Burns Cathal, Woodford Owen, Stephens Susanna L, Rishan Muhammed, Fuller Linsey, Kalathil Shafeer, Gibson Elizabeth A
Faculty of Health and Life Sciences, Department of Applied Sciences, Northumbria University, Newcastle, NE1 8ST, UK.
Energy Materials Laboratory, Chemistry, School of Natural and Environmental Sciences, Newcastle University, Newcastle upon Tyne, NE1 7RU, UK.
Dalton Trans. 2025 Jan 13;54(3):920-933. doi: 10.1039/d4dt02738h.
This article reports the development of CuO|CuBiO photocathodes stabilized by protective layers of TiO, MgO, or NiO, with Pt or MoS nanoparticles serving as co-catalysts to facilitate H evolution. Most notably, this work demonstrates the first application of MgO as a protection/passivation layer for photocathodes in a water-splitting cell. All configurations of photocathodes were studied structurally, morphologically, and photoelectrochemically revealing that CuO|CuBiO|MgO|Pt photocathodes achieve the highest stable photocurrent densities of -200 μA cm for over 3 hours with a Faradaic efficiency of ∼90%. Bias-free tandem water splitting was then performed by pairing this photocathode with a dye-sensitized TiO photoanode, producing H from neutral water without an external bias. This paper demonstrates key stability findings and proposes the use of spin-coated MgO, TiO, and NiO as feasible earth-abundant protective materials to aid in the formation of a cheap and scalable tandem water splitting system. Charge transfer dynamics have also been probed by combining spectroelectrochemistry and transient absorption spectroscopy.
本文报道了通过TiO、MgO或NiO保护层稳定的CuO|CuBiO光阴极的发展情况，其中Pt或MoS纳米颗粒作为助催化剂以促进析氢反应。最值得注意的是，这项工作展示了MgO作为光电解槽中光阴极的保护/钝化层的首次应用。对所有光阴极配置进行了结构、形态和光电化学研究，结果表明，CuO|CuBiO|MgO|Pt光阴极在超过3小时内实现了最高稳定光电流密度-200 μA/cm²，法拉第效率约为90%。然后通过将该光阴极与染料敏化TiO光阳极配对进行无偏压串联水分解，在无外部偏压的情况下从中性水中产生氢气。本文展示了关键的稳定性研究结果，并提出使用旋涂的MgO、TiO和NiO作为可行的储量丰富的保护材料，以帮助形成廉价且可扩展的串联水分解系统。还通过结合光谱电化学和瞬态吸收光谱对电荷转移动力学进行了研究。
