TY - JOUR
T1 - Micropore-confined Ru nanoclusters catalyst for efficient pH-universal hydrogen evolution reaction
AU - Huang, Xiaoxiao
AU - Lu, Ruihu
AU - Cen, Yaping
AU - Wang, Dunchao
AU - Jin, Shao
AU - Chen, Wenxing
AU - Geoffrey, I.
AU - Waterhouse, N.
AU - Wang, Ziyun
AU - Tian, Shubo
AU - Sun, Xiaoming
N1 - Publisher Copyright:
© 2023, Tsinghua University Press.
PY - 2023/7
Y1 - 2023/7
N2 - Pt-based catalysts are used commercially for the hydrogen evolution reaction (HER), even though the low earth abundance and high cost of platinum hinder scale-up applications. Ru metal is a promising alternative catalyst for HER owing to its lower cost but similar metal-hydrogen bond strength to Pt. However, designing an efficient and robust Ru-based electrocatalyst for pH-universal HER is challenging. Herein, we successfully synthesized N-doped carbon (NC) supported ruthenium catalysts with different Ru sizes (single-atoms, nanoclusters and nanoparticles), and then systematically evaluated their performance for HER. Among these catalysts, the Ru nanocluster catalyst (Ru NCs/NC) displayed optimal catalytic performance with overpotentials of only 14, 30, and 32 mV (at 10 mA·cm−2) in 1 M KOH, 1 M phosphate buffer saline (PBS), and 0.5 M H2SO4, respectively. The corresponding mass activities were 32.2, 12.1 and 8.1 times higher than those of 20 wt.% Pt/C, and also much better than those of the Ru single-atoms (Ru SAs/NC) and Ru nanoparticle (Ru NPs/NC) catalysts, at an overpotential of 100 mV under alkaline, neutral and acidic conditions, respectively. Density functional theory (DFT) calculations revealed that the outstanding HER performance of the Ru NCs/NC catalyst resulted from a strong interaction between the Ru nanoclusters and the N-doped carbon support, which downshifted the d-band center and thus weakened the ⋆H adsorption ability of Ru sites.[Figure not available: see fulltext.]
AB - Pt-based catalysts are used commercially for the hydrogen evolution reaction (HER), even though the low earth abundance and high cost of platinum hinder scale-up applications. Ru metal is a promising alternative catalyst for HER owing to its lower cost but similar metal-hydrogen bond strength to Pt. However, designing an efficient and robust Ru-based electrocatalyst for pH-universal HER is challenging. Herein, we successfully synthesized N-doped carbon (NC) supported ruthenium catalysts with different Ru sizes (single-atoms, nanoclusters and nanoparticles), and then systematically evaluated their performance for HER. Among these catalysts, the Ru nanocluster catalyst (Ru NCs/NC) displayed optimal catalytic performance with overpotentials of only 14, 30, and 32 mV (at 10 mA·cm−2) in 1 M KOH, 1 M phosphate buffer saline (PBS), and 0.5 M H2SO4, respectively. The corresponding mass activities were 32.2, 12.1 and 8.1 times higher than those of 20 wt.% Pt/C, and also much better than those of the Ru single-atoms (Ru SAs/NC) and Ru nanoparticle (Ru NPs/NC) catalysts, at an overpotential of 100 mV under alkaline, neutral and acidic conditions, respectively. Density functional theory (DFT) calculations revealed that the outstanding HER performance of the Ru NCs/NC catalyst resulted from a strong interaction between the Ru nanoclusters and the N-doped carbon support, which downshifted the d-band center and thus weakened the ⋆H adsorption ability of Ru sites.[Figure not available: see fulltext.]
KW - Ru nanoclusters
KW - Ru nanoparticles
KW - Ru single atoms
KW - hydrogen evolution reaction
UR - http://www.scopus.com/inward/record.url?scp=85160318368&partnerID=8YFLogxK
U2 - 10.1007/s12274-023-5711-1
DO - 10.1007/s12274-023-5711-1
M3 - Article
AN - SCOPUS:85160318368
SN - 1998-0124
VL - 16
SP - 9073
EP - 9080
JO - Nano Research
JF - Nano Research
IS - 7
ER -