g-C3N4 与 2,4,6-三(4-氨基苯基)-1,3,5-三嗪通过 π-π 相互作用增强可见光光催化水分解产氢,Catalysis Science & Technology

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g-C3N4 与 2,4,6-三(4-氨基苯基)-1,3,5-三嗪通过 π-π 相互作用增强可见光光催化水分解产氢
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-08-23 , DOI: 10.1039/d3cy00837a
Chen-Chuang Li ₁ , Ikram Ullah ₁ , Gang Wang ₁ , An-Wu Xu ₁

Affiliation

石墨氮化碳（gC ₃ N ₄）是可见光下用于太阳能转化燃料生产的最有前途的无金属光催化剂中最有吸引力的候选者。然而，低光催化性能和光生载流子的快速复合速率阻碍了其实际应用。_{因此，gC 3} N ₄与适当材料的结合对于提高H ₂产量是非常需要的。_{在这项工作中，我们报道了一种由 gC 3} N ₄形成的 TAPT/CN 复合光催化剂2,4,6-三(4-氨基苯基)-1,3,5-三嗪(TAPT)通过π-π相互作用和氢键增强光催化活性。小 TAPT 分子充当空穴中继，从而提高空穴从 gC ₃ N ₄到三乙醇胺 (TEOA) 的转移速率；这反过来又有利于更多的电子转移到 Pt 助催化剂，并最终促进可见光驱动的 H ₂生成。实验结果表明，TAPT/CN纳米异质结构中的TAPT分子大大提高了光催化活性。优化后的5% TAPT/CN（5 wt% TAPT负载）样品的最大H ₂析出速率为99.54 μmol h ^-1，比裸gC ₃ N高7.1倍₄（14.01μmol h^-1）。此外，在长达20小时的连续可见光照射的五个连续循环后，_{H 2}产量没有显着下降_{我们预计这项研究将为设计其他有机材料装饰的 gC 3} N₄光催化剂打开大门，以用于太阳能到氢能转换的潜在应用。

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g-C3N4 coupled with 2,4,6-tris(4-aminophenyl)-1,3,5-triazine via π–π interactions enhanced visible-light photocatalytic H2 evolution from water splitting

Graphitic carbon nitride (g-C₃N₄) is an attractive candidate among the most promising metal-free photocatalysts under visible light for solar-to-fuel production. Nevertheless, the low photocatalytic performance and fast recombination rate of photoinduced charge carriers prevent its practical applications. Therefore, the integration of g-C₃N₄ with an appropriate material is highly desirable for enhancing H₂ production. In this work, we report a TAPT/CN composite photocatalyst formed from g-C₃N₄ and 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT) through π–π interactions and hydrogen bonds to enhance the photocatalytic activity. The small TAPT molecules act as a hole relay and thus elevate the transfer rate of holes from g-C₃N₄ to triethanolamine (TEOA); this in turn favors more electron transfer to the Pt cocatalyst and finally promotes the visible-light-driven H₂ generation. The experimental results display that photocatalytic activity is greatly boosted by TAPT molecules in TAPT/CN nanoheterostructures. The optimized 5% TAPT/CN (5 wt% TAPT loading) sample achieves a maximum H₂ evolution rate of 99.54 μmol h⁻¹, which is 7.1 times higher than that of bare g-C₃N₄ (14.01 μmol h⁻¹). Additionally, there is no significant decrease in H₂ production after five consecutive cycles of continuous visible-light irradiation of up to 20 hours. We expect that this research will open the door to designing other organic material-decorated g-C₃N₄ photocatalysts for potential applications in solar-to-hydrogen energy conversion.

更新日期：2023-08-23

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