Abstract There are increasing concerns about the environmental impact of rising atmospheric carbon dioxide (CO2) concentrations, thus it is necessary to develop new materials and technologies for efficient CO2 capture and conversion. In this work, we investigated CO2 capture on different metal embedded graphynes (M-GYs) under different charge states via density functional theory (DFT) calculations. It was found that the neutral Ti, V, Cr and Mn embedded GYs could effectively capture CO2 molecules, and the adsorption energy of CO2 was dramatically enhanced on negatively charged M-GYs. The process of CO2 capture/release on Fe or Co embedded GY occurs spontaneously once extra electrons are introduced/removed. Therefore, Fe- and Co-GYs are promising materials for reversible efficient CO2 storage. Ti-GY has the largest CO2 adsorption capacity. By comparing the adsorption of CO2 by non-noble metals and noble metals, it is found that non-noble metals are more conducive to large-scale practical application for CO2 capture due to their high sensitivity to CO2 and low cost. This investigation provides valuable information for designing reusable CO2 storage materials.

中文翻译：

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金属原子嵌入石墨炔的电荷调节 CO2 捕获能力：第一性原理研究

摘要 人们越来越关注大气中二氧化碳 (CO2) 浓度升高对环境的影响，因此有必要开发新的材料和技术来有效地捕获和转化 CO2。在这项工作中，我们通过密度泛函理论 (DFT) 计算研究了不同电荷状态下不同金属嵌入石墨烯 (M-GY) 上的 CO2 捕获。发现中性 Ti、V、Cr 和 Mn 嵌入的 GYs 可以有效地捕获 CO2 分子，并且 CO2 的吸附能在带负电荷的 M-GYs 上显着增强。一旦引入/移除额外的电子，嵌入 Fe 或 Co 的 GY 上的 CO2 捕获/释放过程就会自发发生。因此，Fe-GYs 和 Co-GYs 是可逆高效 CO2 储存的有前途的材料。Ti-GY 具有最大的 CO2 吸附能力。通过比较非贵金属和贵金属对CO2的吸附，发现非贵金属对CO2的敏感性高、成本低，更有利于CO2捕集的大规模实际应用。这项调查为设计可重复使用的 CO2 储存材料提供了宝贵的信息。