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首页> 外文期刊>Environmental Science & Technology >Deciphering Visible Light Photoreductive Conversion of CO_2 to Formic Acid and Methanol Using Waste Prepared Material
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Deciphering Visible Light Photoreductive Conversion of CO_2 to Formic Acid and Methanol Using Waste Prepared Material

机译:使用废旧材料破译可见光将CO_2还原为甲酸和甲醇的光还原

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摘要

As gradual increases in atmospheric CO_2 and depletion of fossil fuels have raised considerable public concern in recent decades, utilizing the unlimited solar energy to convert CO_2 to fuels (e.g., formic acid and methanol) apparently could simultaneously resolve these issues for sustainable development. However, due to the complicated characteristics of CO_2 reduction, the mechanism has yet to be disclosed. To clarify the postulated pathway as mentioned in the literature, the technique of electron paramagnetic resonance (ESR) was implemented herein to confirm the mechanism and related pathways of CO_2 reduction under visible light using graphene- TiO_2 as catalyst. The findings indicated that CO~(-·) radicals, as the main intermediates, were first detected herein to react with several hydrogen ions and electrons for the formation of CH_3OH. For example, the generation of CO~(-·) radicals is possibly the vital rate-controlling step for conversion of CO_2 to methanol as hypothesized elsewhere. The kinetics behind the proposed mechanism was also determined in this study. The mechanism and kinetics could provide the in-depth understanding to the pathway of CO_2 reduction and disclose system optimization of maximal conversion for further application.
机译:近几十年来,随着大气中CO_2的逐渐增加和化石燃料的枯竭引起了公众的广泛关注,利用无限的太阳能将CO_2转化为燃料(例如甲酸和甲醇)显然可以同时解决这些问题,以实现可持续发展。但是,由于CO 2还原的复杂特性,其机理尚未公开。为了弄清文献中提到的假定途径,本文实施了电子顺磁共振技术(ESR),以确认使用石墨烯-TiO_2作为催化剂在可见光下CO_2还原的机理和相关途径。研究结果表明,本文首先检测到CO〜(-)自由基作为主要中间体,与几个氢离子和电子反应形成CH_3OH。例如,CO _(-·)自由基的产生可能是将CO_2转化为甲醇的重要速率控制步骤,如在其他地方假设的那样。在这项研究中还确定了所提出机制背后的动力学。该机理和动力学可以提供对CO 2还原途径的深入了解,并公开最大转化率的系统优化以供进一步应用。

著录项

  • 来源
    《Environmental Science & Technology》 |2015年第4期|2405-2417|共13页
  • 作者单位

    Institute of Environmental Engineering, National Taiwan University, Taipei, 106, Taiwan;

    Institute of Environmental Engineering, National Taiwan University, Taipei, 106, Taiwan;

    Department of Chemical and Materials Engineering, National Ⅰ-Lan University, Ilan, 260, Taiwan;

    College of the Environment and Ecology, Xiamen University, South Road of Xiangan, Xiamen City, 361102 Fujian, China;

    Department of Environmental Engineering, National Ⅰ-Lan University, Ilan, 260, Taiwan;

  • 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
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