The development of efficient hydrogen evolution reaction (HER) electrocatalysts is critical for water splitting. Herein, rutile/anatase titanium dioxide heterojunction supported platinum nanoparticles (Pt-NPs) design with interfacial effect was developed as efficient HER catalyst (Pt@R/A-TiO2) over wide pH range. The R/A-TiO2 support design induces aggregated Pt-NPs on the heterojunction interface. In-situ Raman and in-situ infrared investigations over wide pH range reveal that there exists a strong hydrogen spillover from Pt-NPs to R/A-TiO2 support and fast proton transfer HER kinetics on Pt@R/A-TiO2. Theoretical calculations demonstrate that the R/A-TiO2 heterojunction modulates more electrons transferred from TiO2 support to Pt-NPs, and this electron-rich Pt-NPs weakens H adsorption, thus enhancing the hydrogen spillover effect and improving the HER performance of Pt@R/A-TiO2. In acidic/alkaline/neutral media, Pt@R/A-TiO2 demonstrates excellent HER activity and stability. Especially in acidic media, Pt@R/A-TiO2 exhibits high mass activity of 12.57 A mgPt−1 at an overpotential of 100 mV, which is nearly 11 times higher than Pt/C, and outperforms the recently reported Pt-based catalysts as well. This work advances the design of efficient and stable HER catalysts over wide pH range.

中文翻译：

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二氧化钛异质结支撑设计在宽 pH 范围内诱导强劲的铂催化析氢


高效析氢反应（HER）电催化剂的开发对于水分解至关重要。在此，金红石/锐钛矿二氧化钛异质结支持的具有界面效应的铂纳米颗粒（Pt-NPs）设计被开发为在宽pH范围内的高效HER催化剂（Pt@R/A-TiO2）。 R/A-TiO2 支撑设计会在异质结界面上诱导聚集的 Pt-NP。在较宽 pH 范围内的原位拉曼和原位红外研究表明，存在从 Pt-NP 到 R/A-TiO2 载体的强烈氢溢出以及 Pt@R/A-TiO2 上的快速质子转移 HER 动力学。理论计算表明，R/A-TiO2异质结调节了更多的电子从TiO2载体转移到Pt-NPs，这种富电子的Pt-NPs削弱了H吸附，从而增强了氢溢出效应，提高了Pt@R的HER性能/A-TiO2。在酸性/碱性/中性介质中，Pt@R/A-TiO2表现出优异的HER活性和稳定性。特别是在酸性介质中，Pt@R/A-TiO2在100 mV的过电势下表现出12.57 A mgPt−1的高质量活性，比Pt/C高出近11倍，并且优于最近报道的Pt基催化剂：出色地。这项工作推进了在宽 pH 范围内高效、稳定的 HER 催化剂的设计。