Charge-Transfer Cocrystal via a Persistent Radical Cation Acceptor for Efficient Solar-Thermal Conversion.
Charge-Transfer Cocrystal via a Persistent Radical Cation Acceptor for Efficient Solar-Thermal Conversion.
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通过持久性自由基阳离子受体进行电荷转移共晶体，实现高效的太阳热转换。
DOI：
10.1002/anie.202202571
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发表时间：
2022
影响因子：
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通讯作者：
Weihong Tan
中科院分区：
文献类型：
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作者：
Jieqiong Xu;Qian Chen;Shengkai Li;Jiachao Shen;Phouphien Keoingthong;Liang Zhang;Zhiwei Yin;Xinqi Cai;Zhuo Chen;Weihong Tan
设计有机电荷转移（CT）共晶用于有效的太阳能热转换是一个长期追求的目标，但仍然具有挑战性。在这里，我们构建了一个独特的CT共晶体，使用持久的2，2 '-连氮基-双（3乙基苯并噻唑啉-6-磺酸）自由基阳离子（ABTS +·）作为电子受体。ABTS +·的强电子亲和势和强余辉使ABTS +·与3，3 '，5，5'-四甲基联苯胺之间的电子离域程度较高。结合ABTS +·的固有长波长吸收，合成的共晶体可以有效地捕获整个太阳光谱，并显示出优异的光热效率。这种共晶进一步用于太阳能驱动的界面蒸发，并且在1个太阳照射下获得了1.407kgm-2 h-1的高蒸发速率和97.0%的显著的太阳能-蒸汽效率。这一工作预示着通过合理的自由基阳离子工程实现电荷转移功能材料的巨大前景。
Designing organic charge-transfer (CT) cocrystals for efficient solar-thermal conversion is a long-sought goal but remains challenging. Here we construct a unique CT cocrystal by using persistent 2,2'-azino-bis (3 ethylbenzothiazoline-6-sulfonic acid) radical cation (ABTS +• ) as the electron acceptor. The strong persistency and electron affinity of ABTS +• endow a high degree of electron delocalization between ABTS +• and 3,3',5,5'-tetramethylbenzidine donor. Together with the intrinsic long-wavelength absorption of ABTS +• , the synthesized cocrystal can effectively capture the full solar spectrum and show distinguished photothermal efficiency. Such cocrystal is further used for solar-driven interfacial evaporation, and a high evaporation rate of 1.407 kg m -2 h -1 and a remarkable solar-to-vapor efficiency of 97.0% have been achieved upon 1 sun irradiation. This work indicates the enormous prospects for charge transfer-based functional materials through rational radical cations engineering.