光驱动的C–H键活化和以CO2作为碳捕获和利用技术的原料建立C–C键的最新进展,Green Chemistry

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光驱动的C–H键活化和以CO2作为碳捕获和利用技术的原料建立C–C键的最新进展
Green Chemistry ( IF 9.3 ) Pub Date : 2020-09-04 , DOI: 10.1039/d0gc01796e
Takayuki Katagiri _{1,

2,

3,

4} , Yutaka Amao _{1,

2,

3,

4,

5}

Affiliation

CO ₂是一种代表性的温室气体（GHG），2015年12月12日以协商一致方式通过的《巴黎协定》规定，到2050年年底，与2013年相比，全球将CO ₂排放量减少80％。在CO _2中，不仅需要建立CO ₂捕集与封存（CCS），还需要建立广泛的技术，例如将CO ₂转化为甲醇等醇类燃料，用作化学原料等（CO ₂捕获和利用CCU）。建立旨在减少CO ₂的利用技术将有助于“ 7。使用可再生原料”和“ 9。催化剂”来自绿色化学的12条原则。CO ₂利用技术可分为两类：具有多个质子的多电子还原和与有机分子的结合。在前一种情况下，会生成CO，甲酸和甲醇，因此未观察到目标产物的碳数增加。在后一种情况下，CO ₂作为羧基键合到有机分子上，因此可以重新建立C–C键。换句话说，利用后一种技术，可以固定CO _2。有机分子并创造新的功能材料。例如，自然光合作用巧妙地利用阳光作为可再生能源和酶催化剂，以CO ₂和水为原料合成葡萄糖。换句话说，基于模拟自然光合作用的CCU技术有助于上述绿色化学原理。为了建立该技术，促进CO ₂与有机分子结合的催化剂是必不可少的因素。换句话说，有必要开发一种催化剂来激活有机分子中的C–H键并促进与CO _2的C–C键形成。在这篇综述中，分子式和基于酶的催化剂可用于C–H键活化以及与CO ₂建立C–C键介绍了适用于使用光氧化还原系统的光驱动CCU的方法。此外，还介绍了光驱动的C–H键活化和使用各种催化剂和光功能材料与CO ₂建立C–C键的方法。还讨论了两个系统的C–H键活化和用CO ₂建立C–C键的反应产率和选择性。最后，我们讨论了光驱动的C–H键活化和与CO ₂建立C–C键的问题，并提到了未来需要改进的地方。我们还讨论了光驱动C–H键活化和使用CO ₂建立C–C键的典型系统的生命周期评估（LCA）的概述。

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Recent advances in light-driven C–H bond activation and building C–C bonds with CO2 as a feedstock for carbon capture and utilization technology

CO₂ is a representative greenhouse gas (GHG), and the Paris Agreement adopted by consensus on 12 December 2015 mandates worldwide reduction of CO₂ emissions by 80% until the end of 2050 relative to that of 2013. In order to achieve a significant reduction in CO₂, it is necessary to establish not only CO₂ capture and storage (CCS), but also a wide range of technologies such as CO₂ conversion to alcohol fuels such as methanol, utilization as chemical raw materials, and so on (CO₂ capture and utilization CCU). The establishment of utilization technology aimed at reducing CO₂ will contribute to “7. Use of renewable feedstocks” and “9. Catalyst” from the 12 principles of green chemistry. CO₂ utilization technology can be divided into two categories: multi-electron reduction with multiple protons and binding to organic molecules. In the former case, CO, formic acid, and methanol are produced, so no extension of the carbon number of the target product is observed. In the latter case, CO₂ is bonded to the organic molecule as a carboxyl group, so that a C–C bond can be newly built. In other words, with the latter technology, it becomes possible to fix CO₂ to organic molecules and create new functional materials. For example, natural photosynthesis skilfully utilizes sunlight as a renewable energy and enzyme catalysts to synthesize glucose from CO₂ and water as a raw material. In other words, CCU technology based on mimicking natural photosynthesis contributes to the above principles of green chemistry. To establish this technology, a catalyst that promotes the binding of CO₂ to organic molecules is an essential factor. In other words, it is necessary to develop a catalyst for activating C–H bonds in organic molecules and promoting C–C bond formation with CO₂. In this review, molecular and enzyme-based catalysts for C–H bond activation and building C–C bonds with CO₂ applicable to light-driven CCU using a photoredox system are introduced. Moreover, light-driven C–H bond activation and building C–C bonds with CO₂ using various catalysts and photofunctional materials are also introduced. The reaction yield and selectivity of both systems for C–H bond activation and building C–C bonds with CO₂ are also discussed. Finally, we discussed the problems of the light-driven C–H bond activation and building C–C bonds with CO₂ and mentioned some areas for improvement in the future. We also discussed the outline of the life cycle assessment (LCA) of a typical system for light-driven C–H bond activation and building C–C bonds with CO₂.

更新日期：2020-10-19

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