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锚定在分级多孔氮掺杂碳球上的RuN簇用于高效碱性析氢反应。

RuN clusters anchored on hierarchically porous N-doped carbon spheres for efficient alkaline hydrogen evolution reaction.

作者信息

Niu Yingying, Tian Zhengbin, Wang Wenquan, Deng Xiaohui, Zhang Botao, Wang Guang-Hui

机构信息

College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, China.

Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.

出版信息

Nanoscale. 2025 Jun 19;17(24):14750-14758. doi: 10.1039/d5nr00721f.

DOI:10.1039/d5nr00721f
PMID:40437983
Abstract

Carbon-supported Ru clusters have been recognized as promising electrocatalysts for alkaline hydrogen evolution reaction (HER), but their catalytic activity is still limited by the weak metal-carbon interaction or the blockage of active sites. Herein, we report a facile method by which RuN clusters are anchored on hierarchically porous N-doped carbon spheres (Ru/NCS) pyrolysis of the polymer precursor of NCS containing Ru ions. Experimental results indicate that the interaction between Ru species and N-doped carbon leads to the formation of ultrafine RuN clusters with uniform distribution on NCS and also optimizes the Ru-H/Ru-OH bond strength, thereby promoting the rate-determining Volmer step in alkaline HER. Furthermore, the open porous structure of the NCS support is beneficial for the transport of gaseous products. Consequently, the as-synthesized Ru/NCS exhibits excellent HER performance with an overpotential of 4 mV, a low Tafel slope of 26 mV dec, a high mass activity of 6.24 A mg Ru at an overpotential of 50 mV, and long-term stability over 1000 h at 10 mA cm with negligible voltage increase, outperforming state-of-the-art commercial Pt/C and Ru/C benchmarks.

摘要

碳负载的钌簇已被认为是用于碱性析氢反应(HER)的有前景的电催化剂,但其催化活性仍受弱金属 - 碳相互作用或活性位点阻塞的限制。在此,我们报道了一种简便的方法,通过该方法,RuN簇锚定在分级多孔的氮掺杂碳球(Ru/NCS)上,该方法是对含Ru离子的NCS聚合物前驱体进行热解。实验结果表明,Ru物种与氮掺杂碳之间的相互作用导致在NCS上形成分布均匀的超细RuN簇,并且还优化了Ru - H/Ru - OH键强度,从而促进了碱性HER中速率决定的Volmer步骤。此外,NCS载体的开放多孔结构有利于气态产物的传输。因此,合成的Ru/NCS表现出优异的HER性能,过电位为4 mV,低塔菲尔斜率为26 mV dec,在50 mV过电位下高质量活性为6.24 A mg Ru,并且在10 mA cm下超过1000 h的长期稳定性,电压增加可忽略不计,优于目前最先进的商业Pt/C和Ru/C基准。

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