Lin Tian, Xiaoping Gao, Mengzhao Zhu, Zixiang Huang, Bei Wu, Cai Chen, Xianhui Ma, Yaner Ruan, Wenxin Guo, Xiangmin Meng, Huijuan Wang, Wubin Du, Shengnan He, Hongge Pan, Xusheng Zheng, Zhijun Wu, Huang Zhou, Jing Xia, Yuen Wu
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引用次数: 0
摘要
在质子交换膜燃料电池(PEMFC)的长期运行过程中,如何保持低铂催化剂的稳定性仍然是一个巨大的挑战。本文介绍了一种双重封闭设计,可显著提高金属间纳米粒子的稳定性,同时保持其对 PEMFC 的高催化活性。首先,在纳米粒子表面涂上一层碳壳,形成碳约束。其次,在退火过程中引入氧气,选择性地蚀刻碳壳,使活性表面暴露出来,并诱导表面过渡金属偏析,形成铂-铂-铂-铂-铂-铂-铂-铂-铂-铂-表层封闭。总之,金属间纳米粒子受到碳约束和铂-表层约束的保护,可以承受 PEMFCs 的恶劣环境。通常,在 PEMFCs 测试中,双封闭 Pt1Co1 催化剂在 0.9 V 时的质量活性为 1.45 A mgPt-1,循环 30,000 次后仅衰减 17.3%,且未观察到结构变化,优于大多数已报道的 PtCo 催化剂和 DOE 2025 目标。此外,还可以通过改变涂层碳壳的厚度来控制碳约束比例,这种策略也适用于合成双约束 Pt1Fe1 和 Pt1Cu1 金属间纳米粒子。
Double Confinement Design to Access Highly Stable Intermetallic Nanoparticles for Fuel Cells
Maintaining the stability of low Pt catalysts during prolonged operation of proton exchange membrane fuel cells (PEMFCs) remains a substantial challenge. Here, a double confinement design is presented to significantly improve the stability of intermetallic nanoparticles while maintaining their high catalytic activity toward PEMFCs. First, a carbon shell is coated on the surface of nanoparticles to form carbon confinement. Second, O2 is introduced during the annealing process to selectively etch the carbon shell to expose the active surface, and to induce the segregation of surface transition metals to form Pt-skin confinement. Overall, the intermetallic nanoparticles are protected by carbon confinement and Pt-skin confinement to withstand the harsh environment of PEMFCs. Typically, the double confined Pt1Co1 catalyst exhibits an exceptional mass activity of 1.45 A mgPt−1 at 0.9 V in PEMFCs tests, with only a 17.3% decay after 30 000 cycles and no observed structure changes, outperforming most reported PtCo catalysts and DOE 2025 targets. Furthermore, the carbon confinement proportion can be controlled by varying the thickness of the coated carbon shell, and this strategy is also applicable to the synthesis of double-confined Pt1Fe1 and Pt1Cu1 intermetallic nanoparticles.
期刊介绍:
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