TY - JOUR
T1 - Ozone decomposition on transition-metal-atom anchored graphdiyne
T2 - Insights from computation and experiment
AU - Zhang, Ying
AU - Zhu, Rui
AU - Zhong, Jiang
AU - Quan, Zhipeng
AU - Zhu, Yongjian
AU - Yang, Jingling
AU - Liang, Ping
AU - Yong Lee, Jin
AU - Liu, Hongguang
N1 - Publisher Copyright:
© 2024 Elsevier Inc.
PY - 2024/8/1
Y1 - 2024/8/1
N2 - Transition-metal-atom anchored graphdiynes (TM@GDY, TM = Mn, Fe, Co, Ni and Cu) have already been synthesized and found applications in hydrogen evolution, nitrogen fixation and etc. By means of first-principle predictions and test experiments, we propose here that Fe@GDY and Co@GDY are efficient catalysts for the sustainable conversion of O3 to O2. These two catalysts can spontaneously chemisorb O3 with zero reaction barrier and have low O3 conversion barriers (0.31 eV and 0.19 eV, respectively). The O3 decomposition experiment in a continuous flow membrane reactor and electron paramagnetic resonance results verify that Fe@GDY and Co@GDY are efficient catalysts under humid conditions. Raman spectra prove the formation of the key Fe-O/Co-O and Fe[sbnd]O[sbnd]O and Co[sbnd]O[sbnd]O intermediates. The hydrophobic nature of graphdiyne and the strongest chemisorption of O3 among tested ambient gases, make Fe@GDY and Co@GDY ideal catalysts under both dry and humid conditions. These findings would stimulate future explorations on metal anchored GDY-based catalysts for applications of toxic gas decomposition or fixation.
AB - Transition-metal-atom anchored graphdiynes (TM@GDY, TM = Mn, Fe, Co, Ni and Cu) have already been synthesized and found applications in hydrogen evolution, nitrogen fixation and etc. By means of first-principle predictions and test experiments, we propose here that Fe@GDY and Co@GDY are efficient catalysts for the sustainable conversion of O3 to O2. These two catalysts can spontaneously chemisorb O3 with zero reaction barrier and have low O3 conversion barriers (0.31 eV and 0.19 eV, respectively). The O3 decomposition experiment in a continuous flow membrane reactor and electron paramagnetic resonance results verify that Fe@GDY and Co@GDY are efficient catalysts under humid conditions. Raman spectra prove the formation of the key Fe-O/Co-O and Fe[sbnd]O[sbnd]O and Co[sbnd]O[sbnd]O intermediates. The hydrophobic nature of graphdiyne and the strongest chemisorption of O3 among tested ambient gases, make Fe@GDY and Co@GDY ideal catalysts under both dry and humid conditions. These findings would stimulate future explorations on metal anchored GDY-based catalysts for applications of toxic gas decomposition or fixation.
KW - Density functional theory
KW - Metal anchored graphdiyne
KW - Ozone decomposition
KW - Surface reaction
UR - https://www.scopus.com/pages/publications/85191155990
U2 - 10.1016/j.jcis.2024.04.112
DO - 10.1016/j.jcis.2024.04.112
M3 - Article
C2 - 38669998
AN - SCOPUS:85191155990
SN - 0021-9797
VL - 668
SP - 77
EP - 87
JO - Journal of Colloid and Interface Science
JF - Journal of Colloid and Interface Science
ER -
