Experimental and theoretical demonstration of the relative effects of O-doping and N-doping in porous carbons for CO2 capture
Experimental and theoretical demonstration of the relative effects of O-doping and N-doping in porous carbons for CO2 capture
复制标题
多孔碳中 O 掺杂和 N 掺杂对 CO2 捕获的相对影响的实验和理论论证
DOI：
10.1016/j.apsusc.2019.03.162
复制
发表时间：
2019-07-01
影响因子：
6.7
通讯作者：
Li, Hailong
中科院分区：
文献类型：
--
作者：
Ma, Xiancheng;Li, Liqing;Li, Hailong
n掺杂会影响CO2的捕获吗？这个问题仍然存在争议，因为氮掺杂多孔碳中氧含量对CO2吸收的影响尚未得到系统的研究。本文通过实验和理论计算研究了无氮和掺氮多孔碳对CO2吸收的影响。为了阐明氮官能团的相对影响，我们通过不同的合成条件合成了一系列未掺杂或掺杂N（2.73-9.44%）的碳。实验结果表明，在碳骨架中引入氧和氮可以改善多孔碳和掺氮多孔碳的CO2捕获。在这些样品中，NPC600在1 bar和25℃下表现出极高的CO2吸附能力（5.01 mmol g(-1)）。根据理论计算，在高氧碳骨架中引入氮气进一步增强了静电相互作用对CO2吸附的作用。此外，氮碳掺杂对CO2/N-2的选择性和CO2吸附的等容热都有较大的影响。预计这项研究将消除任何歧义，并更好地解释n掺杂对CO2捕获的影响。
Will the CO2 capture be affected by the N-doping? This question remains conflict due to the effect of oxygen content in N-doped porous carbons on CO2 uptake has not been systematically investigated. Herein, the effects of N-free and N-doped porous carbons on CO2 uptake were investigated by experiments and theoretical calculations. To elucidate the relative influences of nitrogen functional groups, we synthesized a series of carbons without or with N-doping (2.73-9.44% N) by varying the synthesis conditions. Experimental results show that the introduction of oxygen and nitrogen into carbon framework improves CO2 capture in porous carbons (PCs) and N-doped porous carbons (NPCs). Among these samples, the NPC600 exhibits an exceptionally high CO2 adsorption capacity (5.01 mmol g(-1) at 1 bar and 25 degrees C). Based on the theoretical calculations, the introduction of nitrogen into carbon framework with high oxygen content further enhances electrostatic interaction for CO2 adsorption. Moreover, the doping of nitrogen to carbon framework also has a greater effect on both the selectivity for CO2/N-2 and the isosteric heat of CO2 adsorption. It is predicted that this investigation will eliminate any ambiguities and better explain the influence of N-doping on CO2 capture.