Lee Seunghan, Bae Hyeonhu, Singh Amit, Hussain Tanveer, Kaewmaraya Thanayut, Lee Hoonkyung
Department of Physics, Konkuk University, Seoul 05029, Korea.
Department of Mechanical Engineering, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan.
ACS Omega. 2021 Oct 5;6(41):27045-27051. doi: 10.1021/acsomega.1c03599. eCollection 2021 Oct 19.
Recently, transition metal (TM)-porphyrin-like graphene has been predicted to be a promising material for CO capturing under favorable conditions. Such materials can capture CO at 300 K and release it at 450 K. However, the captured CO gas is mostly stored in oceans. With the aid of first principles calculations, we herein propose a method in which the captured CO is converted into an environmentally friendly product, formic acid. Addition of H to CO molecules adsorbed on Sc- and Ti-porphyrin-like graphene was found to catalyze this conversion. We also performed nudged elastic band calculations and thermodynamic analysis using the first-order Polanyi-Wigner equation and equilibrium statistical mechanics to investigate the chemical reactions involved in this conversion. In addition, we performed Bader charge analysis to obtain insights into the mechanism of charge transfer and adsorption throughout the conversion. Our study presents a novel method in which the captured CO is treated by converting it into an environmentally friendly product. Since this method does not require CO storage, it is expected to be an effective strategy to manage the rising CO level in the environment.
最近，有人预测过渡金属（TM）-卟啉类石墨烯在有利条件下是一种很有前景的二氧化碳捕获材料。这类材料能在300K下捕获二氧化碳，并在450K下释放。然而，捕获的二氧化碳气体大多存储在海洋中。借助第一性原理计算，我们在此提出一种方法，将捕获的二氧化碳转化为环境友好型产物甲酸。发现向吸附在Sc-和Ti-卟啉类石墨烯上的二氧化碳分子添加氢可催化这种转化。我们还使用一阶玻尔兹曼-维格纳方程和平衡统计力学进行了推挤弹性带计算和热力学分析，以研究这种转化过程中涉及的化学反应。此外，我们进行了巴德电荷分析，以深入了解整个转化过程中的电荷转移和吸附机制。我们的研究提出了一种新颖的方法，即通过将捕获的二氧化碳转化为环境友好型产物来进行处理。由于这种方法不需要存储二氧化碳，因此有望成为应对环境中不断上升的二氧化碳水平的有效策略。
