Gao Ziru, Shen Yongqing, Hao Bing, Song Yanhui, Liu Peizhi, Guo Junjie
Key Laboratory of Interface Science and Engineering in Advanced Materials, Ministry of Education, College of Materials Science and Engineering, Taiyuan University of Technology, Shanxi, 030024, P. R. China.
Instrumental Analysis Center, Taiyuan University of Technology, Taiyuan, 030024, P. R. China.
Small. 2025 Jul;21(29):e2503233. doi: 10.1002/smll.202503233. Epub 2025 May 27.
Although ultrathin noble-metal nanosheets have arisen as promising high-efficient electrocatalysts, their catalytic behaviors are still far to be satisfied due to lacking of additional active sites on the basal plane of 2D structure. Herein, partially amorphization strategy is adopted to construct localized amorphous area in ultrathin RuO nanosheets by doping Mn. This strategy endows the MnRuO catalyst enriched basal plane active sites, channels for mass transfer, amorphous/crystalline interfaces, and thus a superior HER activity. Impressively, the optimal MnRuO NSs-250, which is achieved by annealing at 250 °C, shows excellent HER performance within alkaline condition with a low overpotential of only 31 mV at 10 mA cm and a small Tafel slope of 46.7 mV dec which is superior to that of commercial Pt/C catalysts. The key role of localized amorphization on the enhanced HER properties of MnRuO NSs-250 is determined by in situ Raman spectroscopy and theoretical calculations. It is found that Mn doping can promote the adsorption/desorption of HO, thus inducing the electron redistribution at the amorphous/crystalline interfaces and accelerating the Volmer step in alkaline HER. This work provides a valuable guidance for improving the performance and stability of other electrocatalysts for alkaline HER applications.
尽管超薄贵金属纳米片已成为有前景的高效电催化剂,但由于二维结构基面缺乏额外的活性位点,其催化性能仍远不能令人满意。在此,采用部分非晶化策略,通过掺杂锰在超薄RuO纳米片中构建局部非晶区域。该策略赋予MnRuO催化剂丰富的基面活性位点、传质通道、非晶/晶体界面,从而具有优异的析氢活性。令人印象深刻的是,通过在250℃退火获得的最佳MnRuO NSs-250在碱性条件下表现出优异的析氢性能,在10 mA cm时过电位仅为31 mV,塔菲尔斜率为46.7 mV dec,优于商业Pt/C催化剂。通过原位拉曼光谱和理论计算确定了局部非晶化对MnRuO NSs-250增强析氢性能的关键作用。研究发现,锰掺杂可以促进HO的吸附/解吸,从而在非晶/晶体界面诱导电子重新分布,并加速碱性析氢中的Volmer步骤。这项工作为提高其他用于碱性析氢应用的电催化剂的性能和稳定性提供了有价值的指导。