TY - JOUR
T1 - Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis
AU - Li, Lu
AU - Zhang, Gengwei
AU - Zhou, Chenhui
AU - Lv, Fan
AU - Tan, Yingjun
AU - Han, Ying
AU - Luo, Heng
AU - Wang, Dawei
AU - Liu, Youxing
AU - Shang, Changshuai
AU - Zeng, Lingyou
AU - Huang, Qizheng
AU - Zeng, Ruijin
AU - Ye, Na
AU - Luo, Mingchuan
AU - Guo, Shaojun
N1 - Publisher Copyright:
© The Author(s) 2024.
PY - 2024/12
Y1 - 2024/12
N2 - Precisely modulating the Ru-O covalency in RuOx for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d-valence electrons, which were doped into or alloyed with RuOx, are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5s/5p orbitals. Theoretical calculations confirm that the durability of Ln-RuOx following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuOx, Er-RuOx is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO2. Particularly, the Er-RuOx-based device requires only 1.837 V to reach 3 A cm−2 and shows a long-term stability at 500 mA cm−2 for 100 h with a degradation rate of mere 37 μV h−1.
AB - Precisely modulating the Ru-O covalency in RuOx for enhanced stability in proton exchange membrane water electrolysis is highly desired. However, transition metals with d-valence electrons, which were doped into or alloyed with RuOx, are inherently susceptible to the influence of coordination environment, making it challenging to modulate the Ru-O covalency in a precise and continuous manner. Here, we first deduce that the introduction of lanthanide with gradually changing electronic configurations can continuously modulate the Ru-O covalency owing to the shielding effect of 5s/5p orbitals. Theoretical calculations confirm that the durability of Ln-RuOx following a volcanic trend as a function of Ru-O covalency. Among various Ln-RuOx, Er-RuOx is identified as the optimal catalyst and possesses a stability 35.5 times higher than that of RuO2. Particularly, the Er-RuOx-based device requires only 1.837 V to reach 3 A cm−2 and shows a long-term stability at 500 mA cm−2 for 100 h with a degradation rate of mere 37 μV h−1.
UR - https://www.scopus.com/pages/publications/85195673309
U2 - 10.1038/s41467-024-49281-2
DO - 10.1038/s41467-024-49281-2
M3 - 文章
C2 - 38862507
AN - SCOPUS:85195673309
SN - 2041-1723
VL - 15
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 4974
ER -