A H2O2 generation-detection-regulation integrated platform for boosting the efficiency of peroxygenase-catalysed C–H oxidative hydroxylation

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Abstract

The peroxygenases are ideal biocatalysts for the selective oxyfunctionalisation of stable C–H bonds. However, the catalytic efficiency of this approach is limited due to enzyme lability toward oxidant H2O2. Although the reported in-situ H2O2 generation system enables the stable biocatalytic process without deactivating the enzyme, the greatest catalytic potential of peroxygenases still cannot be fulfilled effectively. To address the above issue, a H2O2 generation-detection-regulation platform that integrated an effective organocatalyst-driven H2O2 generation system, a precise electrochemical H2O2 real-time detection device, and a convenient H2O2 regulation strategy was first developed. The suitable range of H2O2 generation rate for maximizing the catalytic efficiency of peroxygenases while minimizing inactivation of the enzyme was firstly obtained by simply adjusting the amount of organocatalyst. According to the determined suitable range, the C–H oxyfunctionalisation efficiency of peroxygenases for each substrate was significantly boosted, achieving ∼3-fold of the reported highest turnover frequency.

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提高过氧酶催化C-H氧化羟基化效率的H2O2生成-检测-调控一体化平台
过氧酶是稳定碳氢键选择性氧化功能化的理想生物催化剂。然而,由于酶对氧化剂H2O2的不稳定性,这种方法的催化效率受到限制。虽然报道的原位生成H2O2系统能够在不使酶失活的情况下实现稳定的生物催化过程,但过氧酶的最大催化潜能仍然无法有效发挥。为了解决上述问题,首次开发了一种H2O2生成检测调节平台,该平台集成了有效的有机催化剂驱动的H2O2生成系统、精确的电化学H2O2实时检测装置和方便的H2O2调节策略。首先通过简单调整有机催化剂的用量,获得了使过氧酶的催化效率最大化,同时使酶失活最小化的H2O2生成速率的合适范围。根据确定的合适范围,每种底物的过氧酶的C-H氧化功能化效率显著提高,达到报道的最高周转频率的约3倍。
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