In nature, green leaves accomplish photosynthesis via chloroplasts, where the Mg-N₄-centered chlorophyll and enzymes undertake light absorption and catalytic reaction, involving CO₂ fixation, with the resultant six-carbon compound, respectively. This intriguing phenomenon inspired us to design an artificial photosynthetic system that synergizes these dual attributes, a field that has remained largely unexplored. Herein, we developed a highly stable artificial chlorophyll-like nitrogen-decorated amorphous carbon material (Mg-NC) featuring abundant Mg-N₄ moieties (with high Mg content reaching ≈ 9.2 wt %), which simultaneously integrated the light-absorption center and catalytic reaction center to mimic natural photosynthesis of CO₂ valorization. As demonstrated, taking the photocatalytic CO₂ cycloaddition reaction as an example, the Mg-N₄ active center in Mg-NC played the role of an electronic donor, which could readily inject hot electrons into the adsorbed substrates, resulting in the swift formation of cyclic carbonate products. Remarkably, the as-designed Mg-NC exhibited outstanding photocatalytic CO₂ cycloaddition performance, achieving an impressive reaction rate up to 9.67 mmol·g⁻¹·h⁻¹ under mild conditions, which could be sustained even under gram scale conditions. Our current study offers an artificial biomimetic enzyme heterogeneous photocatalysis for CO₂ valorization.

在自然界中，绿叶通过叶绿体完成光合作用，其中以Mg-N ₄为中心的叶绿素和酶分别进行光吸收和催化反应，涉及CO ₂固定，并生成六碳化合物。这种有趣的现象启发我们设计一种人工光合作用系统来协同这些双重属性，这是一个很大程度上尚未探索的领域。在此，我们开发了一种高度稳定的人工叶绿素氮修饰无定形碳材料（Mg-NC），具有丰富的Mg-N ₄部分（Mg含量高达约9.2 wt%），该材料同时集成了光吸收中心和催化反应中心模拟自然光合作用的CO ₂增值。结果表明，以光催化CO ₂环加成反应为例，Mg-NC中的Mg-N ₄活性中心起到了电子供体的作用，可以很容易地将热电子注入到吸附的基质中，从而迅速形成环状碳酸酯产品。值得注意的是，所设计的Mg-NC表现出出色的光催化CO ₂环加成性能，在温和条件下实现了高达9.67 mmol·g ^-1 ·h ^-1的令人印象深刻的反应速率，甚至在克级条件下也能持续。我们目前的研究提供了一种用于CO ₂增值的人工仿生酶异质光催化。