Liu Xing, Cheng Bin, Hu Jifan
Jinan Engineering Polytechnic, Jinan 250200, China.
School of Physics, State Key Laboratory for Crystal Materials, Shandong University, Jinan 250100, China.
Phys Chem Chem Phys. 2024 Aug 28;26(34):22582-22592. doi: 10.1039/d4cp02461c.
This work employed density functional theory (DFT) to further study the adsorption of HCO, HCO, and CO on the CaSiO(001) surface, which could provide additional insights into the mechanism of carbonation on the CaSiO surface. It was concluded that the carbonation of CO promoted carbon sequestration, whereby the aqueous carbonation route increased the reaction rate substantially compared to direct gas-solid carbonation. HCO is more conducive to CO sequestration, which can be attributed to the interaction of H atoms with the surface. Further, HCO can be converted into HCO or CO on the CaO-terminated (001) surface, whereas only HCO was formed on the SiO-terminated (001) surface. All the adsorption energies of HCO were negative, suggesting that HCO adsorption was energetically stable and spontaneous. The most likely adsorption model of HCO, having negative adsorption energy, was the one adsorbed on the SiO-terminated (001) surface, in which HCO is transformed into CO. The other adsorption models of HCO and all the adsorption models of CO have positive adsorption energies. Considering the adsorption process of HCO, HCO and CO adsorption reactions may occur successively to some extent depending on the environment.
本工作采用密度泛函理论（DFT）进一步研究了HCO、HCO和CO在CaSiO(001)表面的吸附情况，这可为深入了解CaSiO表面碳酸化机理提供更多见解。研究得出结论，CO的碳酸化促进了碳封存，与直接气固碳酸化相比，水相碳酸化途径显著提高了反应速率。HCO更有利于CO封存，这可归因于H原子与表面的相互作用。此外，HCO在CaO端接的(001)表面可转化为HCO或CO，而在SiO端接的(001)表面仅形成HCO。HCO的所有吸附能均为负值，表明HCO吸附在能量上是稳定且自发的。具有负吸附能的HCO最可能的吸附模型是吸附在SiO端接的(001)表面，其中HCO转化为CO。HCO的其他吸附模型以及CO的所有吸附模型均具有正吸附能。考虑到HCO的吸附过程，HCO、HCO和CO的吸附反应可能会根据环境在一定程度上相继发生。
