Zeolite-templated carbons as effective sorbents to remove methylsiloxanes and derivatives: A computational screening
Zeolite-templated carbons as effective sorbents to remove methylsiloxanes and derivatives: A computational screening
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DOI：
10.1016/j.gee.2020.07.007
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发表时间：
2020-07
影响因子：
13.3
通讯作者：
Shiru Lin;Kaitlyn A. Jacoby;Jinxing Gu;Dariana R. Vega-Santander;A. J. Hernández-Maldonado;Zhongfang Chen
中科院分区：
文献类型：
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作者：
Shiru Lin;Kaitlyn A. Jacoby;Jinxing Gu;Dariana R. Vega-Santander;A. J. Hernández-Maldonado;Zhongfang Chen
虽然在我们的日常生活中广泛使用，但挥发性甲基硅氧烷及其衍生物正在成为新的污染物，并成为高度优先的环境和公共卫生问题。开发有效的吸附剂材料可以以具有成本效益的方式去除硅氧烷。在此，通过大典范蒙特卡罗（GCMC）模拟，我们评估了最近提出的68种稳定的沸石模板碳（ZTC）（PNAS 2018，115，E8116-E8124）去除四种线性甲基硅氧烷及其衍生物的潜力。通过计算的平均负载量和平均吸附能值，以及两种环状甲基硅氧烷。四种ZTC，即ISV，FAU 1，FAU 3和H8326836，被鉴定为对所有六种目标污染物具有前50%的吸附性能，其优于活性炭。进一步的第一性原理计算表明，空间位阻，静电相互作用（进一步增强的电荷转移），和CH-π相互作用占这些ZTC的出色的吸附性能。这项工作提供了一种快速程序，可以通过计算筛选有希望去除硅氧烷的ZTC，并帮助指导未来的实验和理论研究。
Though widely used in our daily lives, volatile methylsiloxanes and derivatives are emerging contaminants and becoming a high-priority environment and public health concern. Developing effective sorbent materials can remove siloxanes in a cost-effective manner. Herein, by means of Grand Canonical Monte Carlo (GCMC) simulations, we evaluated the potentials of the recently proposed 68 stable zeolite-templated carbons (ZTCs) (PNAS2018,115, E8116-E8124) for the removal of four linear methylsiloxanes and derivatives as well as two cyclic methylsiloxanes by the calculated average loading and average adsorption energy values. Four ZTCs, namely ISV, FAU1, FAU3, and H8326836, were identified with the top 50% adsorption performance toward all the six targeted contaminants, which outperform activated carbons. Further first principles computations revealed that steric hindrance, electrostatic interactions (further enhanced by charge transfer), and CH-π interactions account for the outstanding adsorption performance of these ZTCs. This work provides a quick procedure to computationally screen promising ZTCs for siloxane removal, and help guide future experimental and theoretical investigations.