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首页> 外文期刊>Advanced Materials >Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride
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Runaway Carbon Dioxide Conversion Leads to Enhanced Uptake in a Nanohybrid Form of Porous Magnesium Borohydride

机译：失控的二氧化碳转化导致多孔硼氢化镁纳米杂化形式的吸收增加。

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摘要

Leveraging molecular-level controls to enhance CO2 capture in solid-state materials has received tremendous attention in recent years. Here, a new class of hybrid nanomaterials constructed from intrinsically porous gamma-Mg(BH4)(2) nanocrystals and reduced graphene oxide (MBHg) is described. These nanomaterials exhibit kinetically controlled, irreversible CO2 uptake profiles with high uptake capacities (>19.9 mmol g(-1)) at low partial pressures and temperatures between 40 and 100 degrees C. Systematic experiments and first-principles calculations reveal the mechanism of reaction between CO2 and MBHg and unveil the role of chemically activated, metastable (BH3-HCOO)(-) centers that display more thermodynamically favorable reaction and potentially faster reaction kinetics than the parent BH4- centers. Overall, it is demonstrated that size reduction to the nanoscale regime and the generation of reactive, metastable intermediates improve the CO2 uptake properties in metal borohydride nanomaterials.
机译：近年来，利用分子水平的控制来增强固态材料中的CO2捕集受到了极大的关注。在此，描述了一种新型的杂化纳米材料，该杂化纳米材料由本征多孔的γ-Mg（BH4）（2）纳米晶体和还原的氧化石墨烯（MBHg）构成。这些纳米材料在低分压和40至100摄氏度之间的温度下，具有高吸收容量（> 19.9 mmol g（-1））的动力学控制，不可逆的CO2吸收曲线。系统实验和第一性原理计算揭示了两者之间反应的机理CO2和MBHg并揭示了化学活化的亚稳态（BH3-HCOO）（-）中心的作用，与母体BH4-中心相比，该中心显示出更多的热力学上有利的反应和可能更快的反应动力学。总体而言，已证明将尺寸减小至纳米级范围并生成反应性，亚稳态的中间体可改善金属硼氢化物纳米材料中的CO2吸收性能。

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  • 来源
    《Advanced Materials》 |2019年第44期|1904252.1-1904252.9|共9页
  • 作者

    Jeong Sohee; Milner Phillip J.; Wan Liwen F.; Liu Yi-Sheng; Oktawiec Julia; Zaia Edmond W.; Forse Alexander C.; Leick Noemi; Gennett Thomas; Guo Jinghua; Prendergast David; Long Jeffrey R.; Urban Jeffrey J.;

  • 作者单位

    Lawrence Berkeley Natl Lab Mol Foundry Berkeley CA 94720 USA;

    Univ Calif Berkeley Dept Chem Berkeley CA 94720 USA|Lawrence Berkeley Natl Lab Mat Sci Div Berkeley CA 94720 USA|Cornell Univ Dept Chem & Chem Biol Ithaca NY 14853 USA;

    Lawrence Berkeley Natl Lab Mol Foundry Berkeley CA 94720 USA|Lawrence Livermore Natl Lab Livermore CA 94550 USA;

    Lawrence Berkeley Natl Lab Adv Light Source Berkeley CA 94720 USA;

    Univ Calif Berkeley Dept Chem Berkeley CA 94720 USA|Lawrence Berkeley Natl Lab Mat Sci Div Berkeley CA 94720 USA;

    Univ Calif Berkeley Dept Chem Berkeley CA 94720 USA;

    Natl Renewable Energy Lab Colorado Colorado City CO 80401 USA;

    Natl Renewable Energy Lab Colorado Colorado City CO 80401 USA|Colorado Sch Mines Chem Dept 1012 14th St Golden CO 80401 USA;

    Lawrence Berkeley Natl Lab Adv Light Source Berkeley CA 94720 USA|Univ Calif Santa Cruz Dept Chem & Biochem Santa Cruz CA 95064 USA;

    Univ Calif Berkeley Dept Chem Berkeley CA 94720 USA|Lawrence Berkeley Natl Lab Mat Sci Div Berkeley CA 94720 USA|Univ Calif Berkeley Dept Chem & Biomol Engn Berkeley CA 94720 USA;

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  • 原文格式 PDF
  • 正文语种 eng
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  • 关键词

    carbon dioxide capture; kinetics; magnesium borohydride gamma phase (gamma-Mg(BH4)(2)); nanomaterials; reduced graphene oxide;

    机译：二氧化碳捕获动力学;硼氢化镁伽马相（γ-Mg（BH4）（2））;纳米材料还原氧化石墨烯;

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