非金属等离子体诱导的载流子回流和延长的二氧化碳光还原寿命

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Peiyu Hu, Jianjun Zhang, Guijie Liang, Jiaguo Yu, Feiyan Xu
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引用次数: 0

摘要

通过局部表面等离子体共振(LSPR)效应分离电子/空穴对并改善光吸收,构建涉及贵金属协同催化剂的传统异质结是提高光催化效率的一种行之有效的策略。然而,贵金属的高成本和有限供应限制了它们的应用,而等离子体效应对电荷载流子动力学和寿命的影响(这对调节光催化性能至关重要)却一直被忽视。在此,我们提出将石墨碳点(CD)作为高效非金属协同催化剂集成到二氧化锡纳米纤维中,以促进高效光反应。在光照射下,SnO2 中的光电子在弯曲带和内部电场的驱动下迁移到 CD 上,与固有的自由电子一起,在 LSPR 效应的作用下激发成高能激发电子。飞秒瞬态吸收光谱证实,这些高能电子随后回流到二氧化锡以实现稳定,从而启动了一个循环过程,有效延长了二氧化锡/CDs 纳米杂化材料中载流子的寿命。由于 CD 促进了光学吸收和二氧化碳化学吸附的增强,由此产生的二氧化锡/CDs 纳米纤维显示出更好的二氧化碳光电还原性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Nonmetal Plasmon-Induced Carrier Backflow and Prolonged Lifetime for CO2 Photoreduction

Nonmetal Plasmon-Induced Carrier Backflow and Prolonged Lifetime for CO2 Photoreduction
Constructing traditional heterojunctions involving noble metal cocatalysts is a well-established strategy for boosting photocatalytic efficiency by separating electron/hole pairs and improving light absorption through localized surface plasmon resonance (LSPR) effects. However, the high cost and limited availability of noble metals constrain their application, while the impact of plasmon effects on charge carrier dynamics and lifetimes, crucial for regulating photocatalytic performance, has been overlooked. Here, we propose integrating graphitic carbon dots (CDs) as proficient nonmetal cocatalysts into SnO2 nanofibers to facilitate high-efficiency photoreactions. Under light irradiation, photoelectrons within the SnO2 migrate to the CDs driven by the bent bands and the internal electric field, alongside inherent free electrons, stimulating into high-energy excited electrons due to LSPR effects. These energized electrons subsequently backflow to the SnO2 for stabilization, initiating a cyclic process that effectively prolongs carrier lifetimes within the SnO2/CDs nanohybrids, as confirmed by femtosecond transient absorption spectroscopy. Synergizing with enhanced optical absorption and CO2 chemisorption facilitated by the CDs, the resulting SnO2/CDs nanofibers demonstrate improved CO2 photoreduction performance.
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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