Guo Yan, Zhu Bowen, Tang Chuyang Y, Zhou Qixin, Zhu Yongfa
Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Department of Civil Engineering, The University of Hong Kong, Hong Kong, 999077, China.
Nat Commun. 2024 Jan 10;15(1):428. doi: 10.1038/s41467-024-44700-w.
Rapid mass transfer in solid-solid reactions is crucial for catalysis. Although phoretic nanoparticles offer potential for increased collision efficiency between solids, their implementation is hindered by limited interaction ranges. Here, we present a self-driven long-range electrophoresis of organic nanocrystals facilitated by a rationally designed photogenerated outer electric field (OEF) on their surface. Employing perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecular nanocrystals as a model, we demonstrate that a directional OEF with an intensity of 13.6-0.4 kV m across a range of 25-200 μm. This OEF-driven targeted electrophoresis of PTCDA nanocrystals onto the microplastic surface enhances the activity for subsequent decomposition of microplastics (196.8 mg h) into CO by solid-solid catalysis. As supported by operando characterizations and theoretical calculations, the OEF surrounds PTCDA nanocrystals initially, directing from the electron-rich (0 1 1) to the hole-rich [Formula: see text] surface. Upon surface charge modulation, the direction of OEF changes toward the solid substrate. The OEF-driven electrophoretic effect in organic nanocrystals with anisotropic charge enrichment characteristics indicates potential advancements in realizing effective solid-solid photocatalysis.
固-固反应中的快速传质对催化作用至关重要。尽管泳动纳米颗粒为提高固体间的碰撞效率提供了潜力，但其应用受到相互作用范围有限的阻碍。在此，我们展示了一种由在有机纳米晶体表面合理设计的光生外电场（OEF）促进的自驱动长程电泳。以苝-3,4,9,10-四羧酸二酐（PTCDA）分子纳米晶体为模型，我们证明了在25 - 200μm范围内强度为13.6 - 0.4 kV m的定向OEF。这种OEF驱动的PTCDA纳米晶体向微塑料表面的靶向电泳提高了随后通过固-固催化将微塑料分解为CO（196.8 mg h）的活性。经原位表征和理论计算支持，OEF最初围绕PTCDA纳米晶体，从富电子的（0 1 1）面指向富空穴的[化学式：见原文]面。在表面电荷调制后，OEF的方向朝固体基质改变。具有各向异性电荷富集特性的有机纳米晶体中的OEF驱动电泳效应表明在实现有效的固-固光催化方面有潜在进展。
