苄基二硫化物，-二硒化物和-二碲化物捕获和释放二氧化碳的密度泛函理论研究,The Journal of Physical Chemistry A

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苄基二硫化物，-二硒化物和-二碲化物捕获和释放二氧化碳的密度泛函理论研究
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2019-03-25 00:00:00 , DOI: 10.1021/acs.jpca.9b01862
Derek Harris ₁ , Eric Bushnell ₁

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我们大气中CO ₂浓度的上升及其对气候变化的贡献是地球面临的最大问题之一。过去的实验工作表明，苄基二硫键可逆地结合CO _2的能力。在目前的工作中，使用密度泛函理论方法将苄基-二硒化物和苄基-二碲化物可逆结合CO ₂的能力与苄基-二硫化物的能力进行了比较。还研究了溶剂极性对捕获CO ₂的热力学的影响。从结果中发现，苄基二碲化物为CO ₂捕获和释放提供了最大的热中性途径，而苄基二硫化物为CO ₂提供了最少的热中性途径。捕获。据说步骤之间的这种热中性是碳捕获和存储（CCS）技术的重要属性。关于CO ₂捕集的各个步骤，在目前的理论水平上发现，在还原苄基二卤化碳化合物后，形成的BnX ^–化合物通过无障碍过程与CO ₂结合，因此有望有效捕获CO _2个。此外，由于在电子转移步骤中结构和电子变化相似，因此在所研究的化合物中，电子转移步骤的动力学预计相似。因此，本文提出的结果表明，应研究BnTe-TeBn和BnSe-SeBn作为CCS技术的潜在用途。

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Density Functional Theory Study of the Capture and Release of Carbon Dioxide by Benzyl–Disulfide, −Diselenide, and −Ditelluride

Rising levels of CO₂ concentration in our atmosphere and its contribution to climate change are one of the greatest issues our planet is facing. Past experimental work has shown the ability of benzyl–disulfide to reversibly bind CO₂. In the present work, the ability of benzyl–diselenide and benzyl–ditelluride to reversibly bind CO₂ was compared to that of benzyl–disulfide using a density functional theory approach. The effect of solvent polarity on the thermodynamics of CO₂ capture was also investigated. From the results it was found that benzyl–ditelluride offered the most thermoneutral pathway for CO₂ capture and release, whereas benzyl–disulfide offered the least thermoneutral pathway for CO₂ capture. Such thermoneutrality between steps has been stated to be an important property of carbon capture and storage (CCS) technologies. Regarding the various steps involved in CO₂ capture, it was found at the present level of theory that after reduction of the benzyl–dichalcogenide compounds, the formed BnX^– compounds bind to CO₂ via a barrierless process and are therefore expected to efficiently capture CO₂. Moreover, given the similar structural and electronic changes during the electron transfer steps, the kinetics of the electron transfer steps are expected to be similar among the compounds investigated. Thus, the results presented herein suggest that BnTe–TeBn and BnSe–SeBn should be investigated for potential use as CCS technologies.

更新日期：2019-03-25

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