PDF(Pubmed)
Abstract：
The sensitivity and responsiveness of living cells to environmental changes are enabled by dynamic protein structures, inspiring efforts to construct artificial supramolecular protein assemblies. However, despite their sophisticated structures, designed protein assemblies have yet to be incorporated into macroscale devices for real-life applications. We report a 2D crystalline protein assembly of C98/E57/E66L-rhamnulose-1-phosphate aldolase (CEERhuA) that selectively blocks or passes molecular species when exposed to a chemical trigger. CEERhuA crystals are engineered via cobalt(II) coordination bonds to undergo a coherent conformational change from a closed state (pore dimensions <1 nm) to an ajar state (pore dimensions ~4 nm) when exposed to an HCN(g) trigger. When layered onto a mesoporous silicon (pSi) photonic crystal optical sensor configured to detect HCN(g), the 2D CEERhuA crystal layer effectively blocks interferents that would otherwise result in a false positive signal. The 2D CEERhuA crystal layer opens in selective response to low-ppm levels of HCN(g), allowing analyte penetration into the pSi sensor layer for detection. These findings illustrate that designed protein assemblies can function as dynamic components of solid-state devices in non-aqueous environments.
摘要：
活细胞对环境变化的敏感性和反应性是通过动态蛋白质结构实现的，构建人工超分子蛋白质组装体的努力令人鼓舞。然而,尽管它们复杂的结构，设计的蛋白质组件尚未被纳入到大规模设备的现实生活中应用。我们报告了C98/E57/E66L-鼠李糖-1-磷酸醛缩酶（CEERhuA）的2D结晶蛋白质组装体，该组装体在暴露于化学触发剂时选择性地阻断或传递分子物种。CEERhuA晶体通过钴（II）配位键进行工程改造，当暴露于HCN（g）触发剂时，会发生从封闭状态（孔尺寸<1nm）到半开状态（孔尺寸〜4nm）的相干构象变化。当层叠到被配置为检测HCN(g)的介孔硅(pSi)光子晶体光学传感器上时，例如,2DCEERhuA晶体层有效地阻挡否则将导致假阳性信号的干扰物。2DCEERhuA晶体层选择性响应于低ppm水平的HCN（g）而打开，允许分析物渗透到pSi传感器层中进行检测。这些发现说明所设计的蛋白质组件可以在非水环境中充当固态装置的动态组件。
