Daniels Emma L, Runge James R, Oshinowo Matthew, Leese Hannah S, Buchard Antoine
University of Bath Institute for Sustainability, Claverton Down, Bath BA2 7AY, U.K.
Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, U.K.
ACS Appl Energy Mater. 2023 Feb 22;6(5):2924-2935. doi: 10.1021/acsaem.2c03937. eCollection 2023 Mar 13.
This report describes the synthesis and characterization of organogels by reaction of a diol-containing polyether, derived from the sugar d-xylose, with 1,4-phenylenediboronic acid (PDBA). The cross-linked materials were analyzed by infrared spectroscopy (FT-IR), thermal gravimetric analysis (TGA), scanning electron microscopy (FE-SEM), and rheology. The rheological material properties could be tuned: gel or viscoelastic behavior depended on the concentration of polymer, and mechanical stiffness increased with the amount of PDBA cross-linker. Organogels demonstrated self-healing capabilities and recovered their storage and loss moduli instantaneously after application and subsequent strain release. Lithiated organogels were synthesized through incorporation of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) into the cross-linked matrix. These lithium-borate polymer gels showed a high ionic conductivity value of up to 3.71 × 10 S cm at 25 °C, high lithium transference numbers ( = 0.88-0.92), and electrochemical stability (4.51 V). The gels were compatible with lithium-metal electrodes, showing stable polarization profiles in plating/stripping tests. This system provides a promising platform for the production of self-healing gel polymer electrolytes (GPEs) derived from renewable feedstocks for battery applications.
本报告描述了由源自糖类d-木糖的含二醇聚醚与1,4-苯二硼酸（PDBA）反应合成并表征有机凝胶的过程。通过红外光谱（FT-IR）、热重分析（TGA）、扫描电子显微镜（FE-SEM）和流变学对交联材料进行了分析。流变材料性能可以调节：凝胶或粘弹性行为取决于聚合物浓度，机械刚度随PDBA交联剂用量的增加而提高。有机凝胶表现出自愈能力，在施加应变并随后释放后能立即恢复其储能模量和损耗模量。通过将双（三氟甲磺酰）亚胺锂（LiTFSI）掺入交联基质中合成了锂化有机凝胶。这些锂硼聚合物凝胶在25℃时显示出高达3.71×10 S cm的高离子电导率值、高锂迁移数（=0.88 - 0.92）和电化学稳定性（4.51 V）。这些凝胶与锂金属电极相容，在电镀/剥离测试中显示出稳定的极化曲线。该体系为生产源自可再生原料的用于电池应用的自愈凝胶聚合物电解质（GPE）提供了一个有前景的平台。
