TY - JOUR
T1 - Robust tuning metal/carbon heterointerfaces via ketonic oxygen enables hydrogen evolution reaction outperforming Pt/C
AU - Yu, Jiaying
AU - Yang, Yunshuo
AU - Jia, Runtao
AU - Daasbjerg, Kim
AU - Wang, Jun
AU - Carraro, Mauro
AU - Xin, Zhuo
AU - Huang, Yuxing
AU - Skrydstrup, Troels
PY - 2020/11
Y1 - 2020/11
N2 - 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[dbnd]O groups of carbon nanotubes (CNTs) (9.6 g in one batch). From both experimental results and theoretical calculations, we demonstrate that C[dbnd]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[dbnd]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[dbnd]O groups for engineering metal/carbon heterointerfaces towards robust and efficient electrocatalysis.
AB - 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[dbnd]O groups of carbon nanotubes (CNTs) (9.6 g in one batch). From both experimental results and theoretical calculations, we demonstrate that C[dbnd]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[dbnd]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[dbnd]O groups for engineering metal/carbon heterointerfaces towards robust and efficient electrocatalysis.
KW - Electronic structures
KW - Hydrogen evolution reaction
KW - Large-scale synthesis
KW - Metal/carbon heterointerfaces
KW - Oxygen dopants
UR - http://www.scopus.com/inward/record.url?scp=85087275070&partnerID=8YFLogxK
U2 - 10.1016/j.apsusc.2020.147080
DO - 10.1016/j.apsusc.2020.147080
M3 - Journal article
AN - SCOPUS:85087275070
SN - 0169-4332
VL - 529
JO - Applied Surface Science
JF - Applied Surface Science
M1 - 147080
ER -