By analogy to mono-nuclear metalloenzymes, single-atom dispersed catalysts (SACs) demonstrate very promising performance for many conventional heterogeneous and homogeneous reactions. However, the prospect of integrating SACs with enzymatic catalysis is still unexplored. Herein, atomically dispersed Co sites on ultrathin two-dimensional carbon nitride nanosheets (Co₁/C₃N₄) were constructed and applied for efficiently photochemical cofactor (NADH) regeneration. The NADH regeneration yield reached as high as 99%. Subsequently, the in-situ regenerated-NADH triggered alcohol dehydrogenase for enzymatic reduction of aldehyde where 100% alcohol yield was achieved at room temperature. Using atomic spectroscopy characterization and theoretical calculation, the genuine active sites of Co₁/C₃N₄ catalyst in reaction system were revealed in the form of CoN₃-Cp* moieties (Cp*, 1,2,3,4,5-pentamethylcyclopentadiene). Such a well-defined atomic catalyst opens a new avenue for the organic transformation application of single-atom catalysts in enzyme catalysis.

与单核金属酶类似，单原子分散催化剂（SAC）对许多常规的异相和均相反应显示出非常有前途的性能。然而，将SAC与酶催化整合的前景仍未得到开发。在本文中，原子分散在超薄二维氮化碳纳米片（Co ₁ / C ₃ N ₄）上的Co位置被构建并应用于有效的光化学辅因子（NADH）再生。NADH的再生收率高达99％。随后，就地再生的NADH引发的醇脱氢酶用于醛的酶促还原，其中在室温下可获得100％的醇收率。使用原子光谱表征和理论计算，以CoN ₃ - Cp *部分（Cp *，1,2,3,4,5-）的形式揭示了反应体系中Co ₁ / C ₃ N ₄催化剂的真正活性位。五甲基环戊二烯）。这种定义明确的原子催化剂为单原子催化剂在酶催化中的有机转化应用开辟了新途径。