| Summary: | Photocatalytic hydrogen generation via water decomposition is a promising avenue in the pursuit of large-scale, cost-effective renewable hydrogen energy generation. However, the design of an efficient photocatalyst plays a crucial role in achieving high yields in hydrogen generation. Herein, we have engineered a fullerene-2,3,9,10,16,17,23,24-octa(octyloxy)copper phthalocyanine (C<sub>60</sub>-CuPcOC<sub>8</sub>) photocatalyst, achieving both efficient hydrogen generation and high stability. The significant donor–acceptor (D–A) interactions facilitate the efficient electron transfer from CuPcOC<sub>8</sub> to C<sub>60</sub>. The rate of photocatalytic hydrogen generation for C<sub>60</sub>-CuPcOC<sub>8</sub> is 8.32 mmol·g<sup>−1</sup>·h<sup>−1</sup>, which is two orders of magnitude higher than the individual C<sub>60</sub> and CuPcOC<sub>8</sub>. The remarkable increase in hydrogen generation activity can be attributed to the development of a robust internal electric field within the C<sub>60</sub>-CuPcOC<sub>8</sub> assembly. It is 16.68 times higher than that of the pure CuPcOC<sub>8</sub>. The strong internal electric field facilitates the rapid separation within 0.6 ps, enabling photogenerated charge transfer efficiently. Notably, the hydrogen generation efficiency of C<sub>60</sub>-CuPcOC<sub>8</sub> remains above 95%, even after 10 h, showing its exceptional photocatalytic stability. This study provides critical insight into advancing the field of photocatalysis.
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