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.

中文翻译：

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一种 H2O2 生成-检测-调节集成平台，用于提高过加氧酶催化的 C-H 氧化羟基化反应的效率


过加氧酶是稳定 C-H 键选择性氧官能化的理想生物催化剂。然而，由于酶对氧化剂 H 2 O 2 的不稳定性，这种方法的催化效率受到限制。尽管报道的原位 H₂O₂ 生成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，但过加氧酶的最大催化潜力仍然无法有效实现。为解决上述问题，首先开发了一个 H₂O₂ 生成检测调控平台，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 调控策略。 首先通过简单地调整有机催化剂的量来获得 H 2 O 2 生成速率的合适范围，以最大限度地提高过加氧酶的催化效率，同时最大限度地减少酶的失活。根据确定的合适范围，每种底物的过加氧酶的 C-H 氧官能化效率显着提高，达到报告的最高周转频率的 3 倍。