A bioinspired dual-crosslinked tough silk protein hydrogel as a protective biocatalytic matrix for carbon sequestration
A bioinspired dual-crosslinked tough silk protein hydrogel as a protective biocatalytic matrix for carbon sequestration
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DOI：
10.1038/am.2017.71
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发表时间：
2017-06-30
影响因子：
9.7
通讯作者：
Cha, Hyung Joon
中科院分区：
文献类型：
--
作者：
Kim, Chang Sup;Yang, Yun Jung;Cha, Hyung Joon
开发基于碳酸酐酶(CA)的材料，在温和的条件下对环境友好地封存二氧化碳(CO2)，对于控制对环境的排放和生产增值化学品具有重要价值。在这里，一种高度坚韧和稳定的包裹CA的丝蛋白水凝胶被开发为一种强大的生物催化剂，通过生物启发的双重交联策略，采用光诱导的双赖氨酸化学交联和脱水介导的物理交联。将目标酶有效地包埋在丝素水凝胶中，游离酸的活性保留率接近60%，且包埋物具有良好的多用性、保存性和热稳定性。双交联型CA包埋的蚕丝水凝胶具有显著的压缩模数，超过了大多数传统水凝胶和双网络水凝胶以及酶包埋水凝胶的压缩模数。该水凝胶具有较高的弹性和弹性，结构稳定性较好。重要的是，双交联包覆CA的丝素水凝胶有助于将CO2固定到具有高CO2水化活性的碳酸钙中。因此，丝素蛋白与CA酶的生物诱导双重交联的独特组合表明，这种蛋白质水凝胶具有高活性、强大的机械性能和优异的结构稳定性，是一种有前途的二氧化碳固定生物催化剂。
The development of carbonic anhydrase (CA)-based materials for the environment-friendly sequestration of carbon dioxide (CO2) under mild conditions would be highly valuable for controlling emissions to the environment and for producing value-added chemicals. Here, a highly tough and stable CA-encapsulating silk protein hydrogel was developed as a robust biocatalyst for CO2 sequestration through a bioinspired dual-crosslinking strategy that employed photoinduced dityrosine chemical crosslinking followed by dehydration-mediated physical crosslinking. The target enzyme was efficiently encapsulated in the silk hydrogel with similar to 60% retention of the activity of free CA, and the encapsulated CA exhibited excellent overall multi-use, storage and thermal stabilities. The dual-crosslinked CA-encapsulating silk hydrogel exhibited a significant compressive modulus, which surpassed the moduli of most traditional and double-network hydrogels as well as those of enzyme-encapsulated hydrogels. This hydrogel also showed high resiliency and elasticity and outstanding structural stability. Importantly, the dual-crosslinked CA-encapsulating silk hydrogel facilitated the sequestration of CO2 into calcium carbonate with high CO2 hydration activity. Thus, the unique combination of bioinspired dual-crosslinking with silk fibroin protein and CA enzyme demonstrates the successful application of this protein hydrogel as a promising biocatalyst for CO2 sequestration by showing high activity, strong mechanical properties and outstanding structural stability.