<p>Photocatalysis, a light-driven chemical conversion process, is a promising alternative to energy-intensive, heat-driven catalytic systems. However, current photocatalytic systems have significantly lower chemical throughput than their heat-driven counterparts, which limits their commercial viability. While substantial progress has been made improving photocatalytic activity and efficiency, a reassessment of the existing photocatalyst design framework is essential for further advancement. This perspective aims to broaden the current framework by considering product selectivity, a critical performance metric in catalytic systems. We begin by analyzing photocatalytic water splitting, a challenging reaction that has guided current design strategies to emphasize tuning band-edge energetics and charge carrier dynamics, and explore its potential application as a model for other photocatalytic reactions. We then examine the role of photogenerated reactive intermediates, using the photocatalytic generation of reactive oxygen species to demonstrate how reactive intermediates can be tuned to enhance selectivity and enable new chemical pathways. Next, we examine the reaction mechanism of photocatalytic acceptorless alcohol dehydrogenation to demonstrate how photocatalyst surface interactions can be engineered to facilitate the reaction and enhance selectivity. Building upon these insights, we propose the strategic use of thin-film coatings to enhance stability and selectivity. Lastly, we briefly outline photoreactor design considerations that are crucial to develop scaled-up photoreactors or photocatalytic conversion devices. By discussing these strategies, this perspective aims to provide a framework to advance the development of photocatalytic systems, focusing on optimizing key processes that govern photocatalytic reactions.</p> Graphical Abstract

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Opportunities for Heterogeneous Photocatalysis: Quantum Efficiency Enhancement, Selectivity Control, and Scale Up

  • Atsu Kludze,
  • Lucas Bertucci,
  • Saumya Gulati,
  • Shu Hu

摘要

Photocatalysis, a light-driven chemical conversion process, is a promising alternative to energy-intensive, heat-driven catalytic systems. However, current photocatalytic systems have significantly lower chemical throughput than their heat-driven counterparts, which limits their commercial viability. While substantial progress has been made improving photocatalytic activity and efficiency, a reassessment of the existing photocatalyst design framework is essential for further advancement. This perspective aims to broaden the current framework by considering product selectivity, a critical performance metric in catalytic systems. We begin by analyzing photocatalytic water splitting, a challenging reaction that has guided current design strategies to emphasize tuning band-edge energetics and charge carrier dynamics, and explore its potential application as a model for other photocatalytic reactions. We then examine the role of photogenerated reactive intermediates, using the photocatalytic generation of reactive oxygen species to demonstrate how reactive intermediates can be tuned to enhance selectivity and enable new chemical pathways. Next, we examine the reaction mechanism of photocatalytic acceptorless alcohol dehydrogenation to demonstrate how photocatalyst surface interactions can be engineered to facilitate the reaction and enhance selectivity. Building upon these insights, we propose the strategic use of thin-film coatings to enhance stability and selectivity. Lastly, we briefly outline photoreactor design considerations that are crucial to develop scaled-up photoreactors or photocatalytic conversion devices. By discussing these strategies, this perspective aims to provide a framework to advance the development of photocatalytic systems, focusing on optimizing key processes that govern photocatalytic reactions.

Graphical Abstract