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Control of Chemical Reaction Pathways by Light–Matter Coupling
Annual Review of Physical Chemistry ( IF 11.7 ) Pub Date : 2021-04-20 , DOI: 10.1146/annurev-physchem-090519-045502
Dinumol Devasia 1 , Ankita Das 1 , Varun Mohan 2 , Prashant K. Jain 1, 3
Affiliation  

Because plasmonic metal nanostructures combine strong light absorption with catalytically active surfaces, they have become platforms for the light-assisted catalysis of chemical reactions. The enhancement of reaction rates by plasmonic excitation has been extensively discussed. This review focuses on a less discussed aspect: the induction of new reaction pathways by light excitation. Through commentary on seminal reports, we describe the principles behind the optical modulation of chemical reactivity and selectivity on plasmonic metal nanostructures. Central to these phenomena are excited charge carriers generated by plasmonic excitation, which modify the energy landscape available to surface reactive species and unlock pathways not conventionally available in thermal catalysis. Photogenerated carriers can trigger bond dissociation or desorption in an adsorbate-selective manner, drive charge transfer and multielectron redox reactions, and generate radical intermediates. Through one or more of these mechanisms, a specific pathway becomes favored under light. By improved control over these mechanisms, light-assisted catalysis can be transformational for chemical synthesis and energy conversion.

中文翻译:


光-质耦合对化学反应途径的控制

由于等离激元金属纳米结构将强光吸收与催化活性表面结合在一起,因此它们已成为光辅助催化化学反应的平台。已经广泛地讨论了通过等离子体激元激发来提高反应速率。这篇评论集中在讨论较少的方面:通过光激发诱导新的反应途径。通过对开创性报告的评论,我们描述了对等离激元金属纳米结构的化学反应性和选择性进行光学调制的原理。这些现象的核心是由等离激元激发产生的激发电荷载流子,这些载流子改变了表面反应物种可用的能量格局,并解锁了热催化中常规不可用的途径。光生载流子可以以吸附物选择性方式触发键解离或解吸,驱动电荷转移和多电子氧化还原反应,并生成自由基中间体。通过这些机制中的一种或多种,​​特定的途径在光照下变得受宠。通过对这些机制的改进控制,光辅助催化可以转化为化学合成和能量转化。

更新日期:2021-04-21
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