Electrochemical conversion of CO2 and water to valuable chemicals and fuels is one of the promising alternatives to replace fossil fuel-based processes in realizing a carbon–neutral cycle. For practical application of such technologies, suppressing hydrogen evolution reaction and facilitating the activation of stable CO2 molecules still remain major challenges. Furthermore, high production selectivity toward high-value chemicals such as ethylene, ethanol, and even n-propanol is also not easy task to achieve. To settle these challenges, deeper understanding on underlying basis of reactions such as how intermediate binding affinities can be engineered at catalyst surfaces need to be discussed. In this review, we briefly outline recent strategies to modulate the binding energies of key intermediates for CO2 reduction reactions, based on theoretical insights from density functional theory calculation studies. In addition, important design principles of catalysts and electrolytes are also provided, which would contribute to the development of highly active catalysts for CO2 electroreduction.

中文翻译：

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二氧化碳选择性电化学转化的理论见解。

将二氧化碳和水电化学转化为有价值的化学品和燃料是替代基于化石燃料的过程以实现碳中和循环的有前途的替代方案之一。对于此类技术的实际应用，抑制析氢反应并促进稳定CO2分子的活化仍然是主要挑战。此外，对乙烯、乙醇甚至正丙醇等高价值化学品的高生产选择性也并非易事。为了解决这些挑战，需要讨论对反应基础的更深入理解，例如如何在催化剂表面设计中间结合亲和力。在这篇综述中，我们基于密度泛函理论计算研究的理论见解，简要概述了调节二氧化碳还原反应关键中间体结合能的最新策略。此外，还提供了催化剂和电解质的重要设计原理，这将有助于开发用于CO2电还原的高活性催化剂。