Biobased Colloids and Materials group (BiCMat), Department of Bioproducts and Biosystems, School of Chemical Engineering, Aalto University , FI-00076, Espoo, Finland.
Department of Chemical and Biomolecular Engineering, North Carolina State University , Raleigh, North Carolina 27695, United States.
Biomacromolecules. 2017 Jun 12;18(6):1803-1813. doi: 10.1021/acs.biomac.7b00256. Epub 2017 May 3.
We demonstrate benzophenone (BP) conjugation via amine-reactive esters onto oxidized cellulosic fibers that were used as precursors, after microfluidization, of photoactive cellulose nanofibrils (CNF). From these fibrils, cellulose I filaments were synthesized by hydrogel spinning in an antisolvent followed by fast biradical UV cross-linking. As a result, the wet BP-CNF filaments retained extensively the original dry strength (a remarkable ∼80% retention). Thus, the principal limitation of these emerging materials was overcome (the wet tensile strength is typically <0.5% of the value measured in dry conditions). Subsequently, antihuman hemoglobin (anti-Hb) antibodies were conjugated onto residual surface carboxyl groups, making the filaments bifunctional for their active groups and properties (wet strength and bioactivity). Optical (surface plasmon resonance) and electroacoustic (quartz crystal microgravimetry) measurements conducted with the bifunctional CNF indicated effective anti-Hb conjugation (2.4 mg m), endowing an excellent sensitivity toward Hb targets (1.7 ± 0.12 mg m) and negligible nonspecific binding. Thus, the anti-Hb biointerface was deployed on filaments that captured Hb efficiently from aqueous matrices (confocal laser microscopy of FITC-labeled antibodies). Significantly, the anti-Hb biointerface was suitable for regeneration, while its sensitivity and selectivity in affinity binding can be tailored by application of blocking copolymers. The developed bifunctional filaments based on nanocellulose offer great promise in detection and affinity binding built upon 1D systems, which can be engineered into other structures for rational use of material and space.
我们通过胺反应酯将二苯甲酮 (BP) 键合到氧化纤维素纤维上,这些纤维在微流化后作为前体,进一步制备出光活性纤维素纳米纤维 (CNF)。从这些纤维中,通过在抗溶剂中凝胶纺丝和快速双自由基 UV 交联合成纤维素 I 长丝。结果,湿 BP-CNF 纤维保留了广泛的原始干强度(显著的约 80%保留率)。因此,克服了这些新兴材料的主要限制(湿拉伸强度通常<干燥条件下测量值的 0.5%)。随后,将抗人血红蛋白 (anti-Hb) 抗体共轭到残留的表面羧基上,使纤维在其活性基团和性质(湿强度和生物活性)上具有双功能。用双功能 CNF 进行的光学(表面等离子体共振)和电化学生物传感器(石英晶体微天平)测量表明,有效的 anti-Hb 共轭(2.4 mg m),赋予了对 Hb 靶标的出色敏感性(1.7±0.12 mg m)和可忽略的非特异性结合。因此,将抗-Hb 生物界面部署在能够从水基基质中有效捕获 Hb 的纤维上(FITC 标记抗体的共聚焦激光显微镜)。重要的是,抗-Hb 生物界面适合于再生,而其在亲和结合中的灵敏度和选择性可以通过应用封端共聚物进行调整。基于纳米纤维素的双功能纤维在基于 1D 系统的检测和亲和结合方面具有很大的应用前景,这些纤维可以进一步设计成其他结构,以合理利用材料和空间。