TY - JOUR
T1 - Spatial segregation of catalytic sites within Pd doped H-ZSM-5 for fatty acid hydrodeoxygenation to alkanes
AU - Ding, Shengzhe
AU - Ainaga, Dario Luis Fernandez
AU - Hu, Min
AU - Qiu, Boya
AU - Khalid, Ushna
AU - D'Agostino, Carmine
AU - Ou, Xiaoxia
AU - Spencer, Ben
AU - Zhong, Xiangli
AU - Peng, Yani
AU - Hondow, Nicole
AU - Theodoropoulos, Constantinos
AU - Jiao, Yilai
AU - Parlett, Christopher M. A.
AU - Fan, Xiaolei
PY - 2024/9/4
Y1 - 2024/9/4
N2 - Spatial control over features within multifunctional catalysts can unlock efficient one-pot cascade reactions, which are themselves a pathway to aviation biofuels via hydrodeoxygenation. A synthesis strategy that encompasses spatial orthogonality, i.e., one in which different catalytic species are deposited exclusively within discrete locations of a support architecture, is one solution that permits control over potential interactions between different sites and the cascade process. Here, we report a Pd doped hierarchical zeolite, in which Pd nanoparticles are selectively deposited within the mesopores, while acidity is retained solely within the micropores of ZSM-5. This spatial segregation facilitates hydrodeoxygenation while suppressing undesirable decarboxylation and decarbonation, yielding significant enhancements in activity (30.6 vs 3.6 mol
dodecane mol
Pd
−1 h
−1) and selectivity (C
12:C
11 5.2 vs 1.9) relative to a conventionally prepared counterpart (via wet impregnation). Herein, multifunctional material design can realise efficient fatty acid hydrodeoxygenation, thus advancing the field and inspiring future developments in rationalised catalyst design.
AB - Spatial control over features within multifunctional catalysts can unlock efficient one-pot cascade reactions, which are themselves a pathway to aviation biofuels via hydrodeoxygenation. A synthesis strategy that encompasses spatial orthogonality, i.e., one in which different catalytic species are deposited exclusively within discrete locations of a support architecture, is one solution that permits control over potential interactions between different sites and the cascade process. Here, we report a Pd doped hierarchical zeolite, in which Pd nanoparticles are selectively deposited within the mesopores, while acidity is retained solely within the micropores of ZSM-5. This spatial segregation facilitates hydrodeoxygenation while suppressing undesirable decarboxylation and decarbonation, yielding significant enhancements in activity (30.6 vs 3.6 mol
dodecane mol
Pd
−1 h
−1) and selectivity (C
12:C
11 5.2 vs 1.9) relative to a conventionally prepared counterpart (via wet impregnation). Herein, multifunctional material design can realise efficient fatty acid hydrodeoxygenation, thus advancing the field and inspiring future developments in rationalised catalyst design.
UR - https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=pure_starter&SrcAuth=WosAPI&KeyUT=WOS:001335948800010&DestLinkType=FullRecord&DestApp=WOS_CPL
UR - http://www.scopus.com/inward/record.url?scp=85203128594&partnerID=8YFLogxK
U2 - 10.1038/s41467-024-51925-2
DO - 10.1038/s41467-024-51925-2
M3 - Article
C2 - 39231994
SN - 2041-1723
VL - 15
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 7718
ER -