There is a need to design substrate-supported catalysts for the heterogeneous fields, especially with large porosity, which can facilitate mass transport. Herein, aiming at enhancing the performance of CO₂ fixation, a hollow carbon sphere-supported catalyst of Fe_NPs/HCS (Fe_NPs, Fe nanoparticles; HCS, hollow carbon sphere) is facilely designed and fabricated. Excitingly, the experimental and calculation results reveal that Fe_NPs/HCS displays an ultrahigh activity with almost complete conversions in CO₂ cycloaddition, surpassing the performance of Fe_NPs/CS (CS, carbon sphere); this demonstrates that the HCS plays a key role, which may be attributed to the hollow structure tuning the electron density and enhancing the enrichment of the substrate and CO₂, consequently lowering the barrier associated with mass transfer. The work not only provides a novel strategy to construct an efficient catalyst but also proposes, for the first time, an electron redistribution tactic to influence the catalytic process for CO₂ cycloaddition.

中文翻译：

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电子密度的重新分布促进 CO2 转化率


需要为非均相场设计衬底负载的催化剂，尤其是孔隙率大的催化剂，这可以促进质量传递。本文旨在提高 CO₂ 固定性能，一种 Fe_NPs/HCS（Fe_NPs、Fe 纳米颗粒;HCS，空心碳球）的设计和制造非常简单。令人兴奋的是，实验和计算结果表明，Fe_NPs/HCS 表现出超高活性，在 CO₂ 环加成反应中几乎完全转化，超过了 Fe_NPs/CS （CS，碳球）的性能;这表明 HCS 起着关键作用，这可能归因于中空结构调节了电子密度并增强了衬底和 CO₂ 的富集，从而降低了与传质相关的势垒。这项工作不仅提供了一种构建高效催化剂的新策略，还首次提出了一种电子再分布策略来影响 CO₂ 环加成反应的催化过程。