Nannan Jiang, Hao Wang, Huihui Jin, Xuwei Liu and Lunhui Guan
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引用次数: 0
摘要
铂溶解是影响质子交换膜燃料电池(PEMFC)中氧还原反应(ORR)铂基催化剂稳定性的主要因素之一。如何防止铂溶解并提高铂基催化剂的耐久性是一项重大挑战。在本研究中,我们采用一步快速焦耳热冲击法制备了一种具有嵌入式 Pt5Ce 合金(E-Pt5Ce)的稳定 ORR 催化剂。铂-铈层之间强烈的催化剂-支撑相互作用抑制了颗粒团聚和奥斯特瓦尔德熟化,其立体阻碍效应降低了铂位点的电子密度,降低了铂与含氧中间产物的吸附能,防止了铂的溶解。Pt-C 层还增加了活性位点的可达性,提高了 ORR 活性。在酸性介质中,E-Pt5Ce 的质量活性(MA)和比活性(SA)分别为 2.86 A mgPt-1 和 2.03 mA cm-2,分别比商用 Pt/C 高出约 15 倍和 5 倍。在用作 PEMFC 阴极催化剂时,0.90 V 时的 MA 值几乎是 DOE 2025 目标值的两倍。经过稳定性测试,催化活性没有明显下降。密度泛函理论计算证实,Pt-C 配位键也是反应位点。这项工作揭示了铂-铂配位层的作用机理,这在 ORR 催化剂的制备和性能方面起着至关重要的作用。
Embedding the intermetallic Pt5Ce alloy in mesopores through Pt–C coordination layer interactions as a stable electrocatalyst for the oxygen reduction reaction†
Platinum dissolution is one of the primary factors affecting the stability of Pt-based catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). It is a significant challenge to prevent the dissolution of Pt and enhance the durability of Pt-based catalysts. In this study, we employed a one-step rapid Joule thermal shock method to fabricate a stable ORR catalyst with embedded Pt5Ce alloy (E-Pt5Ce). The strong catalyst-support interactions between the Pt–C layer suppress particle agglomeration and Ostwald ripening, and its steric hindrance effect reduces the electronic density at Pt sites, decreasing the adsorption energy of Pt with oxygen-containing intermediates and preventing Pt dissolution. The Pt–C layer also increases the accessibility of active sites, boosting the ORR activity. In acidic media, E-Pt5Ce shows a mass activity (MA) and specific activity (SA) of 2.86 A mgPt−1 and 2.03 mA cm−2, outperforming the commercial Pt/C by factors of approximately 15 and 5, respectively. When used as a cathode catalyst for a PEMFC, the MA at 0.90 V is almost twice the DOE 2025 target. After stability testing, there is no prominent loss in catalytic activity. Density functional theory calculations confirm that the Pt–C coordination bonds also serve as reactive sites. This work uncovers the mechanism of action of the Pt–C coordination layer, which plays a crucial role in the preparation and performance of ORR catalysts.