用于酶生物催化的酶@金属-有机材料（MOM）生物复合材料的一锅法合成,Green Chemistry

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用于酶生物催化的酶@金属-有机材料（MOM）生物复合材料的一锅法合成
Green Chemistry ( IF 9.3 ) Pub Date : 2021-5-13 , DOI: 10.1039/d1gc00775k
Yanxiong Pan _{1,

2,

3,

4} , Hui Li _{2,

3,

4,

5} , Mary Lenertz _{1,

2,

3,

4} , Yulun Han _{1,

2,

3,

4} , Angel Ugrinov _{1,

2,

3,

4} , Dmitri Kilin _{1,

2,

3,

4} , Bingcan Chen _{2,

3,

4,

5} , Zhongyu Yang _{1,

2,

3,

4}

Affiliation

金属有机框架/材料 (MOFs/MOMs) 是先进的酶固定化平台，可改善生物催化、材料科学和蛋白质生物物理学。一种独特的固定酶的方法是共结晶/共沉淀，它消除了对酶/底物大小的限制。迄今为止，大多数酶@MOF 复合材料依赖于不可持续的化学品的使用，在某些情况下还依赖于重金属，这不仅引起了对环境保护的担忧，而且限制了它们在营养和生物医学中的应用。在这里，我们展示了一种源自木质素的二聚化合物，5,5'-脱氢二香草酸 (DDVA)，与酶和低毒金属 Ca ²⁺和 Zn ²⁺共沉淀，并形成稳定的酶@Ca/Zn-MOM 复合材料。我们在具有不同等电点 (IEP)、分子量和底物大小的四种酶上展示了这种策略。此外，我们发现所有酶在固定在 Ca-DDVA 和 Zn-DDVA MOM 中时都显示出略有不同但合理的催化效率，以及在两种复合材料中的合理可重用性。然后我们使用代表性酶探测了这种差异的结构基础，发现 Zn-DDVA 中酶的限制比 Ca-DDVA 中的酶限制性更强，这可能导致了活性差异。据我们所知，这是木质素衍生的“绿色”酶@MOF/MOM 平台的第一个水相一锅合成，该平台可以承载酶，对酶 IEP、分子量和底物大小没有任何限制. 由 Ca-DDVA 和 Zn-DDVA MOM 形成的复合材料的不同形态和结晶度根据感兴趣的问题拓宽了它们的应用。我们固定化酶的方法不仅提高了几乎所有酶的可持续性/可重复使用性，而且减少/消除了非可持续性资源的使用。这种合成方法对环境的影响可以忽略不计，而产品对生物和环境无毒。生物相容性还使得为营养或生物医学应用进行酶递送/释放成为可能我们固定化酶的方法不仅提高了几乎所有酶的可持续性/可重复使用性，而且减少/消除了非可持续性资源的使用。这种合成方法对环境的影响可以忽略不计，而产品对生物和环境无毒。生物相容性还使得为营养或生物医学应用进行酶递送/释放成为可能我们固定化酶的方法不仅提高了几乎所有酶的可持续性/可重复使用性，而且减少/消除了非可持续性资源的使用。这种合成方法对环境的影响可以忽略不计，而产品对生物和环境无毒。生物相容性还使得为营养或生物医学应用进行酶递送/释放成为可能通过我们的“绿色”生物复合材料。

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One-pot synthesis of enzyme@metal–organic material (MOM) biocomposites for enzyme biocatalysis

Metal–organic frameworks/materials (MOFs/MOMs) are advanced enzyme immobilization platforms that improve biocatalysis, materials science, and protein biophysics. A unique way to immobilize enzymes is co-crystallization/co-precipitation, which removes the limitation on enzyme/substrate size. Thus far, most enzyme@MOF composites rely on the use of non-sustainable chemicals and, in certain cases, heavy metals, which not only creates concerns regarding environmental conservation but also limits their applications in nutrition and biomedicine. Here, we show that a dimeric compound derived from lignin, 5,5′-dehydrodivanillate (DDVA), co-precipitates with enzymes and low-toxicity metals, Ca²⁺ and Zn²⁺, and forms stable enzyme@Ca/Zn–MOM composites. We demonstrated this strategy on four enzymes with different isoelectric points (IEPs), molecular weights, and substrate sizes. Furthermore, we found that all enzymes displayed slightly different but reasonable catalytic efficiencies upon immobilization in the Ca–DDVA and Zn–DDVA MOMs, as well as reasonable reusability in both composites. We then probed the structural basis of such differences using a representative enzyme and found enhanced restriction of enzymes in Zn–DDVA than in Ca–DDVA, which might have caused the activity difference. To the best of our knowledge, this is the first aqueous-phase, one-pot synthesis of a lignin-derived “green” enzyme@MOF/MOM platform that can host enzymes without any limitations on enzyme IEP, molecular weight, and substrate size. The different morphologies and crystallinities of the composites formed by Ca–DDVA and Zn–DDVA MOMs broaden their applications depending on the problem of interest. Our approach of enzyme immobilization not only improves the sustainability/reusability of almost all enzymes but also reduces/eliminates the use of non-sustainable resources. This synthesis method has a negligible environmental impact while the products are non-toxic to living things and the environment. The biocompatibility also makes it possible to carry out enzyme delivery/release for nutritional or biomedical applications via our “green” biocomposites.

更新日期：2021-05-28

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