TY - JOUR
T1 - Fabrication of a NiFe Alloy Oxide Catalyst via Surface Reconstruction for Selective Hydrodeoxygenation of Fatty Acid to Fatty Alcohol
AU - Han, Depeng
AU - Yin, Wang
AU - Wang, Shengping
AU - Xia, Shuqian
N1 - Funding Information:
Financial support by the National Basic Research Program of China (973) special preliminary study program (2014CB260408) is gratefully acknowledged.
Publisher Copyright:
©
PY - 2021/11/8
Y1 - 2021/11/8
N2 - Traditional NiFe alloy catalyst (NiFe AC) possesses low alcohol selectivity for the hydrodeoxygenation (HDO) of fatty acid due to its excessive deoxygenation into alkane. Herein, we innovatively provide the NiFe alloy oxide catalyst (NiFe AOC) to suppress the adsorption of aldehyde, which is the crucial intermediate of objective product alcohol converting into a side product, via the steric hindrance of lattice oxygen to inhibit the further conversion of alcohol. NiFe AOC reaches 100% conversion of lauric acid with 90% selectivity to lauryl alcohol. Kinetic analysis indicated that the apparent activation energy of side reaction increases by 71.1 kJ/mol for NiFe AOC relative to NiFe AC, evidencing the inhibition for the conversion of objective product alcohol into alkane for NiFe AOC. Furthermore, DFT calculation also suggests that the activation energy of the side reaction increases by 0.33 eV on NiFe AOC compared to NiFe AC. In addition, used NiFe AOC can be totally regenerated via surface reconstruction during the reduction-reoxidation treatment. However, overoxidation inducing NiFe surface phase separation weakened the synergistic interaction of Ni-Fe bimetallic sites and further decreased the catalytic activity.
AB - Traditional NiFe alloy catalyst (NiFe AC) possesses low alcohol selectivity for the hydrodeoxygenation (HDO) of fatty acid due to its excessive deoxygenation into alkane. Herein, we innovatively provide the NiFe alloy oxide catalyst (NiFe AOC) to suppress the adsorption of aldehyde, which is the crucial intermediate of objective product alcohol converting into a side product, via the steric hindrance of lattice oxygen to inhibit the further conversion of alcohol. NiFe AOC reaches 100% conversion of lauric acid with 90% selectivity to lauryl alcohol. Kinetic analysis indicated that the apparent activation energy of side reaction increases by 71.1 kJ/mol for NiFe AOC relative to NiFe AC, evidencing the inhibition for the conversion of objective product alcohol into alkane for NiFe AOC. Furthermore, DFT calculation also suggests that the activation energy of the side reaction increases by 0.33 eV on NiFe AOC compared to NiFe AC. In addition, used NiFe AOC can be totally regenerated via surface reconstruction during the reduction-reoxidation treatment. However, overoxidation inducing NiFe surface phase separation weakened the synergistic interaction of Ni-Fe bimetallic sites and further decreased the catalytic activity.
KW - hydrodeoxygenation
KW - NiFe alloy oxide catalyst
KW - regenerate
KW - steric hindrance
KW - surface reconstruction
UR - http://www.scopus.com/inward/record.url?scp=85118710761&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.1c05919
DO - 10.1021/acssuschemeng.1c05919
M3 - Article
AN - SCOPUS:85118710761
SN - 2168-0485
VL - 9
SP - 15027
EP - 15041
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
IS - 44
ER -