TY - JOUR
T1 - CO2 hydrogenation to methanol over bimetallic Pd-Cu catalysts supported on TiO2-CeO2 and TiO2-ZrO2
AU - Lin, Fawei
AU - Jiang, Xiao
AU - Boreriboon, Nuttakorn
AU - Song, Chunshan
AU - Wang, Zhihua
AU - Cen, Kefa
N1 - Funding Information:
This work was supported by in part by the Pennsylvania State University through the EMS Energy Institute and Penn State Institute of Energy and the Environment . The overseas expense of FWL in the US was supported by the College of Energy Engineering and Institute for Thermal Power Engineering, Zhejiang University . The author also appreciates for work support from Tianjin University .
Funding Information:
This work was supported by in part by the Pennsylvania State University through the EMS Energy Institute and Penn State Institute of Energy and the Environment. The overseas expense of FWL in the US was supported by the College of Energy Engineering and Institute for Thermal Power Engineering, Zhejiang University. The author also appreciates for work support from Tianjin University.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2021/7/1
Y1 - 2021/7/1
N2 - Binary supports TiO2-CeO2 and TiO2-ZrO2 improved CH3OH formation and selectivity effectively, but with little effect on CO2 conversion. Pd-Cu/Ti0.8Ce0.2O2 enhanced CH3OH formation by ca. 46 % comparing to Pd-Cu/TiO2-C. Pd-Cu/Ti0.1Zr0.9O2 exhibited the highest catalytic performance: CH3OH formation rate was 0.62 μmol g-cat−1s−1, which was enhanced by 121 %, 51 %, and 51 % in comparison to Pd-Cu/TiO2-C, Pd-Cu/ZrO2-C, and Pd-Cu/Ti0.8Ce0.2O2, respectively. More interestingly, lowering temperature from 523 K to 493 K further enhanced CH3OH selectivity from 44.6%–58.8%. Binary supports significantly increased surface area. Unexpectedly, it did not improve H2 reduction for Pd-Cu/TixZr1-xO2 in H2-TPR, but decreased H2 uptake to stoichiometric level, implying SMSI was adjusted to moderate state. However, the excessive H2 uptake further increased for Pd-Cu/TixCe1-xO2, indicating unalleviated SMSI. Furthermore, Pd-Cu alloy formation was improved in Pd-Cu/TixZr1-xO2, which was favorable for CH3OH synthesis. Binary supports also improved CO2 adsorptive behavior towards weakly-bonded species, contributing to better performance.
AB - Binary supports TiO2-CeO2 and TiO2-ZrO2 improved CH3OH formation and selectivity effectively, but with little effect on CO2 conversion. Pd-Cu/Ti0.8Ce0.2O2 enhanced CH3OH formation by ca. 46 % comparing to Pd-Cu/TiO2-C. Pd-Cu/Ti0.1Zr0.9O2 exhibited the highest catalytic performance: CH3OH formation rate was 0.62 μmol g-cat−1s−1, which was enhanced by 121 %, 51 %, and 51 % in comparison to Pd-Cu/TiO2-C, Pd-Cu/ZrO2-C, and Pd-Cu/Ti0.8Ce0.2O2, respectively. More interestingly, lowering temperature from 523 K to 493 K further enhanced CH3OH selectivity from 44.6%–58.8%. Binary supports significantly increased surface area. Unexpectedly, it did not improve H2 reduction for Pd-Cu/TixZr1-xO2 in H2-TPR, but decreased H2 uptake to stoichiometric level, implying SMSI was adjusted to moderate state. However, the excessive H2 uptake further increased for Pd-Cu/TixCe1-xO2, indicating unalleviated SMSI. Furthermore, Pd-Cu alloy formation was improved in Pd-Cu/TixZr1-xO2, which was favorable for CH3OH synthesis. Binary supports also improved CO2 adsorptive behavior towards weakly-bonded species, contributing to better performance.
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U2 - 10.1016/j.cattod.2020.05.049
DO - 10.1016/j.cattod.2020.05.049
M3 - Article
AN - SCOPUS:85086875095
VL - 371
SP - 150
EP - 161
JO - Catalysis Today
JF - Catalysis Today
SN - 0920-5861
ER -