Zhang Zeyi, Wu Wei, Chen Suhao, Wang Zichen, Tan Yangyang, Chen Wei, Guo Fei, Chen Runzhe, Cheng Niancai
College of Materials Science and Engineering, Fuzhou University, Fuzhou, 350108, China.
Department of Chemistry, University of Zurich, Winterthurerstrasse 190, Zurich, CH-8057, Switzerland.
Small. 2024 May;20(22):e2307135. doi: 10.1002/smll.202307135. Epub 2023 Dec 21.
Achieving high catalytic activity with a minimum amount of platinum (Pt) is crucial for accelerating the cathodic hydrogen evolution reaction (HER) in proton exchange membrane (PEM) water electrolysis, yet it remains a significant challenge. Herein, a directed dual-charge pumping strategy to tune the d-orbital electronic distribution of Pt nanoclusters for efficient HER catalysis is proposed. Theoretical analysis reveals that the ligand effect and electronic metal-support interactions (EMSI) create an effective directional electron transfer channel for the d-orbital electrons of Pt, which in turn optimizes the binding strength to H*, thereby significantly enhancing HER efficiency of the Pt site. Experimentally, this directed dual-charge pumping strategy is validated by elaborating Sb-doped SnO (ATO) supported Fe-doped PtSn heterostructure catalysts (Fe-PtSn/ATO). The synthesized 3%Fe-PtSn/ATO catalysts exhibit lower overpotential (requiring only 10.5 mV to reach a current density of 10 mA cm ), higher mass activity (28.6 times higher than commercial 20 wt.% Pt/C), and stability in the HER process in acidic media. This innovative strategy presents a promising pathway for the development of highly efficient HER catalysts with low Pt loading.
在质子交换膜（PEM）水电解中，以最少的铂（Pt）实现高催化活性对于加速阴极析氢反应（HER）至关重要，但这仍然是一项重大挑战。在此，提出了一种定向双电荷泵浦策略，用于调节Pt纳米团簇的d轨道电子分布以实现高效HER催化。理论分析表明，配体效应和电子金属-载体相互作用（EMSI）为Pt的d轨道电子创造了一个有效的定向电子转移通道，进而优化了对H*的结合强度，从而显著提高了Pt位点的HER效率。实验上，通过精心制备Sb掺杂的SnO（ATO）负载的Fe掺杂PtSn异质结构催化剂（Fe-PtSn/ATO）验证了这种定向双电荷泵浦策略。合成的3%Fe-PtSn/ATO催化剂表现出更低的过电位（达到10 mA cm的电流密度仅需10.5 mV）、更高的质量活性（比商业20 wt.% Pt/C高28.6倍）以及在酸性介质中HER过程中的稳定性。这种创新策略为开发低Pt负载的高效HER催化剂提供了一条有前景的途径。
