ZnIn2S4 单层中分离的单原子钴，用于 CO2 光固定,ACS Catalysis

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ZnIn2S4 单层中分离的单原子钴，用于 CO2 光固定
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-06-07 , DOI: 10.1021/acscatal.3c00992
Chang-Long Tan ₁ , Ming-Yu Qi ₁ , Zi-Rong Tang ₁ , Yi-Jun Xu ₁

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构建具有丰富反应位点的高活性光催化剂，用于用有机化合物光固定 CO _{2实现了 CO}₂增值和碳中和的环境友好途径。在此，我们报道了分离的钴 (Co) 单原子 (SA) 装饰的二维 (2D) 单层 ZnIn ₂ S ₄ (ZIS) 纳米片复合材料 (Co ^-s ZIS)，具有 Co 和 Zn 双活性中心用于在可见光下用环氧化物固定CO _{2 。}^{Co- s} ZIS的独特整体优化了光捕获，促进了载流子分离，并丰富了双功能活性位点，以有效吸附和活化环氧化物和 CO 的反应物₂ . 因此，与本体 ZIS 相比，Co- ^s ZIS 表现出显着改善的 CO _{2 -环氧化物环加成性能。}_{此外，同时利用光生电子和空穴的协同光氧化还原方式有效地促进了CO 2}和环氧化物的活化，从而进一步降低了CO ₂固定的能垒。这项工作不仅为 CO ₂增值提供了合理界面工程 SA-to-2D 半导体的范例，而且还强调了这个基于 SA 的混合平台中定义明确的活性位点的结构-活性关系。

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Isolated Single-Atom Cobalt in the ZnIn2S4 Monolayer with Exposed Zn Sites for CO2 Photofixation

Constructing highly active photocatalysts with rich reactive sites for photofixation of CO₂ with organic compounds implements an environmentally friendly route for CO₂ valorization and carbon neutralization. Herein, we report the isolated cobalt (Co) single-atom (SA)-decorated two-dimensional (2D) single-layer ZnIn₂S₄ (ZIS) nanosheet composites (Co-^sZIS) with dual active centers of Co and Zn for CO₂ fixation with epoxides under visible light. The unique ensemble of Co-^sZIS optimizes light harvesting, promotes charge carrier separation, and enriches the bifunctional active sites for the efficient adsorption and activation of the reactants of epoxides and CO₂. Consequently, the Co-^sZIS exhibits significantly improved CO₂-epoxide cycloaddition performance compared to bulk ZIS. In addition, the synergetic photoredox manner of simultaneously exploiting photogenerated electrons and holes efficiently facilitates the activation of CO₂ and epoxides, thereby further reducing the energy barrier of CO₂ fixation. This work not only provides a paradigm of rationally interfacial engineered SA-onto-2D semiconductors for CO₂ valorization but also highlights the structure–activity relationship by the well-defined active sites in this SA-based hybrid platform.

更新日期：2023-06-07

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