Lin Xin, Geng Shize, Du Xianglong, Wang Feiteng, Zhang Xu, Xiao Fang, Xiao Zhengyi, Wang Yucheng, Cheng Jun, Zheng Zhifeng, Huang Xiaoqing, Bu Lingzheng
College of Energy, Xiamen University, Xiamen, China.
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
Nat Commun. 2025 Jan 2;16(1):147. doi: 10.1038/s41467-024-55612-0.
The lack of high-efficiency platinum (Pt)-based nanomaterials remains a formidable and exigent challenge in achieving high formic acid oxidation reaction (FAOR) and membrane electrode assembly (MEA) catalysis for direct formic acid fuel cell (DFAFC) technology. Herein, we report 16 Pt-based heterophase nanotrepang with rare earth (RE)-doped face-centered cubic Pt (fcc-Pt) and trigonal Pt-tellurium (t-PtTe) configurations ((RE-Pt)-PtTe HPNT). Yttrium (Y) is identified as the optimal dopant, existing as single sites and clusters on the surface. The (Y-Pt)-PtTe HPNT/C demonstrates the superior mass and specific activities of 6.4 A mg and 5.4 mA cm, outperforming commercial Pt/C by factors of 49.2 and 25.7, respectively. Additionally, it achieves a normalized MEA power density of 485.9 W g, tripling that of Pt/C. Density functional theory calculations further reveal that Y doping enhances HCOO* intermediate adsorption and suppresses CO intermediate formation, thereby promoting FAOR kinetics. This work highlights the role of RE metals in heterostructure regulation of Pt-based anodic nanomaterials for achieving the efficient direct formic acid electrocatalysis.
在直接甲酸燃料电池（DFAFC）技术中，实现高效的甲酸氧化反应（FAOR）和膜电极组件（MEA）催化，缺乏高效的铂（Pt）基纳米材料仍然是一个严峻且迫切的挑战。在此，我们报道了一种具有稀土（RE）掺杂面心立方Pt（fcc-Pt）和三角Pt-碲（t-PtTe）构型的16种Pt基异相海参状纳米材料（（RE-Pt）-PtTe HPNT）。钇（Y）被确定为最佳掺杂剂，以单原子和团簇形式存在于表面。（Y-Pt）-PtTe HPNT/C展现出6.4 A mg和5.4 mA cm的优异质量活性和比活性，分别比商业Pt/C高出49.2倍和25.7倍。此外，它实现了485.9 W g的归一化MEA功率密度，是Pt/C的三倍。密度泛函理论计算进一步表明，Y掺杂增强了HCOO*中间体的吸附并抑制了CO中间体的形成，从而促进了FAOR动力学。这项工作突出了稀土金属在基于Pt的阳极纳米材料异质结构调控中对实现高效直接甲酸电催化的作用。
