Liu Xinmei, Sun Xingwang, Zhou Xue, Wang Yu, Liu Gang, Yang Wenglong
Harbin University of Science and Technology, China.
Harbin University of Science and Technology, China.
Environ Res. 2025 Feb 15;267:120662. doi: 10.1016/j.envres.2024.120662. Epub 2024 Dec 18.
The electrocatalytic mechanisms of electrocatalysts were constrained by the disparities between the genuine catalytic interface and construction interface. This work demonstrated the relationship between the CuPt nano-alloy atomic ratios and their catalytic performance. Firstly, we developed a facile synthesis of surfactant-free CuPt nano-alloys with tunable Cu atomic ratios (ranging from 35 to 72 at%) under ambient conditions. Considering no surfactant-free was applied, surface active sites were uncovered, which was beneficial to ensured consistency between the calculated interface and the actual interface. Based on the experiment and calculation, the relationship between the Pt loading rate and electrocatalytic activity of CuPt nano-alloy toward hydrogen evolution reaction (HER) was systematically investigated. Under the acidic media, the over-potential by CuPt was 7.17 mV, which was 11.5% by the pure Pt nano-particles (NPs). The lower over-potential could be derived from a favorable d-band center of CuPt, which accelerated the adsorption and desorption of H. The correlation between the d-band center and the electrocatalytic activity of CuPt nano-alloy was investigated. Benefiting from the surfactant-free surface, the CuPt nano-alloy exhibited a favorable electrocatalytic activity toward methanol detection. With the increase in methanol concentration, the anodic peak for methanol oxidation was linearly increased. The linear relationship endowed the CuPt nano-alloy with a favorable sensor performance. It is suggested that the CuPt nano-alloy with a higher Pt atomic ratio showed a wider detection range and the CuPt nano-alloy with a higher Cu atomic ratio showed an enhanced sensitivity. The superior sensor performances could also be utilized for ethanol detection. This work demonstrated the favorable performance of the surfactant-free CuPt nano-alloy toward hydrogen generation and alcoholic solution (methanol and ethanol) detection. Considering the experiential results were agreed well with calculation, this work pave the way for designing cost-effective electrocatalysis by optimizing its d band center and maximized active sites.
电催化剂的电催化机制受到真实催化界面与构建界面之间差异的限制。这项工作展示了CuPt纳米合金原子比与其催化性能之间的关系。首先,我们在环境条件下开发了一种简便的合成方法,可制备出具有可调铜原子比(范围为35至72原子%)的无表面活性剂CuPt纳米合金。由于未使用无表面活性剂,表面活性位点得以暴露,这有利于确保计算界面与实际界面之间的一致性。基于实验和计算,系统研究了CuPt纳米合金对析氢反应(HER)的铂负载率与电催化活性之间的关系。在酸性介质下,CuPt的过电位为7.17 mV,而纯铂纳米颗粒(NPs)的过电位为11.5%。较低的过电位可归因于CuPt有利的d带中心,这加速了氢的吸附和解吸。研究了CuPt纳米合金的d带中心与电催化活性之间的相关性。得益于无表面活性剂的表面,CuPt纳米合金对甲醇检测表现出良好的电催化活性。随着甲醇浓度的增加,甲醇氧化的阳极峰呈线性增加。这种线性关系赋予了CuPt纳米合金良好的传感器性能。结果表明,具有较高铂原子比的CuPt纳米合金具有更宽的检测范围,而具有较高铜原子比的CuPt纳米合金具有更高的灵敏度。这种优异的传感器性能也可用于乙醇检测。这项工作展示了无表面活性剂CuPt纳米合金在制氢和酒精溶液(甲醇和乙醇)检测方面的良好性能。考虑到实验结果与计算结果吻合良好,这项工作为通过优化其d带中心和最大化活性位点来设计具有成本效益的电催化铺平了道路。