N-rich porous carbon with high CO2 capture capacity derived from polyamine-incorporated metal–organic framework materials
N-rich porous carbon with high CO2 capture capacity derived from polyamine-incorporated metal–organic framework materials
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DOI：
10.1039/c6ra09472d
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发表时间：
2016-05
期刊：
影响因子：
3.9
通讯作者：
Junwen Wang;Yichao Lin;Q. Yue;K. Tao;Chunlong Kong;Liang Chen
中科院分区：
文献类型：
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作者：
Junwen Wang;Yichao Lin;Q. Yue;K. Tao;Chunlong Kong;Liang Chen
氮掺杂多孔炭在气体吸附、超级电容器等领域有着广泛的应用前景，因此开发高效的富氮多孔炭材料成为研究热点。本研究以多胺掺杂的金属有机骨架材料（MOFs）为原料，制备了一系列富氮多孔炭材料。结果表明，聚乙烯亚胺（PEI）负载到ZIF-70骨架上，可以吸附在ZIF-70的孔壁上，在炭化过程中同时提供碳源和氮源，从而大大提高了多孔炭的含氮量。结果，所制备的样品的表面积也增加。此外，多孔碳的N含量可以通过PEI负载量和碳化温度来调节。与ZIF-70和由ZIF-70衍生的多孔碳相比，所制备的富N多孔碳表现出大大增强的CO2选择性吸附能力。在这里，由于掺杂的N和CO2分子之间具有相当大的相互作用亲和力，所制备的富N多孔材料的CO2捕获能力随着N含量的增加而增加。因此，所制备的具有11.08重量%的N含量的多孔碳在0 °C和1巴下显示出4.86 mmol g-1的高CO2吸收，尽管其具有652 m2 g-1的中等表面积。此外，富N多孔碳清楚地显示出优异的CO2/N2和CO2/CH 4分离性能。总的来说，多胺掺入的MOFs是一种有效的策略，用于可控的富氮多孔碳的制造。所得产物显示出高的CO2选择性捕获性能。应该注意的是，为了实现最佳的CO2捕集能力，应该对聚胺-MOFs衍生的多孔碳进行全面优化。
N-doped porous carbon has a wide range of applications in many fields, such as gas adsorption and super-capacitor, which has stimulated active research for developing efficient strategies to fabricate N-rich porous carbon. In the present study, a series of N-rich porous carbons are derived from polyamine-incorporated metal–organic framework materials (MOFs). Results show that the N content of as-prepared porous carbon is greatly increased by loading polyethyleneimine (PEI) into ZIF-70 frameworks because the loaded PEI can adsorb onto the pore walls of the ZIF-70 and simultaneously supply carbon and N sources during the carbonization process. As a result, the surface area of the as-prepared sample is also increased. In addition, the N content of the porous carbon can be tuned by PEI loadings and carbonization temperature. The as-prepared N-rich porous carbons exhibit greatly enhanced CO2-selective adsorption capacity compared to ZIF-70 and porous carbon derived from ZIF-70. Here the CO2 capture capacity of the as-prepared N-rich porous increases with increasing N content due to considerable interaction affinity between doped N and CO2 molecules. Thus, the as-prepared porous carbon with N content of 11.08 wt% displays high CO2 uptake of 4.86 mmol g−1 at 0 °C and 1 bar, albeit it has a moderate surface area of 652 m2 g−1. Moreover, the N-rich porous carbon clearly shows an excellent separation performance for CO2-over-N2 and CO2-over-CH4. Overall, polyamine-incorporated MOFs are an efficient strategy for controllable fabrication of N-rich porous carbon. The resulting products display a high CO2-selective capture performance. It should be noted that, to achieve the optimal CO2 capture ability, a comprehensive optimization of the polyamine-MOFs-derived porous carbon should be performed.