氧化过程中的主要反应中间体。通过丰富的Fe〜Ⅲ/ Fe〜Ⅱ-Cuss作为酸/碱和氧化还原位点来捕获和激活Hcho，H_2O和O_2，触发协同ros生成和Hcho氧化，涉及合作酸碱和氧化还原催化过程。本研究将新的见解，以利用新型MOF催化剂，以便在环境温度下进行高效O_2活化和可靠的室内空气净化。

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  • 来源
    《Environmental Science & Technology》 |2021年第12期|8341-8350|共10页
  • 作者

    Shuping Zhang; Yifan Zhuo; Chizoba I. Ezugwu; Chong-chen Wang; Chuanhao Li; Shengwei Liu;

  • 作者单位

    School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510006 P. R. China;

    School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510006 P. R. China;

    School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510006 P. R. China;

    Beijing Key Laboratory of Functional Materials for Building Structure and Environment Remediation Beijing University of Civil Engineering and Architecture Beijing 100044 P. R. China;

    School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510006 P.R. China;

    School of Environmental Science and Engineering Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology Sun Yat-sen University Guangzhou 510006 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);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    metal-organic framework; coordinatively unsaturated sites; molecular oxygen activation; jormaldehyde; catalytic; synergetic; Fenton-like;

    机译：金属 - 有机框架;协调不饱和位点;分子氧活化;jormaldehyde;催化;协同作用;芬顿般的;

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