TY - JOUR
T1 - Enhanced Nitrous Oxide Decomposition on Zirconium-Supported Rhodium Catalysts by Iridium Augmentation
AU - Zhang, Ningqiang
AU - He, Chenxi
AU - Jing, Yuan
AU - Qian, Yucheng
AU - Obuchi, Minami
AU - Toyoshima, Ryo
AU - Kondoh, Hiroshi
AU - Oka, Kohei
AU - Wu, Bo
AU - Li, Lingcong
AU - Anzai, Akihiko
AU - Toyao, Takashi
AU - Shimizu, Ken Ichi
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025/1/28
Y1 - 2025/1/28
N2 - The effective elimination of N2O from automobile exhaust at low temperatures poses significant challenges. Compared to other materials, supported RhOx catalysts exhibit high N2O decomposition activities, even in the presence of O2, CO2, and H2O. Metal additives can enhance the low-temperature N2O decomposition activities over supported RhOx catalysts; however, the enhancement mechanism and active sites require further investigation. In this study, we demonstrate the significant enhancement of the low-temperature N2O decomposition activity of a monoclinic ZrO2-supported Rh catalyst [Rh(1)/ZrO2] with Ir addition in the presence of N2O + O2 + CO2 + H2O. The promotional effect of Ir and the active sites on N2O decomposition in Rh(1)-Ir(1)/ZrO2 (Rh = 1 wt % and Ir = 1 wt %) were investigated by kinetic studies and in situ spectroscopic methods, including X-ray absorption spectroscopy, ambient-pressure X-ray photoelectron spectroscopy, and ultraviolet-visible spectroscopy. These results indicate that both surface Rh and Ir species in Rh(1)-Ir(1)/ZrO2 were active sites for N2O catalytic decomposition at low temperatures, and Ir augmentation promoted the desorption of gaseous O2, which are regarded as key steps in N2O decomposition.
AB - The effective elimination of N2O from automobile exhaust at low temperatures poses significant challenges. Compared to other materials, supported RhOx catalysts exhibit high N2O decomposition activities, even in the presence of O2, CO2, and H2O. Metal additives can enhance the low-temperature N2O decomposition activities over supported RhOx catalysts; however, the enhancement mechanism and active sites require further investigation. In this study, we demonstrate the significant enhancement of the low-temperature N2O decomposition activity of a monoclinic ZrO2-supported Rh catalyst [Rh(1)/ZrO2] with Ir addition in the presence of N2O + O2 + CO2 + H2O. The promotional effect of Ir and the active sites on N2O decomposition in Rh(1)-Ir(1)/ZrO2 (Rh = 1 wt % and Ir = 1 wt %) were investigated by kinetic studies and in situ spectroscopic methods, including X-ray absorption spectroscopy, ambient-pressure X-ray photoelectron spectroscopy, and ultraviolet-visible spectroscopy. These results indicate that both surface Rh and Ir species in Rh(1)-Ir(1)/ZrO2 were active sites for N2O catalytic decomposition at low temperatures, and Ir augmentation promoted the desorption of gaseous O2, which are regarded as key steps in N2O decomposition.
KW - automobile emissions
KW - iridium
KW - metal additives
KW - nitrous oxide decomposition
KW - rhodium
UR - https://www.scopus.com/pages/publications/85216692423
UR - https://www.scopus.com/inward/citedby.url?scp=85216692423&partnerID=8YFLogxK
U2 - 10.1021/acs.est.4c08083
DO - 10.1021/acs.est.4c08083
M3 - Article
C2 - 39813396
AN - SCOPUS:85216692423
SN - 0013-936X
VL - 59
SP - 1598
EP - 1607
JO - Environmental Science and Technology
JF - Environmental Science and Technology
IS - 3
ER -