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

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL
Atsu Kludze, Lucas Bertucci, Saumya Gulati, Shu Hu
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Abstract

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

多相光催化的机会:量子效率增强,选择性控制和规模扩大
光催化是一种光驱动的化学转化过程,是一种很有前途的替代能源密集型热驱动催化系统的方法。然而,目前的光催化系统的化学吞吐量明显低于热驱动系统,这限制了它们的商业可行性。虽然在提高光催化活性和效率方面取得了实质性进展,但对现有光催化剂设计框架的重新评估对于进一步发展至关重要。这一观点的目的是扩大目前的框架,通过考虑产品选择性,催化系统的关键性能指标。我们首先分析光催化水分解,这是一个具有挑战性的反应,指导了当前的设计策略,强调调整带边能量学和载流子动力学,并探索其作为其他光催化反应模型的潜在应用。然后,我们研究了光生成反应性中间体的作用,使用光催化生成活性氧来证明如何调整反应性中间体以提高选择性并实现新的化学途径。接下来,我们研究了光催化无受体醇脱氢的反应机理,以证明如何设计光催化剂表面相互作用来促进反应并提高选择性。基于这些见解,我们建议战略性地使用薄膜涂层来提高稳定性和选择性。最后,我们简要概述了光反应器设计考虑因素,这些因素对于开发放大光反应器或光催化转化装置至关重要。通过讨论这些策略,本观点旨在提供一个框架来推进光催化系统的发展,重点是优化控制光催化反应的关键过程。图形抽象
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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