Macroporous Interlayers Stabilize Long-Lived Hole Polarons in Organic Semiconductor Photoanodes

IF 17.5 1区材料科学 Q1 CHEMISTRY, PHYSICAL

ACS Energy Letters Pub Date : 2026-10-20 DOI:10.1021/acsenergylett.6c02492

Eunsong Jeon,Gayoung Ham,Jin Su Park,Hoon Kim,Euimin Lee,Donghyun Lee,Hyuna Kim,Jun-Ho Yum,Kevin Sivula,Hyojung Cha,Han-Hee Cho

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Abstract

Integrating alternative oxidation reactions (AORs) into photoelectrochemical (PEC) systems is promising for unassisted hydrogen production and value-added chemical synthesis, yet organic semiconductor (OS) photoanodes suffer from poor charge extraction and short carrier lifetimes. Here, we address this bottleneck by stabilizing long-lived hole polarons through macroporous tin oxide (mcSnO2) interlayers. Transient absorption spectroscopy reveals that accelerated electron extraction through mcSnO2 stabilizes hole polaron states, substantially prolonging carrier lifetimes. Consequently, the optimized organic photoanodes outperform bare counterparts by more than 5.5-fold, retaining 74% of their initial photocurrent over 15 h for iodide oxidation and 61% over 35 h for ascorbic acid oxidation. Furthermore, integrating this robust organic photoanode with an OS-based photocathode enables the first bias-free organic PEC tandem cell coupling hydrogen evolution with AORs, delivering a remarkable solar-to-hydrogen conversion efficiency of 1.4%. These findings establish interfacial carrier lifetime engineering as an effective strategy for realizing high-performance and durable organic PEC systems.

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大孔间层稳定有机半导体光阳极的长寿命空穴极化子

将替代氧化反应（AORs）集成到光电化学（PEC）系统中，有望实现无辅助制氢和增值化学合成，但有机半导体（OS）光阳极存在电荷提取不良和载流子寿命短的问题。在这里，我们通过大孔氧化锡（mcSnO2）中间层稳定长寿命的空穴极化子来解决这一瓶颈。瞬态吸收光谱显示，通过mcSnO2加速电子萃取可以稳定空穴极化子态，大大延长载流子寿命。因此，优化后的有机光阳极的性能比裸阳极高出5.5倍以上，在碘化物氧化15小时内保持74%的初始光电流，在抗坏血酸氧化35小时内保持61%的初始光电流。此外，将这种强大的有机光阳极与基于os的光电阴极集成在一起，实现了第一个无偏置有机PEC串联电池，将氢与AORs耦合在一起，实现了1.4%的太阳能到氢转换效率。这些发现表明界面载流子寿命工程是实现高性能和耐用有机PEC系统的有效策略。

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来源期刊

ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment

CiteScore

31.20

自引率

5.00%

发文量

469

审稿时长

1 months

期刊介绍： ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.