Synthetic engineering of a new biocatalyst encapsulating [NiFe]-hydrogenases for enhanced hydrogen production.
Synthetic engineering of a new biocatalyst encapsulating [NiFe]-hydrogenases for enhanced hydrogen production.
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DOI：
10.1039/d2tb02781j
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发表时间：
2023-03-22
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氢化酶是一种高效催化分子氢与质子可逆相互转化的微生物金属酶，在开发新型可再生燃料电催化剂方面具有巨大潜力。在这里，我们设计了完整的蛋白质壳的羧基体，自组装蛋白质细胞器的蓝藻和变形菌中的CO2固定，并隔离异源产生的[NiFe]-氢化酶到羧基体壳。在E.大肠杆菌中的[NiFe]-氢化酶与未包封的[NiFe]-氢化酶相比，在需氧和厌氧条件下均显示出显著改善的氢产生，以及增强的材料和功能稳健性。催化功能纳米反应器以及自组装和封装策略为设计新的生物启发电催化剂提供了一个框架，以改善生物技术和化学应用中燃料和化学品的可持续生产。通过将[NiFe]-氢化酶结合到蛋白质羧基体壳中，我们产生了一种新型的生物催化剂，该催化剂提高了清洁氢气的生产，耐氧性和热稳定性，突出了其在生物技术应用中的巨大潜力。
Hydrogenases are microbial metalloenzymes capable of catalyzing the reversible interconversion between molecular hydrogen and protons with high efficiency, and have great potential in the development of new electrocatalysts for renewable fuel production. Here, we engineered the intact proteinaceous shell of the carboxysome, a self-assembling protein organelle for CO2 fixation in cyanobacteria and proteobacteria, and sequestered heterologously produced [NiFe]-hydrogenases into the carboxysome shell. The protein-based hybrid catalyst produced in E. coli shows substantially improved hydrogen production under both aerobic and anaerobic conditions and enhanced material and functional robustness, compared to unencapsulated [NiFe]-hydrogenases. The catalytically functional nanoreactor as well as the self-assembling and encapsulation strategies provide a framework for engineering new bioinspired electrocatalysts to improve the sustainable production of fuels and chemicals in biotechnological and chemical applications. By incorporating [NiFe]-hydrogenases into a proteinaceous carboxysome shell, we generate a novel biocatalyst that has improved production of clean hydrogen, oxygen tolerance, and thermostability, highlighting its great potential in biotechnological applications.
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影响因子：
4.7
作者：
Chen T;Fang Y;Jiang Q;Dykes GF;Lin Y;Price GD;Long BM;Liu LN
通讯作者：
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DOI：
10.1073/pnas.2007990117
发表时间：
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影响因子：
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作者：
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影响因子：
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作者：
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通讯作者：
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DOI：
10.1073/pnas.0905959106
发表时间：
2009-12-08
影响因子：
11.1
作者：
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通讯作者：
Armstrong, Fraser A.