Aggregation induced emission (AIE) active molecules have emerged as a kind of unique and important functional materials of wide scientific and technical interests, but the photoelectrochemistry (PEC) of AIE-active molecules is still little understood to date. Herein, we investigate the first-time use of AIE-active molecules for PEC hydrogen production. Au nanoparticles (AuNPs) were electrodeposited on an indium tin oxide (ITO) electrode and AIE-active 1,1,2,2-tetrakis(4-(9H-carbazol-9-yl)phenyl)ethene (TCPE) was then electropolymerized to obtain a PTCPE/AuNPs/ITO photoanode (PTCPE = poly(TCPE)). Under 100 mW cm AM 1.5G simulated sunlight irradiation at a bias of 0 V vs RHE in 0.5 M aqueous NaSO containing 0.1 M ascorbic acid (AA), the photocurrent density of this photoanode was 1.32 mA cm (0.16 mA cm if simply without AA), which is notably higher than those of PTCPE/ITO (0.43 mA cm) and AuNPs/ITO (0.62 μA cm) control photoanodes. The excellent PEC performance is explained by the broadened light absorption range of PTCPE versus the monomer, the quenching of PTCPE fluorescence via the efficient electron transfer from the lowest unoccupied molecular orbital of PTCPE to AuNPs, and the consumption of the photogenerated holes on the highest occupied molecular orbital of PTCPE by AA, because all these factors can improve the separation and transfer of photogenerated charges. This work may have provided a reference for exploring new applications of AIE-active molecules and developing new PEC and photocatalysis materials.

中文翻译：

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基于聚集诱导发射活性1,1,2,2-四(4-(9H-咔唑-9-基)苯基)乙烯聚合物、Au纳米颗粒和抗坏血酸的光电化学产氢


聚集诱导发射（AIE）活性分子已成为一种具有广泛科学和技术兴趣的独特而重要的功能材料，但迄今为止，AIE活性分子的光电化学（PEC）仍然知之甚少。在此，我们研究了首次使用 AIE 活性分子来生产 PEC 氢气。将金纳米颗粒 (AuNPs) 电沉积在氧化铟锡 (ITO) 电极上，然后电聚合具有 AIE 活性的 1,1,2,2-四(4-(9H-咔唑-9-基)苯基)乙烯 (TCPE)获得 PTCPE/AuNPs/ITO 光电阳极（PTCPE = 聚（TCPE））。在含有 0.1 M 抗坏血酸 (AA) 的 0.5 M NaSO 水溶液中，在 100 mW cm AM 1.5G 模拟太阳光照射下，0 V vs RHE 的偏压下，该光电阳极的光电流密度为 1.32 mA cm（如果简单地没有 AA，则为 0.16 mA cm） ），明显高于 PTCPE/ITO (0.43 mA cm) 和 AuNPs/ITO (0.62 μA cm) 对照光电阳极。优异的 PEC 性能是通过 PTCPE 相对于单体的光吸收范围变宽、通过从 PTCPE 的最低未占分子轨道到 AuNP 的有效电子转移来猝灭 PTCPE 荧光以及消耗最高占据分子轨道上的光生空穴来解释的。通过AA对PTCPE的分子轨道进行修饰，因为所有这些因素都可以改善光生电荷的分离和转移。该工作可能为探索AIE活性分子的新应用以及开发新型PEC和光催化材料提供参考。