Huang Shaoda, Lu Shuanglong, Gong Shun, Zhang Qiuju, Duan Fang, Zhu Han, Gu Hongwei, Dong Weifu, Du Mingliang
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, Jiangsu 214122, P. R. China.
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, Zhejiang 315201, P. R. China.
ACS Nano. 2022 Jan 25;16(1):522-532. doi: 10.1021/acsnano.1c07574. Epub 2021 Dec 23.
Engineering the morphology and electronic properties simultaneously of emerging metallene materials is an effective strategy for enhancing their performance as oxygen reduction reaction (ORR) electrocatalysts. Herein, a highly efficient and stable ORR electrocatalyst, Fe-doped ultrathin porous Pd metallene (Fe-Pd UPM) composed of a few layers of 2D atomic metallene layers, was synthesized using a simple one pot wet-chemical method and characterized. Fe-Pd UPM was measured to have enhanced ORR activity compared to undoped Pd metallene. Fe-Pd UPM exhibits a mass activity of 0.736 A mg with a loss of mass activity of only 5.1% after 10 000 cycles at 0.9 V versus the reversible hydrogen electrode (vs RHE) in 0.1 M KOH solution. Density functional theory (DFT) calculations reveal that the stable Fe dopant in the inner atomic layers of Fe-Pd UPM delivers a much smaller overpotential during O* hydrogenation into OH*. The morphology, porous structure, and Fe doping were verified to have enhanced ORR activity. We believe that the rational design of metallene materials with porous structures and interlayer doping is promising for the development of efficient and stable electrocatalysts.
同时调控新兴金属烯材料的形貌和电子性质是提高其作为氧还原反应（ORR）电催化剂性能的有效策略。在此，我们采用简单的一锅湿化学法合成并表征了一种由几层二维原子金属烯层组成的高效稳定的ORR电催化剂——铁掺杂超薄多孔钯金属烯（Fe-Pd UPM）。与未掺杂的钯金属烯相比，Fe-Pd UPM的ORR活性有所增强。在0.1 M KOH溶液中，相对于可逆氢电极（vs RHE），在0.9 V下循环10000次后，Fe-Pd UPM的质量活性为0.736 A mg，质量活性损失仅为5.1%。密度泛函理论（DFT）计算表明，Fe-Pd UPM内原子层中稳定的铁掺杂剂在O氢化生成OH的过程中提供了小得多的过电位。形貌、多孔结构和铁掺杂被证实增强了ORR活性。我们认为，合理设计具有多孔结构和层间掺杂的金属烯材料对于开发高效稳定的电催化剂具有广阔前景。
