Beijing Key Laboratory of Optical Detection Technology for Oil and Gas, Basic Research Center for Energy Interdisciplinary, College of Science, China University of Petroleum-Beijing, Beijing 102249, China.
State-Province Joint Engineering Laboratory of Zeolite Membrane Materials, Jiangxi Normal University, Nanchang 330022, China.
Langmuir. 2023 May 9;39(18):6613-6622. doi: 10.1021/acs.langmuir.3c00595. Epub 2023 Apr 25.
Development of high-performance materials for the capture and separation of CO from the gas mixture is significant to alleviate carbon emission and mitigate the greenhouse effect. In this work, a novel structure of CN slit was developed to explore its CO adsorption capacity and selectivity using Grand Canonical Monte Carlo (GCMC) and Density Functional Theory (DFT) calculations. Among varying slit widths, CN with the slit width of 0.7 nm exhibited remarkable CO uptake with superior CO/N and CO/CH selectivity. At 1 bar and 298 K, a maximum CO adsorption capacity can be obtained as high as 7.06 mmol/g, and the selectivity of CO/N and CO/CH was 41.43 and 18.67, respectively. In the presence of HO, the CO uptake of CN slit decreased slightly as the water content increased, showing better water tolerance. Furthermore, the underlying mechanism of highly selective CO adsorption and separation on the CN surface was revealed. The closer the adsorption distance, the stronger the interaction energy between the gas molecule and the CN surface. The strong interaction between the CN nanosheet and the CO molecule contributes to its impressive CO uptake and selectivity performance, suggesting that the CN slit could be a promising candidate for CO capture and separation.
开发用于从混合气中捕获和分离 CO 的高性能材料对于缓解碳排放和减轻温室效应具有重要意义。在这项工作中，采用巨正则蒙特卡罗（GCMC）和密度泛函理论（DFT）计算方法，开发了一种新型的 CN 狭缝结构，以探索其 CO 吸附能力和选择性。在不同的狭缝宽度中，具有 0.7nm 狭缝宽度的 CN 表现出优异的 CO 吸附量和更高的 CO/N 和 CO/CH 选择性。在 1 巴和 298K 下，最大 CO 吸附量高达 7.06mmol/g，CO/N 和 CO/CH 的选择性分别为 41.43 和 18.67。在存在 HO 的情况下，随着含水量的增加，CN 狭缝的 CO 吸附量略有下降，表现出更好的耐水性。此外，揭示了 CO 在 CN 表面上高选择性吸附和分离的潜在机制。吸附距离越近，气体分子与 CN 表面之间的相互作用能越强。CN 纳米片与 CO 分子之间的强相互作用有助于其具有令人印象深刻的 CO 吸附量和选择性性能，表明 CN 狭缝可能是 CO 捕获和分离的有前途的候选材料。
