Yang Chunliang, Luo Lan, Zhao Tianxiang, Cao Jianxin, Lin Qian
Key Laboratory of Green Chemical and Clean Energy Technology, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, P. R. China.
Engineering Research Center of Efficient Utilization for Industrial Waste, Guizhou University, Guiyang 550025, China.
ACS Appl Mater Interfaces. 2025 Feb 5;17(5):8644-8656. doi: 10.1021/acsami.4c20959. Epub 2025 Jan 24.
Electron-induced effects, which are prevalent in adsorption and heterogeneous catalytic reactions, can significantly influence the state and uptake of adsorbates. Here, we demonstrate the in situ doping of electron-deficient boron into the backbone of chitosan-based porous carbon materials. Despite a reduction in specific surface area, the resulting boron-doped porous carbons (NBPCs) exhibit an enhanced CO adsorption performance, with sample NBPC-10 achieving CO adsorption capacities of 7.62 and 4.82 mmol·g at 273 and 298 K, respectively. This improvement is attributed to the electron-induced effect of boron doping, which also enhances the separation selectivity of CO from N. Additionally, the high CO adsorption capacity fosters synergism between NBPCs and the cocatalyst tetrabutylammonium bromide (TBAB), thereby augmenting the catalytic activity for the cycloaddition of CO and epoxide. Notably, cyclic carbonate yields exceeding 99% were attained even under 1 bar of CO. Controlled experiments corroborated the pivotal role of boron-doping-induced modifications in the porous carbon structure in enhancing both CO selective adsorption and conversion performance. Furthermore, NBPCs demonstrated excellent recyclability as both adsorbents and catalysts, offering fresh perspectives for the design of functionalized porous carbon materials tailored for CO capture and conversion.
电子诱导效应在吸附和多相催化反应中普遍存在,可显著影响吸附质的状态和吸附量。在此,我们展示了将缺电子硼原位掺杂到壳聚糖基多孔碳材料的骨架中。尽管比表面积有所降低,但所得的硼掺杂多孔碳(NBPCs)表现出增强的CO吸附性能,样品NBPC-10在273和298 K时的CO吸附容量分别达到7.62和4.82 mmol·g。这种改善归因于硼掺杂的电子诱导效应,它还提高了CO与N的分离选择性。此外,高CO吸附容量促进了NBPCs与助催化剂四丁基溴化铵(TBAB)之间的协同作用,从而增强了CO与环氧化物环加成的催化活性。值得注意的是,即使在1 bar的CO压力下,环状碳酸酯的产率也超过了99%。对照实验证实了硼掺杂诱导的多孔碳结构改性在增强CO选择性吸附和转化性能方面的关键作用。此外,NBPCs作为吸附剂和催化剂都表现出优异的可回收性,为设计用于CO捕获和转化的功能化多孔碳材料提供了新的视角。