Shmool Talia A, Martin Laura K, Bui-Le Liem, Moya-Ramirez Ignacio, Kotidis Pavlos, Matthews Richard P, Venter Gerhard A, Kontoravdi Cleo, Polizzi Karen M, Hallett Jason P
Department of Chemical Engineering, Imperial College London South Kensington Campus London SW7 2AZ UK
Department of Engineering Science, University of Oxford Parks Road Oxford OX1 3PJ UK.
Chem Sci. 2021 Jun 22;12(27):9528-9545. doi: 10.1039/d1sc02520a. eCollection 2021 Jul 14.
Understanding protein folding in different environmental conditions is fundamentally important for predicting protein structures and developing innovative antibody formulations. While the thermodynamics and kinetics of folding and unfolding have been extensively studied by computational methods, experimental methods for determining antibody conformational transition pathways are lacking. Motivated to fill this gap, we prepared a series of unique formulations containing a high concentration of a chimeric immunoglobin G4 (IgG4) antibody with different excipients in the presence and absence of the ionic liquid (IL) choline dihydrogen phosphate. We determined the effects of different excipients and IL on protein thermal and structural stability by performing variable temperature circular dichroism and bio-layer interferometry analyses. To further rationalise the observations of conformational changes with temperature, we carried out molecular dynamics simulations on a single antibody binding fragment from IgG4 in the different formulations, at low and high temperatures. We developed a methodology to study the conformational transitions and associated thermodynamics of biomolecules, and we showed IL-induced conformational transitions. We showed that the increased propensity for conformational change was driven by preferential binding of the dihydrogen phosphate anion to the antibody fragment. Finally, we found that a formulation containing IL with sugar, amino acids and surfactant is a promising candidate for stabilising proteins against conformational destabilisation and aggregation. We hope that ultimately, we can help in the quest to understand the molecular basis of the stability of antibodies and protein misfolding phenomena and offer new candidate formulations with the potential to revive lost therapeutic candidates.
了解蛋白质在不同环境条件下的折叠对于预测蛋白质结构和开发创新抗体配方至关重要。虽然折叠和去折叠的热力学和动力学已通过计算方法进行了广泛研究,但缺乏确定抗体构象转变途径的实验方法。为填补这一空白,我们制备了一系列独特的配方,在有和没有离子液体(IL)磷酸二氢胆碱的情况下,含有高浓度的嵌合免疫球蛋白G4(IgG4)抗体和不同的赋形剂。我们通过进行变温圆二色性和生物层干涉分析,确定了不同赋形剂和离子液体对蛋白质热稳定性和结构稳定性的影响。为了进一步合理解释随温度变化的构象变化观察结果,我们在不同配方中,对来自IgG4的单个抗体结合片段在低温和高温下进行了分子动力学模拟。我们开发了一种方法来研究生物分子的构象转变和相关的热力学,并且我们展示了离子液体诱导的构象转变。我们表明,构象变化倾向的增加是由磷酸二氢根阴离子与抗体片段的优先结合驱动的。最后,我们发现含有离子液体与糖、氨基酸和表面活性剂的配方是稳定蛋白质以防止构象不稳定和聚集的有前途的候选物。我们希望最终能够帮助探索抗体稳定性和蛋白质错误折叠现象的分子基础,并提供有可能挽救失去的治疗候选物的新候选配方。