Cao Yufei, Qiao Yida, Cui Shitong, Ge Jun
Key Lab for Industrial Biocatalysis, Ministry of Education, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
Institute of Biopharmaceutical and Health Engineering, Tsinghua Shenzhen International Graduate School, Shenzhen 518055, China.
JACS Au. 2022 Apr 11;2(4):961-971. doi: 10.1021/jacsau.2c00077. eCollection 2022 Apr 25.
Detailed understanding of how the bio-nano interface orchestrates the function of both biological components and nanomaterials remains ambiguous. Here, through a combination of experiments and molecular dynamics simulations, we investigated how the interface between lipase B and palladium (Pd) nanoparticles (NPs) tunes the structure, dynamics, and catalysis of the enzyme. Our simulations show that the metal binding to protein is a shape matching behavior and there is a transition from saturated binding to unsaturated binding along with the increase in the size of metal NPs. When we engineered the interface with the polymer, not only did the critical size of saturated binding of metal NPs become larger, but also the disturbance of the metal NPs to the enzyme function was reduced. In addition, we found that an enzyme-metal interface engineered with the polymer can boost bio-metal cascade reactions via substrate channeling. Understanding and control of the bio-nano interface at the molecular level enable us to rationally design bio-nanocomposites with prospective properties.
对生物纳米界面如何协调生物成分和纳米材料的功能的详细理解仍然不明确。在这里，通过实验和分子动力学模拟相结合的方法，我们研究了脂肪酶B与钯（Pd）纳米颗粒（NPs）之间的界面如何调节酶的结构、动力学和催化作用。我们的模拟表明，金属与蛋白质的结合是一种形状匹配行为，并且随着金属纳米颗粒尺寸的增加，存在从饱和结合到不饱和结合的转变。当我们用聚合物设计界面时，不仅金属纳米颗粒饱和结合的临界尺寸变大，而且金属纳米颗粒对酶功能的干扰也减少了。此外，我们发现用聚合物设计的酶-金属界面可以通过底物通道促进生物-金属级联反应。在分子水平上对生物纳米界面的理解和控制使我们能够合理设计具有预期性能的生物纳米复合材料。
