Zhang Qianzhong, Jiang Yi, Li Yinwu, Song Xianheng, Luo Xiang, Ke Zhuofeng, Zou Yong
School of Pharmaceutical Sciences, Sun Yat-sen University, Guangzhou 510000, P. R. China.
School of Chemistry, Sun Yat-sen University, Guangzhou 510000, P. R. China.
iScience. 2021 Mar 4;24(4):102263. doi: 10.1016/j.isci.2021.102263. eCollection 2021 Apr 23.
In this study, the concept of biomass-based direct air capture is proposed, and the aminoguanidine CO chemical sorbent 2,5-furan-bis(iminoguanidine) (FuBIG) was designed, synthesized, and elucidated for the physicochemical properties in the process of CO capture and release. Results showed that the aqueous solution of FuBIG could readily capture CO from ambient air and provided an insoluble tetrahydrated carbonate salt FuBIGH(CO) (HO) with a second order kinetics. Hydrogen binding modes of iminoguanidine cations with carbonate ions and water were identified by single-crystal X-ray diffraction analysis. Equilibrium constant (K) and the enthalpies (ΔH) for CO absorption/release were obtained by thermodynamic and kinetic analysis (K = 5.97 × 10, ΔH = -116.1 kJ/mol, ΔH = 209.31 kJ/mol), and the CO-release process was conformed to the geometrical phase-boundary model (1-(1-α) = kt). It was found that the FuBIGH(CO) (HO) can release CO spontaneously in DMSO without heating. Zebrafish models revealed a favorable biocompatibility of FuBIG.
在本研究中，提出了基于生物质的直接空气捕获概念，并设计、合成了氨基胍CO化学吸附剂2,5-呋喃-双(亚氨基胍)(FuBIG)，并对其在CO捕获和释放过程中的物理化学性质进行了阐释。结果表明，FuBIG水溶液能够从环境空气中轻松捕获CO，并以二级动力学提供一种不溶性的四水合碳酸盐盐FuBIGH(CO)(HO)。通过单晶X射线衍射分析确定了亚氨基胍阳离子与碳酸根离子和水的氢键结合模式。通过热力学和动力学分析获得了CO吸收/释放的平衡常数(K)和焓(ΔH)(K = 5.97×10，ΔH = -116.1 kJ/mol，ΔH = 209.31 kJ/mol)，并且CO释放过程符合几何相边界模型(1-(1-α)= kt)。研究发现，FuBIGH(CO)(HO)在DMSO中无需加热即可自发释放CO。斑马鱼模型显示FuBIG具有良好的生物相容性。
