Chinese Journal of Catalysis ›› 2024, Vol. 61: 205-214.DOI: 10.1016/S1872-2067(24)60039-2

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Enhancement of H2O2 generation rate in porphyrin photocatalysts via crystal facets regulation to create strong internal electric field

Yunhang Shaoa,b, Yaning Zhanga,b, Chaofeng Chena,b, Shuai Doua,b, Yang Loua,b, Yuming Donga,b, Yongfa Zhuc, Chengsi Pana,b,*()   

  1. aKey Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, Jiangsu, China
    bInternational Joint Research Center for Photoresponsive Molecules and Materials, Jiangnan University, Wuxi 214122, Jiangsu, China
    cDepartment of Chemistry, Tsinghua University, Beijing 100084, China
  • Received:2024-01-25 Accepted:2024-04-10 Online:2024-06-18 Published:2024-06-20
  • Contact: * E-mail: cspan@jiangnan.edu.cn (S. Pan).
  • Supported by:
    National Natural Science Foundation of China(22172065);National Natural Science Foundation of China(21908079);National Natural Science Foundation of China(21676123);National Natural Science Foundation of China(21902009);National Natural Science Foundation of China(21707052);National Natural Science Foundation of China(U21A20326);Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(BK20220023);National Key R&D Program of China(2021YFB3501900);Jiangsu Specially-Appointed Professor(1046010241211400)

Abstract:

Three TCPP porphyrin-based nanosheet photocatalysts with exposed (400), (022), and (020) planes were synthesized using a dissolution-recrystallization method in a mixture of water and tetrahydrofuran (THF), methanol (MeOH), and ethylene glycol (EG). The TCPP photocatalyst with the exposed (400) surface exhibited the highest H2O2 production rate of 29.33 mmol L‒1 h‒1 g‒1 from only H2O and O2, surpassing the rates observed for ones with exposed (022) and (020) surfaces by factors of 2.7 and 4.1, respectively, and 1.3 times as that of the reported TCPP prepared by a base/acid self-assembling method. This enhancement can be attributed to the strong internal electric field and high carboxyl group content on the (400) surface, which hindered rapid charge recombination and facilitated challenging water oxidation. Hence, successful manipulation of porphyrin exposure to robust IEF planes enhances the photocatalytic activity of the system and provides valuable insights for the design and development of more efficient organic photocatalysts.

Key words: Internal electric field, Facet control, Nanosheet, H2O2 generation, Porphyrin