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Boosting hydrazine oxidation and hydrogen evolution catalysis with anchored Ru clusters by electronically tunable Ru–S–C bonds
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-06-02 , DOI: 10.1039/d3ta02504g
Huaikun Zhang 1 , Wentao Wang 2 , Zechuan Dai 1 , Yin Zhu 1 , Mingyu Cheng 1 , Bocheng Zhang 1 , Yafei Feng 1 , Yangyang Zhang 1 , Genqiang Zhang 1
Affiliation  

Ru clusters have great potential as excellent bifunctional catalysts for the hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR), but suffer from the difficulty of stabilization on the substrate and tuning the electronic environment. Herein, we present Ru clusters supported on N, S co-doped hollow carbon spheres (Ru/NSCS) by elaborately designed Ru–S bonds to anchor Ru clusters and optimize the surrounding coordination environment. The Ru/NSCS exhibits superior electrocatalytic performance for the HER and HzOR, where an ultrasmall overpotential of 40 mV and a working potential of −81 mV at 10 mA cm−2 can be achieved, respectively. The two-electrode system requires an applied voltage of only 26 mV to achieve 10 mA cm−2 and remains stable for 20 hours. Theoretical calculations reveal that the Ru–S bonds induce partial charge transfer from Ru clusters to the N, S co-doped carbon base, thus optimizing the adsorption energy of *H and dehydrogenation intermediates of N2H4.

中文翻译:

通过电子可调的 Ru-S-C 键锚定 Ru 簇促进肼氧化和析氢催化

Ru团簇作为优异的析氢反应(HER)和肼氧化反应(HzOR)双功能催化剂具有巨大的潜力,但其在基底上的稳定性和电子环境的调节方面存在困难。在此,我们提出了通过精心设计的Ru-S键支撑在N、S共掺杂空心碳球(Ru/NSCS)上的Ru簇,以锚定Ru簇并优化周围的配位环境。Ru/NSCS对HER和HzOR表现出优异的电催化性能,在10 mA cm -2下分别可以实现40 mV的超小过电位和-81 mV的工作电位。双电极系统仅需26 mV的外加电压即可实现10 mA cm -2并保持稳定20小时。理论计算表明,Ru-S键诱导部分电荷从Ru团簇转移到N、S共掺杂碳基,从而优化*H和N 2 H 4 脱氢中间体吸附
更新日期:2023-06-02
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