首页> 外文期刊>Chemistry: A European journal >Systematic selection of metalloporphyrin-based catalysts for oxygen reduction by modulation of the donor-acceptor intermolecular hardness
【24h】

Systematic selection of metalloporphyrin-based catalysts for oxygen reduction by modulation of the donor-acceptor intermolecular hardness

机译:通过调节供体-受体分子间硬度来系统选择基于金属卟啉的催化剂进行氧还原

获取原文
获取原文并翻译 | 示例
           

摘要

Incisive modulation of the intermolecular hardness between metalloporphyrins and O_2 can lead to the identification of promising catalysts for oxygen reduction. The dependency of the electrocatalytic reduction of O_2 by metalloporphyrins on the nature of the central metal yields a volcano-type curve, which is rationalized to be in accordance with the Sabatier principle by using an approximation of the electrophilicity of the complexes. By using electrochemical and UV/Vis data, the influence of a selection of meso-substituents on the change in the energy for the π→π* excitation of manganese porphyrins was evaluated allowing one to quantitatively correlate the influence of the various ligands on the electrocatalysis of O_2 reduction by the complexes. A manganese porphyrin was identified that electrocatalyzes the reduction of oxygen at low overpotentials without generating hydrogen peroxide. The activity of the complex became remarkably enhanced upon its pyrolysis at 650 °C. Finding the strength: Incisive modulation of the intermolecular hardness between metalloporphyrins and O_2 can lead to the identification of promising catalysts for the oxygen reduction reaction (see figure). The feasibility of this principle is demonstrated in the selection and design of a manganese metalloporphyrin with promising high activity for electrocatalytic oxygen reduction.
机译:金属卟啉与O_2之间分子间硬度的精确调节可导致鉴定出有希望的氧还原催化剂。金属卟啉对O_2的电催化还原对中心金属性质的依赖性产生了火山型曲线,该曲线通过使用配合物的亲电性近似值,符合Sabatier原理。通过使用电化学和UV / Vis数据,评估了中取代基的选择对锰卟啉从π→π*激发的能量变化的影响,从而可以定量关联各种配体对电催化的影响。络合物还原O_2的能力鉴定出锰卟啉可在低超电势下催化氧的还原而不会产生过氧化氢。在650°C下热解后,复合物的活性显着增强。寻找强度:金属卟啉与O_2之间分子间硬度的精确调节可导致鉴定出有希望的氧还原反应催化剂(见图)。该原理的可行性在锰金属卟啉的选择和设计中得到了证明,该锰金属具有极高的电催化氧还原活性。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号