Zhang Boyan, Ma Peiyu, Wang Ruyang, Cao Heng, Bao Jun
National Synchrotron Radiation Laboratory, Key Laboratory of Precision and Intelligent Chemistry, iChem (Collaborative Innovation Center of Chemistry for Energy Materials), University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Small. 2024 Dec;20(49):e2405234. doi: 10.1002/smll.202405234. Epub 2024 Oct 2.
Designing efficient and durable electrocatalysts for oxygen reduction reaction (ORR) is essential for proton exchange membrane fuel cells (PEMFCs). Platinum-based catalysts are considered efficient ORR catalysts due to their high activity. However, the degradation of Pt species leads to poor durability of catalysts, limiting their applications in PEMFCs. Herein, a Janus heterostructure is designed for high durability ORR in acidic media. The Janus heterostructure composes of crystalline platinum and cassiterite tin oxide nanoparticles with carbon support (J-Pt@SnO/C). Based on the synchrotron fine structure analysis and electrochemical investigation, the crystalline reconstruction and charge redistribution at the interface of Janus structure are revealed. The tightly coupled interface could optimize the valance states of Pt and the adsorption/desorption of oxygenated intermediates. As a result, the J-Pt@SnO/C catalyst possesses distinguishing long-term stability during the accelerated durability test without obvious degradation after 40 000 cycles and keeps the majority of activity after 70 000 cycles. Meanwhile, the catalyst exhibits outstanding activity with half-wave potential at 0.905 V and a mass activity of 0.355 A mg (2.7 times higher than Pt/C). The approach of the Janus catalyst paves an avenue for designing highly efficient and stable Pt-based ORR catalyst in the future implementation.
设计用于氧还原反应(ORR)的高效耐用的电催化剂对于质子交换膜燃料电池(PEMFC)至关重要。基于铂的催化剂因其高活性而被认为是高效的ORR催化剂。然而,铂物种的降解导致催化剂的耐久性较差,限制了它们在PEMFC中的应用。在此,设计了一种用于在酸性介质中实现高耐久性ORR的Janus异质结构。该Janus异质结构由结晶铂和具有碳载体的锡石型氧化锡纳米颗粒组成(J-Pt@SnO/C)。基于同步加速器精细结构分析和电化学研究,揭示了Janus结构界面处的晶体重构和电荷重新分布。紧密耦合的界面可以优化铂的价态以及含氧中间体的吸附/解吸。结果,J-Pt@SnO/C催化剂在加速耐久性测试期间具有显著的长期稳定性,在40000次循环后没有明显降解,并且在70000次循环后保留了大部分活性。同时,该催化剂表现出出色的活性,半波电位为0.905 V,质量活性为0.355 A mg(比Pt/C高2.7倍)。Janus催化剂的方法为未来设计高效稳定的基于铂的ORR催化剂铺平了道路。