Kazemi Shahrzad, Alsaleh Ajyal Z, Karr Paul A, D'Souza Francis
Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, Texas 76203-5017, United States.
Department of Physical Sciences and Mathematics, Wayne State College, 1111 Main Street, Wayne, Nebraska 68787, United States.
J Am Chem Soc. 2024 May 15;146(19):13509-13518. doi: 10.1021/jacs.4c02972. Epub 2024 May 6.
The importance of diameter-sorted single-wall carbon nanotubes (SWCNTs) noncovalently bound to a donor-acceptor , , in prolonging the lifetime of charge-separated states is successfully demonstrated. For this, using a multistep synthetic procedure, a wide-band capturing, multimodular, C-bisstyrylBODIPY-(zinc porphyrin), , was newly synthesized and shown to bind diameter-sorted SWCNTs. The and its supramolecular assemblies were characterized by a suite of physicochemical techniques. Free-energy calculations suggested that both the (6,5) and (7,6) SWCNTs bound to act as hole acceptors during the photoinduced sequential electron transfer events. Consequently, selective excitation of in :SWCNT hybrids revealed a two-step electron transfer, leading to the formation of charge-separated states. Due to the distant separation of the cation and anion radical species within the supramolecules, improved lifetimes of the charge-separated states could be achieved. The present supramolecular strategy of improving charge separation involving SWCNTs and donor-acceptor highlights the potential application of these hybrid materials for various light energy harvesting and optoelectronic applications.
成功证明了与供体 - 受体非共价结合的直径分级单壁碳纳米管（SWCNT）在延长电荷分离态寿命方面的重要性。为此，采用多步合成程序，新合成了一种宽带捕获、多模块的C - 双苯乙烯基BODIPY -（锌卟啉），并证明其能与直径分级的SWCNT结合。通过一系列物理化学技术对其及其超分子组装体进行了表征。自由能计算表明，与结合的（6,5）和（7,6）SWCNT在光诱导的顺序电子转移过程中均充当空穴受体。因此，在：SWCNT杂化物中对进行选择性激发揭示了两步电子转移，导致电荷分离态的形成。由于超分子内阳离子和阴离子自由基物种的远距离分离，可以实现电荷分离态寿命的延长。目前涉及SWCNT和供体 - 受体的改善电荷分离的超分子策略突出了这些杂化材料在各种光能收集和光电子应用中的潜在应用。
