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Robust tuning metal/carbon heterointerfaces via ketonic oxygen enables hydrogen evolution reaction outperforming Pt/C
Applied Surface Science ( IF 6.3 ) Pub Date : 2020-11-01 , DOI: 10.1016/j.apsusc.2020.147080
Jiaying Yu , Yunshuo Yang , Runtao Jia , Kim Daasbjerg , Jun Wang , Mauro Carraro , Zhuo Xin , Yuxing Huang , Troels Skrydstrup

Abstract Large-scale synthesis of metal/carbon hybrids with tunable metal/carbon heterointerfaces is vital for practical application of such hybrids in electrocatalysis. Herein, we developed a facile route for large-scale crafting of ultrafine Ru nanoparticles (NPs) anchored on the ketonic C O groups of carbon nanotubes (CNTs) (9.6 g in one batch). From both experimental results and theoretical calculations, we demonstrate that C O (rather than C–O) groups can be exploited to engineer the heterointerface of CNTs and Ru NPs. In fact, the electronic structure of Ru becomes considerably improved because the high polarity of C O facilitates the interface electron transfer of Ru/CNTs. Consequently, the obtained Ru-O-CNTs hybrids with low Ru loading of 1.5 wt% display a small overpotential of 25 mV at 10 mA cm−2 and with fast kinetics as deduced from a small Tafel slope of 20.4 mV dec−1 for hydrogen evolution reaction (HER) in 1 M KOH. Impressively, at 70 mV overpotential, the hybrids exhibit a record mass activity of 20.4 mA μg−1Ru, which is more than 50-fold of that for commercial Pt/C. Therefore, for the first time, we identified the vital role of C O groups for engineering metal/carbon heterointerfaces towards robust and efficient electrocatalysis.

中文翻译:

通过酮氧稳定调节金属/碳异质界面使析氢反应优于 Pt/C

摘要 大规模合成具有可调金属/碳异质界面的金属/碳杂化物对于这种杂化物在电催化中的实际应用至关重要。在此,我们开发了一种用于大规模制作超细 Ru 纳米粒子 (NPs) 的简便途径,该纳米粒子锚定在碳纳米管 (CNT) 的酮基 CO 基团上(一批 9.6 g)。从实验结果和理论计算来看,我们证明可以利用 CO(而不是 C-O)基团来设计 CNT 和 Ru NPs 的异质界面。事实上,Ru 的电子结构得到了显着改善,因为 CO 的高极性促进了 Ru/CNT 的界面电子转移。因此,所获得的 Ru-O-CNTs 杂化物具有 1 的低 Ru 负载量。5 wt% 在 10 mA cm-2 下显示出 25 mV 的小过电位,并且从 1 M KOH 中析氢反应 (HER) 的 20.4 mV dec-1 小塔菲尔斜率推断出具有快速动力学。令人印象深刻的是,在 70 mV 过电位下,混合体表现出创纪录的 20.4 mA μg-1Ru 质量活性,是商业 Pt/C 的 50 倍以上。因此,我们首次确定了 CO 基团在设计金属/碳异质界面以实现稳健高效的电催化方面的重要作用。
更新日期:2020-11-01
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