TY - JOUR
T1 - Biomimetic Design of a Dynamic M-O-V Pyramid Electron Bridge for Enhanced Nitrogen Electroreduction
AU - Sun, Yuntong
AU - Li, Xuheng
AU - Wang, Zhiqi
AU - Jiang, Lili
AU - Mei, Bingbao
AU - Fan, Wenjun
AU - Wang, Junjie
AU - Zhu, Junwu
AU - Lee, Jong Min
N1 - Publisher Copyright:
© 2024 American Chemical Society
PY - 2024/3/20
Y1 - 2024/3/20
N2 - Electrochemical nitrogen reduction reaction (eNRR) offers a sustainable route for ammonia synthesis; however, current electrocatalysts are limited in achieving optimal performance within narrow potential windows. Herein, inspired by the heliotropism of sunflowers, we present a biomimetic design of Ru-VOH electrocatalyst, featuring a dynamic Ru-O-V pyramid electron bridge for eNRR within a wide potential range. In situ spectroscopy and theoretical investigations unravel the fact that the electrons are donated from Ru to V at lower overpotentials and retrieved at higher overpotentials, maintaining a delicate balance between N2 activation and proton hydrogenation. Moreover, N2 adsorption and activation were found to be enhanced by the Ru-O-V moiety. The catalyst showcases an outstanding Faradaic efficiency of 51.48% at −0.2 V (vs RHE) with an NH3 yield rate exceeding 115 μg h-1 mg-1 across the range of −0.2 to −0.4 V (vs RHE), along with impressive durability of over 100 cycles. This dynamic M-O-V pyramid electron bridge is also applicable to other metals (M = Pt, Rh, and Pd).
AB - Electrochemical nitrogen reduction reaction (eNRR) offers a sustainable route for ammonia synthesis; however, current electrocatalysts are limited in achieving optimal performance within narrow potential windows. Herein, inspired by the heliotropism of sunflowers, we present a biomimetic design of Ru-VOH electrocatalyst, featuring a dynamic Ru-O-V pyramid electron bridge for eNRR within a wide potential range. In situ spectroscopy and theoretical investigations unravel the fact that the electrons are donated from Ru to V at lower overpotentials and retrieved at higher overpotentials, maintaining a delicate balance between N2 activation and proton hydrogenation. Moreover, N2 adsorption and activation were found to be enhanced by the Ru-O-V moiety. The catalyst showcases an outstanding Faradaic efficiency of 51.48% at −0.2 V (vs RHE) with an NH3 yield rate exceeding 115 μg h-1 mg-1 across the range of −0.2 to −0.4 V (vs RHE), along with impressive durability of over 100 cycles. This dynamic M-O-V pyramid electron bridge is also applicable to other metals (M = Pt, Rh, and Pd).
UR - https://www.scopus.com/pages/publications/85187142841
U2 - 10.1021/jacs.3c14816
DO - 10.1021/jacs.3c14816
M3 - 文章
C2 - 38447176
AN - SCOPUS:85187142841
SN - 0002-7863
VL - 146
SP - 7752
EP - 7762
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 11
ER -