TY - JOUR
T1 - Adjacent Fe Site boosts electrocatalytic oxygen evolution at Co site in single-atom-catalyst through a dual-metal-site design
AU - Chen, Changli
AU - Sun, Mingzi
AU - Zhang, Fang
AU - Li, Haijing
AU - Sun, Mengru
AU - Fang, Pin
AU - Song, Tinglu
AU - Chen, Wenxing
AU - Dong, Juncai
AU - Rosen, Brian
AU - Chen, Pengwan
AU - Huang, Bolong
AU - Li, Yujing
N1 - Publisher Copyright:
© 2023 The Royal Society of Chemistry
PY - 2023/2/24
Y1 - 2023/2/24
N2 - Co-based single-atom-catalysts have emerged as possible candidates for the oxygen evolution reaction (OER); however, further improvements in the performance of Co metal sites are challenging with limited optimization space. In this study, a Co-Fe dual-atomic catalyst with optimized intrinsic OER performance was designed, where the individual roles of the single metal sites were investigated in detail. The optimized dual-atomic catalyst exhibited OER activity with an overpotential of 240 mV and turnover frequency (TOF) of 146 s−1 (10 mA cm−2). The systematic microscopy and impedance investigations revealed that the interplay between the Co and Fe metal sites is the key factor for the improved OER performances, wherein the Co sites act as the active sites, with the adjacent Fe serving as the co-catalytic site. Density functional theory (DFT) calculations corroborated the strong orbital coupling between Fe and Co, leading to a d-band structure with improved electroactivity. The Co site coordinated with S and N, enabling efficient site-to-site electron transfer, while the Fe site coordinated with N, which facilitated the chemical stability of the Co site to guarantee efficient OER activity. This work supplied an in-depth understanding of the electrocatalytic performances of dual-atomic catalysts, which is further beneficial for the design of novel atomic catalysts with superior electroactivity towards the OER.
AB - Co-based single-atom-catalysts have emerged as possible candidates for the oxygen evolution reaction (OER); however, further improvements in the performance of Co metal sites are challenging with limited optimization space. In this study, a Co-Fe dual-atomic catalyst with optimized intrinsic OER performance was designed, where the individual roles of the single metal sites were investigated in detail. The optimized dual-atomic catalyst exhibited OER activity with an overpotential of 240 mV and turnover frequency (TOF) of 146 s−1 (10 mA cm−2). The systematic microscopy and impedance investigations revealed that the interplay between the Co and Fe metal sites is the key factor for the improved OER performances, wherein the Co sites act as the active sites, with the adjacent Fe serving as the co-catalytic site. Density functional theory (DFT) calculations corroborated the strong orbital coupling between Fe and Co, leading to a d-band structure with improved electroactivity. The Co site coordinated with S and N, enabling efficient site-to-site electron transfer, while the Fe site coordinated with N, which facilitated the chemical stability of the Co site to guarantee efficient OER activity. This work supplied an in-depth understanding of the electrocatalytic performances of dual-atomic catalysts, which is further beneficial for the design of novel atomic catalysts with superior electroactivity towards the OER.
UR - http://www.scopus.com/inward/record.url?scp=85150419973&partnerID=8YFLogxK
U2 - 10.1039/d2ee03930c
DO - 10.1039/d2ee03930c
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AN - SCOPUS:85150419973
SN - 1754-5692
VL - 16
SP - 1685
EP - 1696
JO - Energy and Environmental Science
JF - Energy and Environmental Science
IS - 4
ER -