Marine diatoms construct their hierarchically ordered, three-dimensional (3D) external structures called frustules through precise biomineralization processes. Recapitulating the remarkable architectures and functions of diatom frustules in artificial materials is a major challenge that has important technological implications for hierarchically ordered composites. Here, we report the construction of highly ordered, mineralized composites based on fabrication of complex self-supporting porous structures—made of genetically engineered amyloid fusion proteins and the natural polysaccharide chitin—and performing in situ multiscale protein-mediated mineralization with diverse inorganic materials, including SiO₂, TiO₂, and Ga₂O₃. Subsequently, using sugar cubes as templates, we demonstrate that 3D fabricated porous structures can become colonized by engineered bacteria and can be functionalized with highly photoreactive minerals, thereby enabling co-localization of the photocatalytic units with a bacteria-based hydrogenase reaction for a successful semi-solid artificial photosynthesis system for hydrogen evolution. Our study thus highlights the power of coupling genetically engineered proteins and polysaccharides with biofabrication techniques to generate hierarchically organized mineralized porous structures inspired by nature.

中文翻译：

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硅藻启发的图案化蛋白质-多糖复合结构的多尺度矿化


海洋硅藻通过精确的生物矿化过程构建分层有序的三维 (3D) 外部结构，称为硅藻壳。概括硅藻壳在人造材料中的卓越结构和功能是一项重大挑战，对分层有序复合材料具有重要的技术意义。在这里，我们报告了高度有序的矿化复合材料的构建，该复合材料基于复杂的自支撑多孔结构的制造（由基因工程淀粉样融合蛋白和天然多糖几丁质制成），并用多种无机材料进行原位多尺度蛋白质介导的矿化，包括SiO ₂ 、TiO ₂和Ga ₂ O ₃ 。随后，使用方糖作为模板，我们证明了 3D 制造的多孔结构可以被工程细菌定植，并且可以用高光反应性矿物质进行功能化，从而使光催化单元与基于细菌的氢化酶反应共定位，从而成功地实现半透明化。 -用于析氢的固体人工光合作用系统。因此，我们的研究强调了将基因工程蛋白质和多糖与生物制造技术结合起来产生受大自然启发的分层组织的矿化多孔结构的力量。