基于介观螺旋材料的生物-无机界面的构筑与调控

Controlling the bio-interfacial recognition and assembly to obtain immobilized enzyme with high bio-activity and stability has been long regarded as a main focus in the field of bio-catalysis. How to fabricate and tune the biocompatible bio-inorganic interfaces is the vital scientific issues in the bio-interface chemistry. The research is mainly focused on the construction of the inorganic bio-mimetic interfaces employing mesoscopic helical materials,the chiral recognition for the biomolecules, and the bio-inorganic interfacial assembly between chiral materials and enzymes. By tailoring the interfacial recognition,the recognition site,the interaction mode and the interaction intensity, the active conformation and orientation are supposed to be obtained, thus achieving the enhanced activity and reactivity. The general rule of the molecular recognition within the bio-inorganic interfaces is to be further investigated combined with the computer simulation using molecular dynamics theory and quantum chemistry theory.The innovative features of this research are proposed to include the following two points: (1) By varying the surface property,the helix mode and the helicity of the helical inorganic nanomaterials,the interfacial assembly is readily controlled; (2) The biomimetic inorganic interface supplies preferably bio-compatible micro- environment for the immobilized enzymes, giving a chance to achieve enhanced bioactivity.

如何控制生物分子与主体材料之间的界面识别和界面组装以获得高活性和稳定性的固定化酶一直是生物催化领域所面临的主要挑战之一。围绕如何构筑生物相容性高的生物-无机界面及控制界面组装，本课题提出利用介观手性螺旋材料构筑仿生无机界面，识别生物大分子，进行生物-无机界面组装。通过调控二者的界面识别、识别位点、作用方式及强度，控制生物大分子活性构象和活性位点优先取向，实现酶分子不对称催化性能的强化，结合理论计算研究生物-无机界面手性识别的机理，揭示界面识别及识别过程的本质。本课题提出的生物-无机界面构筑与调控的特点在于：(1)通过调变手性螺旋材料的表面性质、螺旋方式与螺旋度可方便实现界面组装行为的调控；(2) 仿生无机界面为酶分子提供了更好的生物相容微环境，有望获得性能强化的生物-无机杂化催化材料。

如何控制生物分子与主体材料之间的界面识别和界面组装以获得高活性和稳定性的固定化酶一直是生物催化领域所面临的主要挑战之一。本课题针对生物相容性高的生物-无机界面的构筑及控制界面组装，提出利用介观手性螺旋材料构筑仿生无机界面，识别手性生物分子，如氨基酸、α-螺旋、β-折叠及酶分子，进行生物-无机界面组装。课题通过调控二者的界面识别、识别位点、作用方式及强度，控制了生物大分子活性构象和活性位点优先取向，进而实现了活性分子不对称催化性能的强化。进一步初步结合了理论计算研究生物-无机界面手性识别的机理，揭示了界面识别及识别过程的本质。针对不对称Aldol及不对称连串反应等重要反应，发展了2-3种高效的多相不对称催化材料以及绿色的合成途径。