Palladium-mediated hybrid biocatalysts with enhanced enzymatic catalytic performance via allosteric effects

Palladium-mediated hybrid biocatalysts with enhanced enzymatic catalytic performance via allosteric effects
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钯介导的杂化生物催化剂通过变构效应增强酶催化性能

DOI:
10.1016/j.jcis.2018.08.052
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发表时间:
2019
影响因子:
9.9
通讯作者:
Jiang Yanbin
Jiang Yanbin
中科院分区:
化学1区
文献类型:
--
作者:
Xia Huan;Zhong Xue;Li Zhixian;Jiang Yanbin

文献摘要

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几十年来,固定化酶的高活性和稳定性一直是人们不断追求和面临的严峻挑战。本文将细胞色素c(过氧化物酶,Cyt c)及其相应的酶模拟物(Pd纳米颗粒)结合并成功嵌入到沸石咪唑酸框架-8 (ZIF-8)中,利用仿生矿化方法增强酶催化性能。由于Cyt c- pd配合物的变构效应,与游离Cyt c相比,合成的Cyt c-Pd@ZIF-8复合材料表现出增加的周转次数(约2.4倍叉猫)和增强的催化效率(约2.3倍叉猫/KM);ZIF-8的屏蔽作用也使酶具有更好的抵抗恶劣条件(如高温和有机溶剂)的能力。该策略将酶与过渡金属纳米颗粒衍生的酶模拟物相结合,以提高酶的催化性能,可能为设计高效、多功能的生物催化剂提供一种通用、简便的技术。
High activity and stability of immobilized enzymes have been constant pursuits and critical challenges for decades. Herein, Cytochrome c (peroxidase, Cyt c) and its corresponding enzyme mimic (Pd nanoparticles) were combined and successfully embedded into a zeolitic imidazolate framework-8 (ZIF-8) to enhance the enzymatic catalytic performance using a biomimetic mineralization approach. Owing to allosteric effects of Cyt c-Pd complexes, the as-synthesized Cyt c-Pd@ZIF-8 composites exhibit an increased turnover number (approximately 2.4-fold forkcat) and an enhanced catalytic efficiency (approximately 2.3-fold forkcat/KM) compared to free Cyt c; also the shielding effect of ZIF-8 endows enzyme with improved resistance against harsh conditions (e.g. high temperatures and organic solvents). The strategy, which integrates enzyme with its enzyme mimic derived from transition metal nanoparticles to enhance enzymatic catalytic performances, may provide a versatile and facile technique for designing highly efficient and multi-functional bio-catalysts.