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Theoretical and Experimental Evidence for the Carbon-Oxygen Group Enhancement of NO Reduction

机译：碳氧基团增强NO还原的理论和实验证据

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摘要

The relation between a catalytic center and the surrounding carbon-oxygen groups influences the catalytic activity in various reactions. However, the impact of this relation on catalysis is usually discussed separately. For the first time, we proved that carbon-oxygen, groups increased the reducibility of Fe-C bonds toward NO reduction. Experimentally, we compared the reductive activities of Materials with either one or both factors, i.e., carbon-oXygen groups and Fe-C bonds. As a result, graphene oxide-supported Fe (with both factors) showed the best activity, duration of activity, and selectivity. This material reduced 100% of NO to N-2 at 300 degrees C. Moreover, theoretical calculations revealed that the adsorption energy of graphene for NO increased from -13.51 (physical adsorption) to -327.88 kJ/mol (chemical adsorption) after modification with Fe-C. When the graphene-supported Fe was further modified with carboxylic acid groups, the ability to transfer charge increased dramatically from 0.109 to 0:180 1e(-)vertical bar. Therefore, the carbon-oxygen groups increased the reducibility of Fe-C. The main results will contribute to the understanding of NO reduction and the design of effective catalysts.
机译：催化中心与周围的碳氧基团之间的关系影响各种反应中的催化活性。但是，这种关系对催化的影响通常单独讨论。我们首次证明了碳氧基团增加了Fe-C键向NO还原的还原性。在实验上，我们将材料的还原活性与一个或两个因素（即碳氧基团和Fe-C键）进行了比较。结果，氧化石墨烯负载的Fe（同时具有两个因素）显示出最佳的活性，活性持续时间和选择性。该材料在300摄氏度时将100％的NO还原为N-2。此外，理论计算表明，石墨烯对NO的吸附能从-13.51（物理吸附）增加至-327.88 kJ / mol（化学吸附）。铁碳当石墨烯负载的铁进一步用羧酸基团改性时，转移电荷的能力从0.109到0：180 1e（-）竖线急剧增加。因此，碳-氧基团增加了Fe-C的还原性。主要结果将有助于理解NO还原和有效催化剂的设计。

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  • 来源
    《Environmental Science & Technology》 |2017年第24期|14209-14216|共8页
  • 作者

    Li Jinyang; Wang Yirui; Song Jia; Gao Qi; Zhang Jia; Zhang Jingyi; Zhai Dong; Zhou Jizhi; Liu Qiang; Xu Zhi Ping; Qian Guangren; Liu Yi;

  • 作者单位

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Inst Mat Genome, 99 Shangda Rd, Shanghai 200111, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Inst Mat Genome, 99 Shangda Rd, Shanghai 200111, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Univ, Sch Environm & Chem Engn, SHU Ctr Green Urban Min & Ind Ecol, 333 Nanchen Rd, Shanghai 200411, Peoples R China;

    Shanghai Inst Mat Genome, 99 Shangda Rd, Shanghai 200111, Peoples 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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