Shi Weiwei, Wang Rongzhen, Liu Huili, Chang Binbin, Yang Baocheng, Zhang Zuling
Henan Key Laboratory of Nanocomposites and Applications, Institute of Nanostructured Functional Materials, Huanghe Science and Technology College Zhengzhou Henan 450006 China
Henan Provincial Chemi-Industries Research Station Co., Ltd Zhengzhou 450000 China.
RSC Adv. 2019 Jul 26;9(40):23241-23253. doi: 10.1039/c9ra03659h. eCollection 2019 Jul 23.
Considering the characteristics of abundant narrow micropores of <1 nm, appropriate proportion of mesopores/macropores and suitable surface functionalization for a highly-efficient carbon-based CO adsorbent, we proposed a facile and cost-effective strategy to prepare N and S dual-doped carbons with well-interconnected hierarchical pores. Benefiting from the unique structural features, the resultant optimal material showed a prominent CO uptake of up to 7.76 and 5.19 mmol g at 273 and 298 K under 1 bar, and importantly, a superb CO uptake of 1.51 mmol g at 298 K and 0.15 bar was achieved, which was greatly significant for CO capture from the post-combustion flue gases in practical application. A systematic study demonstrated that the synergetic effect of ultramicroporosity and surface functionalization determined the CO capture properties of porous carbons, and the synergistic influence mechanism of nitrogen/sulfur dual-doping on CO capture performance was also investigated in detail. Importantly, such as-prepared carbon-based CO adsorbents also showed an outstanding recyclability and CO/N selectivity. In view of cost-effective fabrication, the excellent adsorption capacity, high selectivity and simple regeneration, our developed strategy was valid and convenient to design a novel and highly-efficient carbonaceous adsorbent for large-scale CO capture and separation from post-combustion flue gases.
考虑到高效碳基CO吸附剂具有丰富的<1 nm窄微孔、适当比例的中孔/大孔以及合适的表面功能化等特性,我们提出了一种简便且经济高效的策略来制备具有良好互连分级孔结构的N和S双掺杂碳。受益于独特的结构特征,所得的最优材料在1 bar下于273和298 K时分别表现出高达7.76和5.19 mmol g的显著CO吸附量,重要的是,在298 K和0.15 bar时实现了1.51 mmol g的优异CO吸附量,这对于实际应用中从燃烧后烟道气中捕获CO具有重大意义。系统研究表明,超微孔性和表面功能化的协同效应决定了多孔碳的CO捕获性能,并且还详细研究了氮/硫双掺杂对CO捕获性能的协同影响机制。重要的是,如此制备的碳基CO吸附剂还表现出出色的可回收性和CO/N选择性。鉴于具有成本效益的制备、优异的吸附容量、高选择性和简单的再生过程,我们开发的策略对于设计一种用于从燃烧后烟道气中大规模捕获和分离CO的新型高效碳质吸附剂是有效且便捷的。