Sulfur-Doped Millimeter-Sized Microporous Activated Carbon Spheres Derived from Sulfonated Poly(styrene-divinylbenzene) for CO2 Capture
Sulfur-Doped Millimeter-Sized Microporous Activated Carbon Spheres Derived from Sulfonated Poly(styrene-divinylbenzene) for CO2 Capture
复制标题
用于二氧化碳捕获的磺化聚（苯乙烯-二乙烯基苯）衍生的掺硫毫米级微孔活性炭球
DOI：
10.1021/acs.jpcc.7b02195
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发表时间：
2017
影响因子：
3.7
通讯作者：
Li Kaixi
中科院分区：
文献类型：
--
作者：
Sun Yahui;Zhao Jianghong;Wang Jianlong;Tang Nan;Zhao Rijie;Zhang Dongdong;Guan Taotao;Li Kaixi
毫米级活性炭球是工业规模二氧化碳捕集的潜在候选者。在目前的工作中，毫米级的硫掺杂微孔活性炭球是由聚（苯乙烯-二乙烯基苯）（一种非常便宜且易于操作的树脂产品）合成的，并研究了二氧化碳的吸收。通过聚合物前驱体的磺化、氧化、碳化和KOH活化，得到了一系列硫掺杂球形碳材料。除了促进聚合物分子的交联之外，磺酸基取代基在热解后直接将硫官能团引入到碳材料中。 SCS-700样品表现出最好的CO2吸附性能，其硫含量达到0.69 wt%，并表现出1526 m2g–1的高比表面积和0.726 cm3g–1的大孔体积。由于其丰富的超微孔和高比例的氧化硫官能团，该吸附剂在环境压力下在 25 °C (4.21 mmol g–1) 和 50 °C (2.54 mmol g–1) 下均表现出较高的 CO2 吸收率。由于其微孔体积高达 0.617 cm3g–1，25 °C 时 8 bar 下的 CO2 性能为 10.66 mmol g–1。热力学表明吸附过程是放热和自发的，主要由物理吸附机制决定。此外，TGA分析仪上的CO2吸收曲线采用不同的动力学模型进行拟合，分数阶模型与实验数据吻合得最好。 SCS-700的回收曲线表现出优异的循环吸附性能，即使在十次吸附-解吸循环后也没有明显的容量损失。这表明这种优异的CO2吸收是由于发达的微孔结构和氧化的含硫官能团的协同效应。
Millimeter-sized activated carbon spheres are potential candidates for industrial-scale CO2capture. Millimeter-sized sulfur-doped microporous activated carbon spheres were synthesized from poly(styrene–divinylbenzene), a very cheap and easily operated resin product, in the present work and studied for CO2uptake. A series of sulfur-doped spherical carbon materials were yielded through the sulfonation, oxidation, carbonization, and KOH activation of the polymer precursors. In addition to promoting the cross-linking of the polymer molecules, the sulfonic substituents directly introduced sulfur functional groups into the carbon materials after pyrolysis. The SCS-700 sample showed the best CO2adsorption performance, whose sulfur content reached 0.69 wt %, and exhibited a high surface area of 1526 m2g–1and a large pore volume of 0.726 cm3g–1. The adsorbent showed high CO2uptake at both 25 °C (4.21 mmol g–1) and 50 °C (2.54 mmol g–1) under ambient pressure due to its abundant ultramicropores and a high proportion of oxidized sulfur functional groups. Thanks to its high microporous volume of 0.617 cm3g–1, the CO2performance at 8 bar was 10.66 mmol g–1at 25 °C. The thermodynamics indicated the exothermic and spontaneous nature of the adsorption process, which was dominated by a physisorption mechanism. Furthermore, the CO2uptake curves on a TGA analyzer were fitted with different kinetic models, and the fractional order model showed the best agreement with the experimental data. The recycling curve of SCS-700 exhibited excellent cyclic adsorption performance with no significant capacity loss even after ten adsorption–desorption cycles. It is suggested that this excellent CO2uptake was due to the synergistic effect of the well-developed microporous structure and the oxidized sulfur-containing functional groups.