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Cooperative Coupling of Oxidative Organic Synthesis and Hydrogen Production over Semiconductor-Based Photocatalysts
Chemical Reviews ( IF 51.4 ) Pub Date : 2021-08-11 , DOI: 10.1021/acs.chemrev.1c00197 Ming-Yu Qi 1 , Marco Conte 2 , Masakazu Anpo 3 , Zi-Rong Tang 1 , Yi-Jun Xu 1
Chemical Reviews ( IF 51.4 ) Pub Date : 2021-08-11 , DOI: 10.1021/acs.chemrev.1c00197 Ming-Yu Qi 1 , Marco Conte 2 , Masakazu Anpo 3 , Zi-Rong Tang 1 , Yi-Jun Xu 1
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Merging hydrogen (H2) evolution with oxidative organic synthesis in a semiconductor-mediated photoredox reaction is extremely attractive because the clean H2 fuel and high-value chemicals can be coproduced under mild conditions using light as the sole energy input. Following this dual-functional photocatalytic strategy, a dreamlike reaction pathway for constructing C–C/C–X (X = C, N, O, S) bonds from abundant and readily available X–H bond-containing compounds with concomitant release of H2 can be readily fulfilled without the need of external chemical reagents, thus offering a green and fascinating organic synthetic strategy. In this review, we begin by presenting a concise overview on the general background of traditional photocatalytic H2 production and then focus on the fundamental principles of cooperative photoredox coupling of selective organic synthesis and H2 production by simultaneous utilization of photoexcited electrons and holes over semiconductor-based catalysts to meet the economic and sustainability goal. Thereafter, we put dedicated emphasis on recent key progress of cooperative photoredox coupling of H2 production and various selective organic transformations, including selective alcohol oxidation, selective methane conversion, amines oxidative coupling, oxidative cross-coupling, cyclic alkanes dehydrogenation, reforming of lignocellulosic biomass, and so on. Finally, the remaining challenges and future perspectives in this flourishing area have been critically discussed. It is anticipated that this review will provide enlightening guidance on the rational design of such dual-functional photoredox reaction system, thereby stimulating the development of economical and environmentally benign solar fuel generation and organic synthesis of value-added fine chemicals.
中文翻译：
半导体光催化剂上氧化有机合成与制氢的协同耦合
在半导体介导的光氧化还原反应中将析氢 (H 2 ) 与氧化有机合成结合起来极具吸引力，因为清洁的 H 2燃料和高价值化学品可以在温和的条件下使用光作为唯一的能量输入来共同生产。遵循这种双功能光催化策略，从丰富且易于获得的含 X-H 键的化合物中构建 C-C/C-X (X = C, N, O, S) 键的梦幻般的反应途径，同时释放 H 2无需外部化学试剂即可轻松实现，从而提供了一种绿色且引人入胜的有机合成策略。在这篇综述中，我们首先简要概述了传统光催化 H 2的一般背景然后专注于通过在半导体催化剂上同时利用光激发电子和空穴来实现选择性有机合成和 H 2生产的协同光氧化还原耦合的基本原理，以满足经济和可持续性目标。此后，我们重点介绍了H 2协同光氧化还原耦合的近期关键进展。生产和各种选择性有机转化，包括选择性醇氧化、选择性甲烷转化、胺类氧化偶联、氧化交叉偶联、环烷烃脱氢、木质纤维素生物质重整等。最后，批判性地讨论了这个蓬勃发展领域的剩余挑战和未来前景。预计该综述将为这种双功能光氧化还原反应体系的合理设计提供启发性指导，从而促进经济、环保的太阳能燃料发电和高附加值精细化学品的有机合成的发展。
更新日期：2021-08-11
中文翻译：
半导体光催化剂上氧化有机合成与制氢的协同耦合
在半导体介导的光氧化还原反应中将析氢 (H 2 ) 与氧化有机合成结合起来极具吸引力，因为清洁的 H 2燃料和高价值化学品可以在温和的条件下使用光作为唯一的能量输入来共同生产。遵循这种双功能光催化策略，从丰富且易于获得的含 X-H 键的化合物中构建 C-C/C-X (X = C, N, O, S) 键的梦幻般的反应途径，同时释放 H 2无需外部化学试剂即可轻松实现，从而提供了一种绿色且引人入胜的有机合成策略。在这篇综述中，我们首先简要概述了传统光催化 H 2的一般背景然后专注于通过在半导体催化剂上同时利用光激发电子和空穴来实现选择性有机合成和 H 2生产的协同光氧化还原耦合的基本原理，以满足经济和可持续性目标。此后，我们重点介绍了H 2协同光氧化还原耦合的近期关键进展。生产和各种选择性有机转化，包括选择性醇氧化、选择性甲烷转化、胺类氧化偶联、氧化交叉偶联、环烷烃脱氢、木质纤维素生物质重整等。最后，批判性地讨论了这个蓬勃发展领域的剩余挑战和未来前景。预计该综述将为这种双功能光氧化还原反应体系的合理设计提供启发性指导，从而促进经济、环保的太阳能燃料发电和高附加值精细化学品的有机合成的发展。
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