Citation: Na Lu, Xuedong Jing, Yao Xu, Wei Lu, Kuichao Liu, Zhenyi Zhang. Effective Cascade Modulation of Charge-Carrier Kinetics in the Well-Designed Multi-Component Nanofiber System for Highly-Efficient Photocatalytic Hydrogen Generation[J]. Acta Physico-Chimica Sinica, ;2023, 39(4): 220704. doi: 10.3866/PKU.WHXB202207045 shu

Effective Cascade Modulation of Charge-Carrier Kinetics in the Well-Designed Multi-Component Nanofiber System for Highly-Efficient Photocatalytic Hydrogen Generation

Key Laboratory of New Energy and Rare Earth Resource Utilization of State Ethnic Affairs Commission; Key Laboratory of Photosensitive Materials and Devices of Liaoning Province, School of Physics and Materials Engineering, Dalian Minzu University, Dalian 116600, Liaoning Province, China

Corresponding author: Zhenyi Zhang, zhangzy@dlnu.edu.cn

^†

Received Date: 22 July 2022
Revised Date: 22 August 2022
Accepted Date: 30 August 2022
Available Online: 31 August 2022
Fund Project: the National Natural Science Foundation of China 62005036the National Natural Science Foundation of China 12074055the National Natural Science Foundation of China 11904046Natural Science Foundation of Liaoning Province for Excellent Young Scholars, China 2022-YQ-13Liaoning BaiQianWan Talents Program, China, Natural Science Foundation of Liaoning Province, China 2020-MZLH-15Program for Dalian Excellent Talents, China 2020RQ131

The photocatalytic reduction of water to hydrogen (H₂) over semiconductors potentially offers an economic way to alleviate the global energy crisis and environmental pollution. Optimal modulation of charge-carrier kinetics is of great importance for enhancing the photocatalytic activity of semiconductors for reducing water to green H₂. The design and manufacture of semiconductor-based heterostructure systems have emerged as promising tactics for modulating charge-carrier kinetics based on sensitization either via the semiconductor heterojunction effect or localized surface plasmon resonance. However, the cascade modulation of charge-carrier kinetics is still difficult to achieve through rationally coupling the abovementioned sensitization processes in well-designed heterostructures for highly-efficient photocatalytic H₂ generation. In this study, we developed a novel quaternary hetero-component nanofibers (HNFs) system by assembling plasmonic Ag nanoparticles (NPs) and two different semiconductors of Ag₂S NPs and g-C₃N₄ nanosheets (NSs) into the electrospun TiO₂ nanofibers (NFs) via in situ oxidation (for g-C₃N₄ exfoliation and Ag₂S) and reduction (for Ag) reactions. By combining time-resolved photoluminescence spectroscopy, three-dimensional finite-difference-time-domain simulation, and control experiments, we found that the overlapping absorption peak of plasmonic Ag NPs and g-C₃N₄ NSs could induce plasmonic resonant energy transfer from the Ag NPs to the neighboring g-C₃N₄, thereby improving the generation of photoinduced charge carriers of g-C₃N₄ in the quaternary HNFs system. Simultaneously, plasmonic hot electrons could be generated on the Ag NPs and transferred to the near-by hetero-components of TiO₂, g-C₃N₄, and Ag₂S, to boost the generation and separation of photoinduced charge carriers in the system. Furthermore, the energy band structure at the g-C₃N₄/TiO₂ hetero-interface belongs to the "type II" heterojunction, while the energy band structure at the TiO₂/Ag₂S hetero-interface can be classified as a "type I" heterojunction. This way, the successive "energy band step" could be constructed at the g-C₃N₄/TiO₂/Ag₂S hetero-interface, resulting in improved separation and migration of photoinduced charge carriers through the transfer of photoinduced electrons from g-C₃N₄ to Ag₂S across TiO₂. Thus, the plasmonic resonant energy transfer, hot electron transfer, and successive energy-band-step-induced charge separation processes were integrated into the as-synthesized quaternary Ag/Ag₂S/g-C₃N₄/TiO₂ HNFs system, thereby achieving the effective cascade modulation of the generation, separation, and migration of photoinduced charge carriers. As such, the photocatalytic H₂-generation rate of the optimal Ag/Ag₂S/g-C₃N₄/TiO₂ HNFs system was higher than that of the mechanically mixed TiO₂ NFs, g-C₃N₄ NSs, Ag NPs, and Ag₂S NPs, with the same amounts as the optimal Ag/Ag₂S/g-C₃N₄/TiO₂ HNFs photocatalyst, by approximately 9-fold under simulated sunlight irradiation. This interesting cascade modulation of charge-carrier kinetics might open new avenues for the development of highly active semiconductor-based heterostructure system for solar-to-fuels conversion.
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