摘要/Abstract

CO₂是大气中主要温室气体之一，也是丰富、可再生的C₁资源，将CO₂转化为有价值的化学品不仅能缓解化学工业对化石资源的依赖，还能有效减少CO₂排放.然而，CO₂内在的热力学稳定性和动力学惰性，决定了CO₂的活化及合理转化路线的开发是其成功转化的关键.18年来，何良年课题组在CO₂转化策略的设计和基于活化机理的高效催化剂开发方面做了系统的工作，不仅提出了碳捕集与转化偶合、CO₂分级可控还原功能化、利用多组分串联反应突破热力学限制及光促进的CO₂转化等策略，还针对不同的策略开发出了相应的高效催化体系，实现了温和条件下CO₂的转化.基于何良年课题组工作对可持续发展的二氧化碳化学进行概述，希望能为同行提供有益借鉴，进一步推动CO₂化学的的应用与发展.
关键词: 二氧化碳, 捕集, 转化, 还原, 串联反应, 光催化, 可持续化学, 合成方法
Climate change and depletion of fossil fuels have drawn considerable attention. Considering carbon dioxide is both the dominant greenhouse gas and renewable C₁ source, CO₂ valorization into valuable chemicals is considered to reconcile the environment benefit and sustainable chemistry development. Unfortunately, the thermodynamic stability and kinetic inertness of CO₂ make its chemical transformation challenging. As a consequence, developing highly efficient catalytic systems and synthetic protocols is crucial for CO₂ conversion. In recent years, He's group made great progress on strategy design and catalyst development for CO₂ conversion. A series novel CO₂ conversion strategies are proposed, including CO₂ capture and in-situ transformation, hierarchical reductive functionalization of CO₂, designing thermodynamically favorable reactions by multi-component cascade reaction and photo-promoted CO₂ transformation. Concurrently, the corresponding highly efficient catalytic systems were also developed based on the reaction mechanism and thus CO₂ transformation was successfully performed under mild conditions. It is hoped that this review can arouse broad concern on CO₂ transformation and spur its further development.
Key words: carbon dioxide, capture, transformation, reduction, cascade reaction, photocatalysis, sustainable chemistry, synthetic method


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