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Ca-Doped PrFeO3 Photocathodes with Enhanced Photoelectrochemical Activity
Solar RRL ( IF 6.0 ) Pub Date : 2024-05-29 , DOI: 10.1002/solr.202400308
Bradley Francis Lewis 1 , Chenhao Huang 1 , Ioanna Itskou 2 , Giuseppe Mallia 3 , Nicholas M. Harrison 3 , Jamie Southouse 4 , Salvador Eslava 1
Affiliation  

Perovskite oxides, renowned for their adaptable structure and optoelectronic characteristics, hold significant potential for applications in catalysis and photoelectrochemical (PEC) processes. In this research, the preparation of praseodymium iron oxide (PrFeO3) by spin coating and the impact of incorporating a calcium (Ca) dopant on its PEC efficacy as photocathodes are investigated. Spin coating of a polymer containing sol–gel yields thin films with uniform morphology and porosity, facilitating effective semiconductor/electrolyte interactions, as characterized by scanning electron microscopy analyses. Evaluation of transient photocurrent responses reveals that introducing Ca at a 5 at% doping level significantly enhances the PEC activity of PrFeO3, resulting in an optimal photocurrent of −124 μA cm−2 at +0.43 V vs. a reversible hydrogen electrode (VRHE) under simulated sunlight conditions. This enhancement is accompanied by an incident photon-to-current efficiency (IPCE) of 3.8% at +0.43 VRHE and 350 nm, along with an onset potential of +1.1 VRHE. Ultraviolet and visible spectroscopy analyses indicate an increase in light-absorption capabilities in the Ca-doped films and a noticeable reduction in bandgap compared to the undoped counterparts, further supported by IPCE measurements. In the findings, the significant role of dopants in augmenting the photocurrent performance of stable perovskite oxides, highlighting their potential in advancing photon conversion technologies, is underscored.

中文翻译:


具有增强光电化学活性的钙掺杂 PrFeO3 光阴极



钙钛矿氧化物以其适应性强的结构和光电特性而闻名,在催化和光电化学(PEC)过程中具有巨大的应用潜力。在本研究中,研究了旋涂法制备氧化镨铁氧化物(PrFeO 3 )以及掺入钙(Ca)掺杂剂对其作为光电阴极的PEC效能的影响。含有溶胶-凝胶的聚合物的旋涂可产生具有均匀形态和孔隙率的薄膜,促进有效的半导体/电解质相互作用,如扫描电子显微镜分析所表征。瞬态光电流响应的评估表明,引入 5 at% 掺杂水平的 Ca 显着增强了 PrFeO 3 的 PEC 活性,在 + 时产生 -124 μA cm −2 的最佳光电流模拟阳光条件下,0.43 V vs. 可逆氢电极 (V RHE )。这种增强伴随着 +0.43 V RHE 和 350 nm 处 3.8% 的入射光子电流效率 (IPCE),以及 +1.1 V RHE 的起始电位。紫外和可见光谱分析表明,与未掺杂的薄膜相比,Ca 掺杂薄膜的光吸收能力增加,带隙显着减小,IPCE 测量进一步支持了这一点。研究结果强调了掺杂剂在增强稳定钙钛矿氧化物的光电流性能方面的重要作用,突显了它们在推进光子转换技术方面的潜力。
更新日期:2024-05-29
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