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由新型环保可持续聚合物合成的 N 掺杂碳纳米球,用于高选择性 CO 捕获。

N-doped carbon nanospheres synthesized from a newly designed eco-friendly sustainable polymer for highly selective CO capture.

机构信息

Department of Chemistry and Chemical Process Technology, Zonguldak Bülent Ecevit University, 67900, Zonguldak, Turkey.

Department of Chemistry and Department of Nano Technology Engineering, Zonguldak Bülent Ecevit University, 67100, Zonguldak, Turkey.

出版信息

Environ Sci Pollut Res Int. 2024 Oct;31(49):58844-58857. doi: 10.1007/s11356-024-35152-2. Epub 2024 Sep 25.

Abstract

N-doped carbon nanospheres and porous carbon were produced by a hydrothermal template and the activation of hexamethylenetetramine (HMTA as a nitrogen source and activator) and ZnCl (only as an activator) from a poly(Ri-S-ε-CL-PDMS) multiblock/graft copolymer produced using a renewable resource and eco-friendly autoxidation. N-doped carbon nanospheres (PPiSiHMTA) exhibited excellent CO adsorption (2.73 mmol/g at 0 °C and 0.15 atm, 1.72 mmol/g at 25 °C and 0.15 atm) and CO/N selectivity (344-512). Despite the higher BET surface area and pore volume, porous carbon (PPiSi) showed low CO adsorption (1.21 and 0.71 mmol/g, 0.15 atm) and CO/N selectivity (57 and 112). PPiSiHMTA and PPiSi have low isosteric heats of adsorption (Qst, 18-33 kJ/mol) and stability in humid environments. In addition, PPiSiHMTA exhibited an excellent CO recycling performance. The experimental data on CO₂ adsorption was evaluated using various isotherm models, including Freundlich, Langmuir, Sips, and Temkin. The results demonstrated a nearly perfect fit between the Freundlich isotherm and the experimental data, indicating the heterogeneous nature of the adsorbent surfaces. Our study is promising for industrial applications, offering excellent CO adsorption, CO/N selectivity, moisture stability, and porous material fabrication strategies.

摘要

氮掺杂碳纳米球和多孔碳是通过水热模板法以及六亚甲基四胺(HMTA,作为氮源和活化剂)和 ZnCl(仅作为活化剂)的活化作用,由可再生资源和环保自氧化法制备的聚(Ri-S-ε-CL-PDMS)多嵌段/接枝共聚物制备得到的。氮掺杂碳纳米球(PPiSiHMTA)表现出优异的 CO 吸附性能(在 0°C 和 0.15 atm 下为 2.73 mmol/g,在 25°C 和 0.15 atm 下为 1.72 mmol/g)和 CO/N 选择性(344-512)。尽管具有更高的 BET 比表面积和孔体积,但多孔碳(PPiSi)的 CO 吸附量较低(在 0.15 atm 下分别为 1.21 和 0.71 mmol/g),CO/N 选择性也较低(分别为 57 和 112)。PPiSiHMTA 和 PPiSi 在潮湿环境中具有较低的等吸附热(Qst,18-33 kJ/mol)和稳定性。此外,PPiSiHMTA 表现出优异的 CO 循环性能。CO₂吸附的实验数据通过各种等温模型进行了评估,包括 Freundlich、Langmuir、Sips 和 Temkin 模型。结果表明,Freundlich 等温线与实验数据之间具有近乎完美的拟合,表明吸附剂表面具有非均相性质。我们的研究为工业应用提供了有前景的方案,具有优异的 CO 吸附、CO/N 选择性、耐湿稳定性和多孔材料制备策略。

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