Kaisi Liu, Tongtong Liu, Xinyi Wu, Jiao Dai, Qingjun Chen, Jun Wan, Lei Liu
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引用次数: 0
摘要
碱性氢进化反应(HER)是可持续能源生产的关键,但由于必须通过水解离来提供质子,因而存在高能量障碍,导致动力学缓慢。为了克服这一挑战,我们提出了一种新方法,即在 CeO2 表面引入和调整氧空位,以构建和控制具有双活性位点的受挫路易斯对(FLPs),从而增强水解离。第一性原理计算显示,增加氧空位的数量可显著提高FLP位点的数量和活性,从而实现高效的水解离。在这些计算的指导下,我们合成了具有不同氧空位浓度的二维 CeO2 纳米片,结果表明空位含量最高的纳米片具有卓越的 HER 性能,过电位为 132 mV,Tafel 斜率为 73 mV-dec-1。这些发现验证了理论模型,并强调了具有 FLP 活性位点的二维 CeO2 作为有效、稳定的 HER 催化剂的潜力。这项研究有望为开发具有 FLP 活性位点的先进催化剂提供信息,用于碱性介质中的氢气进化反应。
Frustrated lewis pair chemistry in 2D CeO₂ for efficient alkaline hydrogen evolution
The alkaline hydrogen evolution reaction (HER) is pivotal for sustainable energy production but is hindered by sluggish kinetics due to the necessity of water dissociation to supply protons, which presents a high energy barrier. To overcome this challenge, a novel approach is proposed involving the introduction and tuning of oxygen vacancies on the surface of CeO2 to construct and control frustrated Lewis pairs (FLPs) with dual active sites for enhanced water dissociation. First-principles calculations reveal that increasing the number of oxygen vacancies significantly improves the quantity and activity of FLP sites for efficient water dissociation. Guided by these calculations, 2D CeO2 nanosheets with varying concentrations of oxygen vacancies were synthesized, showing that those with the highest vacancy content exhibit exceptional HER performance, with an overpotential of 132 mV and a Tafel slope of 73 mV·dec-1. These findings validate the theoretical model and underscore the potential of 2D CeO2 with FLP active sites as effective and stable HER catalysts. This study is anticipated to inform the development of advanced catalysts with FLP active sites for hydrogen evolution reactions in alkaline media.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.