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Scalable and green juglone synthesis via heterogeneous photocatalysis in a photomicroreactor
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2024-08-05 , DOI: 10.1039/d4cy00778f Mohsin Pasha 1 , Yuhan Wang 1 , You Ma 1 , Guozhi Qian 1 , Xiao Xue 1 , Hong Zhang 2 , Yong Yang 3 , Minjing Shang 1 , Pengfei Zhang 4 , Yuanhai Su 1, 4
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2024-08-05 , DOI: 10.1039/d4cy00778f Mohsin Pasha 1 , Yuhan Wang 1 , You Ma 1 , Guozhi Qian 1 , Xiao Xue 1 , Hong Zhang 2 , Yong Yang 3 , Minjing Shang 1 , Pengfei Zhang 4 , Yuanhai Su 1, 4
Affiliation
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The selection of green and scalable heterogeneous photocatalysis is always a great dilemma for the chemistry and chemical engineering communities. In this report, we resolved this vital conundrum by synergistically examining the scalability and green potential of heterogeneous photocatalysis for juglone synthesis. We scaled up juglone productivity and the space–time yield to 15 g per day and 43.87 g L−1 h−1, respectively, via heterogeneous photocatalysis with a high-power LED as a light source and Amb–m-TcPP as a photocatalyst, which was fabricated by incorporating meso-tetracarboxyphenylporphyrine (m-TcPP) over the polystyrene ion-exchange resin Amberlyst-15. Amb–m-TcPP showed excellent recyclability in multiple cycles and exhibited high photostability for 12 h continuous operation without m-TcPP leaching with a turnover frequency of 409.7 h−1. The apparent rate constants were higher than those in previously employed heterogeneous photocatalysis, and intrinsic rate constants of intermediate steps were evaluated using transition state theory with quantum mechanical models using DFT simulations, which was useful for gaining mechanistic insights into this photooxidation process. Finally, heterogeneous DHN photooxidation was confirmed to be well aligned with green chemistry principles, and E factors were found to be under an acceptable range. Thus, this heterogeneous DHN photooxidation can be regarded as a green and sustainable synthesis route for multigram juglone production.
中文翻译:
在光微反应器中通过异相光催化合成可扩展的绿色胡桃醌
选择绿色且可扩展的多相光催化一直是化学和化学工程界面临的一大难题。在本报告中,我们通过协同检查胡桃醌合成的异质光催化的可扩展性和绿色潜力,解决了这一重要难题。我们通过以高功率 LED 作为光源和 Amb– m -TcPP 作为光催化剂的异相光催化,将胡桃醌生产率和时空产量分别提高到 15 g / 天和 43.87 g L -1 h -1 。 ,它是通过在聚苯乙烯离子交换树脂 Amberlyst-15 上掺入内消旋四羧基苯基卟啉 ( m -TcPP) 制成的。 Amb- m -TcPP 在多次循环中表现出优异的可回收性,并且连续运行 12 小时表现出高光稳定性,没有m -TcPP 浸出,周转频率为 409.7 h -1 。表观速率常数高于以前采用的多相光催化,并且使用过渡态理论和使用DFT模拟的量子力学模型评估了中间步骤的固有速率常数,这对于获得对该光氧化过程的机械见解非常有用。最后,多相 DHN 光氧化被证实符合绿色化学原理,并且E因子处于可接受的范围内。因此,这种异质DHN光氧化可以被视为多克胡桃醌生产的绿色且可持续的合成路线。
更新日期:2024-08-05
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
在光微反应器中通过异相光催化合成可扩展的绿色胡桃醌
选择绿色且可扩展的多相光催化一直是化学和化学工程界面临的一大难题。在本报告中,我们通过协同检查胡桃醌合成的异质光催化的可扩展性和绿色潜力,解决了这一重要难题。我们通过以高功率 LED 作为光源和 Amb– m -TcPP 作为光催化剂的异相光催化,将胡桃醌生产率和时空产量分别提高到 15 g / 天和 43.87 g L -1 h -1 。 ,它是通过在聚苯乙烯离子交换树脂 Amberlyst-15 上掺入内消旋四羧基苯基卟啉 ( m -TcPP) 制成的。 Amb- m -TcPP 在多次循环中表现出优异的可回收性,并且连续运行 12 小时表现出高光稳定性,没有m -TcPP 浸出,周转频率为 409.7 h -1 。表观速率常数高于以前采用的多相光催化,并且使用过渡态理论和使用DFT模拟的量子力学模型评估了中间步骤的固有速率常数,这对于获得对该光氧化过程的机械见解非常有用。最后,多相 DHN 光氧化被证实符合绿色化学原理,并且E因子处于可接受的范围内。因此,这种异质DHN光氧化可以被视为多克胡桃醌生产的绿色且可持续的合成路线。