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通过d带中心调控实现增强氧还原和甲醇氧化催化的超薄三元铂镍钌纳米线

Ultrathin ternary PtNiRu nanowires for enhanced oxygen reduction and methanol oxidation catalysis via d-band center regulation.

作者信息

Cai Guopu, Hua Chun, Ren Hongji, Yu Renqin, Xu Deying, Khan Muhammad Arif, Guo Jian, Sun Yu, Tang Ya, Qian Huidong, Xia Zhonghong, Ye Daixin, Zhang Jiujun, Zhao Hongbin

机构信息

Department of Chemistry, College of Sciences, Shanghai University, Shanghai 200444, PR China.

Department of Physics, College of Sciences, Shanghai University, Shanghai 200444, PR China.

出版信息

J Colloid Interface Sci. 2025 Jan 15;678(Pt B):599-608. doi: 10.1016/j.jcis.2024.09.054. Epub 2024 Sep 7.

Abstract

Direct methanol fuel cells rely on the efficiency of their anode/cathode electrocatalysts to facilitate the methanol oxidation reaction and oxygen reduction reaction, respectively. Platinum-based nanocatalysts are at the forefront due to their superior catalytic properties. However, the high-cost, scarcity, and low CO tolerance of platinum pose challenges for the scalable application of DMFCs. Herein, we report novel ultrathin ternary PtNiRu alloy nanowires to improve Pt utilization and CO tolerance. These novel electrocatalysts incorporate the oxophilic metal Ru into ultrathin PtNi nanowires, aiming to enhance the intrinsic activity of platinum while leveraging the long-term durability and high utilization efficiency provided by the bimetallic synergistic effect. The PtNiRu NWs significantly enhance both mass activity and specific activity for ORR, performing about 6.9 times and 3.9 times better than commercial Pt/C, respectively. After a rigorous durability test of 10,000 cycles, the PtNiRu NWs only exhibited a 25.2 % loss in mass activity. Additionally, for MOR, the MA and SA of PtNiRu NWs exceed that of Pt/C catalyst by 4.30 and 2.72 times, respectively, and exhibit exceptional resistance to CO poisoning. Theoretical insights from density functional theory calculations suggest that the introduction of Ru modulates the d-band center of the surface Pt atoms, which contributes to decreased binding strength of oxygenated species and an elevated dissolution potential, substantiating the enhanced performance metrics, and the durability enhancement stems from the stronger PtM bonds than those in PtNiRu NWs resulted from PtRu covalent interactions. These findings not only provide a new perspective on platinum-based nanocatalysts but also significantly advance the quest for more efficient and durable electrocatalysts for DMFCs, representing a substantial stride in fuel cell technology.

摘要

直接甲醇燃料电池依赖于其阳极/阴极电催化剂的效率,分别促进甲醇氧化反应和氧还原反应。基于铂的纳米催化剂因其优异的催化性能而处于前沿地位。然而,铂的高成本、稀缺性和低一氧化碳耐受性给直接甲醇燃料电池的可扩展应用带来了挑战。在此,我们报告了新型超薄三元铂镍钌合金纳米线,以提高铂的利用率和一氧化碳耐受性。这些新型电催化剂将亲氧金属钌引入超薄铂镍纳米线中,旨在提高铂的本征活性,同时利用双金属协同效应提供的长期耐久性和高利用效率。铂镍钌纳米线显著提高了氧还原反应的质量活性和比活性,分别比商业铂碳催化剂高出约6.9倍和3.9倍。经过10000次循环的严格耐久性测试后,铂镍钌纳米线的质量活性仅损失了25.2%。此外,对于甲醇氧化反应,铂镍钌纳米线的质量活性和比活性分别比铂碳催化剂高出4.30倍和2.72倍,并且对一氧化碳中毒表现出优异的抗性。密度泛函理论计算的理论见解表明,钌的引入调节了表面铂原子的d带中心,这有助于降低含氧物种的结合强度和提高溶解电位,证实了性能指标的提高,而耐久性的提高源于铂钌共价相互作用导致的铂镍钌纳米线中比铂镍更强的铂-金属键。这些发现不仅为基于铂的纳米催化剂提供了新的视角,也显著推进了对用于直接甲醇燃料电池的更高效、更耐用的电催化剂的探索,代表了燃料电池技术的重大进展。

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