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Synthesis of bay-substituted perylene diimide as bifunctional photocatalyst for enhanced water oxidation and hydrogen peroxide generation
Molecular Catalysis ( IF 4.6 ) Pub Date : 2024-04-08 , DOI: 10.1016/j.mcat.2024.114116
Bo Zhang , Shoufeng Wang , Shihao Min , Kang Li , Longtian Kang , Wenlie Lin

Rational design of semiconductor molecule structure is of significant importance for achieving the multifunctional photocatalysis. Herein, three end/bay-substituted perylenediimide (PDI) molecules, including bis(N-carboxymethyl) perylenediimide (HPDI), 1,7-dibromo-substituted HPDI (2Br-HPDI) and 1,6,7,12-tetraether-substituted HPDI (4CHCHO-HPDI), are synthesized for photocatalytic oxygen evolution (POE) and oxygen reduction reaction (ORR). One-dimensional HPDI nanorods, two-dimensional 2Br-HPDI nanosheets, and zero-dimensional 4CHCHO-HPDI nanoparticles are obtained. Under visible light, 4CHCHO-HPDI as photocatalyst (5.31 mmol·g·h) exhibits the 1.8-times and 20-times POE rate of 2Br-HPDI (2.93 mmol·g·h) and HPDI (0.26 mmol·g·h) with AgNO as sacrificial agent. Additionally, the POE rate can be further improved to 9.34 mmol·g·h with the Co doping of 4CHCHO-HPDI. With isopropanol as sacrificial agent, the HO evolution rate of 657.4 μM·g·h can be also achieved via photocatalytic ORR with 4CHCHO-HPDI as catalyst, which is ∼3 and ∼4 times those of 2Br-HPDI (220.8 μM·g·h) and HPDI (160.0 μM·g·h), respectively. Especially, in the O- or air- saturated aqueous solution without sacrificial agent, the HO rate of 273.1 or 112.7 μM·g·h can be also achieved. This work provides a promising way to design the PDI-based multifunctional photocatalysts.

中文翻译:

湾取代苝二酰亚胺双功能光催化剂的合成,用于增强水氧化和过氧化氢生成

半导体分子结构的合理设计对于实现多功能光催化具有重要意义。本文中,三个末端/海湾取代的苝二酰亚胺(PDI)分子,包括双(N-羧甲基)苝二酰亚胺(HPDI)、1,7-二溴取代的HPDI(2Br-HPDI)和1,6,7,12-四醚-合成取代的 HPDI (4CHCHO-HPDI),用于光催化析氧 (POE) 和氧还原反应 (ORR)。获得一维HPDI纳米棒、二维2Br-HPDI纳米片和零维4CHCHO-HPDI纳米粒子。在可见光下,4CHCHO-HPDI作为光催化剂(5.31 mmol·g·h)的POE速率是2Br-HPDI(2.93 mmol·g·h)和HPDI(0.26 mmol·g·h)的1.8倍和20倍以AgNO为牺牲剂。此外,通过4CHCHO-HPDI的Co掺杂,POE率可进一步提高至9.34 mmol·g·h。以异丙醇为牺牲剂,以4CHCHO-HPDI为催化剂,通过光催化ORR也能实现657.4 μM·g·h的H2O释放速率,是2Br-HPDI (220.8 μM·g·h)的~3和~4倍。 h) 和 HPDI (160.0 μM·g·h)。特别是,在没有牺牲剂的O-或空气饱和水溶液中,H2O速率也可以达到273.1或112.7 μM·g·h。这项工作为设计基于 PDI 的多功能光催化剂提供了一种有前景的方法。
更新日期:2024-04-08
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