Advances in the Molecular Catalysis of Dioxygen Reduction
Advances in the Molecular Catalysis of Dioxygen Reduction
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DOI：
10.1021/acscatal.9b04477
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发表时间：
2020-02-21
期刊：
影响因子：
12.9
通讯作者：
Machan, Charles W.
中科院分区：
文献类型：
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作者：
Machan, Charles W.
氧(O-2)的还原在能量相关反应中起着至关重要的作用。在生物学中，呼吸作用使用O-2还原作为热力学下沉，而燃料电池将氧还原反应(ORR)配对为与化学燃料氧化的质子相关的半反应。由分子无机物种介导的催化ORR过程作为多相体系的模型继续引起人们的兴趣。根据所提出的反应机理直接观察、量化和合成相关中间体的能力使得分子物种相对于多相体系的纳米和介观形态中的活性中心的分布很容易被优化。下一代阴极材料的发展将取代铂(铂)用于ORR，这将需要改进对O-2作为衬底的基本理解，而明确定义的均匀系统是唯一能够提供这种理解的。这一观点总结了均相催化O-2还原领域的最新进展，特别强调了在机理理解的帮助下，活性和选择性的提高。
The reduction of dioxygen (O-2) is of vital importance to energy-related reactions. In biology, respiration uses O-2 reduction as a thermodynamic sink, whereas fuel cells pair the oxygen reduction reaction (ORR) to H2O as a proton dependent half-reaction to the oxidation of chemical fuels. Catalytic ORR processes mediated by molecular inorganic species continue to garner interest as models for heterogeneous systems. The ability to directly observe, quantify, and synthesize relevant intermediates from proposed reaction mechanisms renders molecular species readily optimizable, relative to the distribution of active sites within the nanoscale and mesoscale morphologies of heterogeneous systems. The development of next-generation cathode materials to displace platinum (Pt) for ORR will require improvements in the fundamental understanding of how O-2 behaves as a substrate, which well-defined homogeneous systems are uniquely positioned to provide. This Perspective provides a summary of recent advances in the area of homogeneous catalytic O-2 reduction, with a particular emphasis on improvements in activity and selectivity aided by mechanistic understanding.