First-Principles Study of Electrocatalytically Reversible CO2 Capture on Graphene-like C3N
First-Principles Study of Electrocatalytically Reversible CO2 Capture on Graphene-like C3N
复制标题
类石墨烯 C3N 电催化可逆 CO2 捕获的第一性原理研究
DOI：
10.1002/cphc.201800385
复制
发表时间：
2018-10-19
期刊：
影响因子：
2.9
通讯作者：
Sun, Qiao
中科院分区：
文献类型：
--
作者：
Qin, Gangqiang;Cui, Qianyi;Sun, Qiao
开发先进的材料和新技术来有效地捕获和分离二氧化碳，可以极大地减轻其对全球气候变化的影响。在这项研究中，我们报告了一个全面的密度泛函理论研究的N-2，CH 4，H-2，和CO2吸附在石墨烯类C3N单层。计算结果表明，这四种气体分子都被物理吸附在中性C3N单分子膜上。然而，通过电化学方法的策略，如引入负电荷或施加外电场，可以显着促进CO2和C3N之间的相互作用。而N-2、CH4和H-2在C3N单分子膜上的吸附受上述策略的影响较小。此外，一旦从系统中去除额外的电荷或电场，CO2将从C3N单层自发释放。这些结果表明，CO2的捕获，再生和分离的C3N单分子膜上可以控制的方法来切换/关闭的电荷状态或电场在吸附过程中。此外，作为一种新合成的2D材料（PNAS，2016，113，7414 - 7419），C3N具有0.39eV的极窄带隙，这保证了通过电化学方法在实验中可以容易地实现向其施加负电荷或电场。
Developing advanced materials and new technologies for efficient CO2 capture and gas separation can enormously alleviate its impact on global climate change. In this study, we report a comprehensive density functional theory investigation of N-2, CH4, H-2, and CO2 adsorption on a graphene-like C3N monolayer. Our calculation results show that the four gas molecules are all physisorbed on the neutral C3N monolayer. However, the interaction between CO2 and C3N can be significantly boosted via the strategies of electrochemical methods such as introducing negative charge or applying external electric field to the system. While the adsorption of N-2, CH4 and H-2 on C3N monolayer is slightly influenced with the above strategies. Moreover, CO2 will release spontaneously from C3N monolayer once the extra charge or electric field is removed from the system. These results demonstrate that the CO2 capture, regeneration and separation on C3N monolayer can be controllable with the method of switching on/off the charge state or electric field during the adsorption. In addition, as a new synthesized 2D material (PNAS, 2016, 113, 7414-7419), C3N possesses an extremely narrow band gap of 0.39eV, which guarantees applying negative charge or electric field to it can be easily realized in experiment by electrochemical methods.