Yeung Celine Wing See, Andrei Virgil, Lee Tack Ho, Durrant James Robert, Reisner Erwin
Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK.
Optoelectronics Group, Cavendish Laboratory, University of Cambridge, JJ Thomson Avenue, Cambridge, CB3 0HE, UK.
Adv Mater. 2024 Aug;36(35):e2404110. doi: 10.1002/adma.202404110. Epub 2024 Jul 15.
Photoelectrochemical (PEC) devices offer a promising platform toward direct solar light harvesting and chemical storage through artificial photosynthesis. However, most prototypes employ wide bandgap semiconductors, moisture-sensitive inorganic light absorbers, or corrosive electrolytes. Here, the design and assembly of PEC devices based on an organic donor-acceptor bulk heterojunction (BHJ) using a carbon-based encapsulant are introduced, which demonstrate long-term H evolution and CO reduction in benign aqueous media. Accordingly, PCE10:EH-IDTBR photocathodes display long-term H production for 300 h in a near-neutral pH solution, whereas photocathodes with a molecular CO reduction catalyst attain a CO:H selectivity of 5.41±0.53 under 0.1 sun irradiation. Their early onset potential enables the construction of tandem PCE10:EH-IDTBR - BiVO artificial leaves, which couple unassisted syngas production with O evolution in a reactor completely powered by sunlight, sustaining a 1:1 ratio of CO to H over 96 h of operation.
光电化学（PEC）装置为通过人工光合作用直接收集太阳光并进行化学储能提供了一个很有前景的平台。然而，大多数原型采用宽带隙半导体、对湿度敏感的无机光吸收剂或腐蚀性电解质。在此，介绍了基于有机供体-受体体异质结（BHJ）并使用碳基密封剂的PEC装置的设计与组装，这些装置在良性水性介质中展示了长期的析氢和一氧化碳还原性能。因此，PCE10:EH-IDTBR光阴极在近中性pH溶液中能持续300小时长期产氢，而含有分子一氧化碳还原催化剂的光阴极在0.1个太阳光照下的一氧化碳与氢气选择性达到5.41±0.53。它们的起始电位使得能够构建串联的PCE10:EH-IDTBR - BiVO人工叶片，该人工叶片在完全由太阳光驱动的反应器中将无辅助合成气生产与析氧过程相结合，在96小时的运行过程中保持一氧化碳与氢气1:1的比例。
