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Spatial segregation of catalytic sites within Pd doped H-ZSM-5 for fatty acid hydrodeoxygenation to alkanes
被引:13
作者:
Ding, Shengzhe
[1
,2
]
Ainaga, Dario Luis Fernandez
[3
]
Hu, Min
[1
]
Qiu, Boya
[1
]
Khalid, Ushna
[1
]
D'Agostino, Carmine
[1
,4
]
Ou, Xiaoxia
[1
,5
]
Spencer, Ben
[6
,7
]
Zhong, Xiangli
[6
,7
]
Peng, Yani
[1
]
Hondow, Nicole
[3
]
Theodoropoulos, Constantinos
[1
]
Jiao, Yilai
[8
]
Parlett, Christopher M. A.
[1
,9
,10
,11
]
Fan, Xiaolei
[1
,5
,12
]
机构:
[1] Univ Manchester, Dept Chem Engn, Manchester M13 9PL, England
[2] Sinopec, Inst Catalysis Sci, Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China
[3] Univ Leeds, Sch Chem & Proc Engn, Leeds LS2 9JT, England
[4] Univ Bologna, Dipartimento Ingn Civile, Chim, I-40131 Bologna, Italy
[5] Nottingham Ningbo China Beacons Excellence Res & I, Ningbo 315100, Peoples R China
[6] Univ Manchester, Henry Royce Inst, Manchester M13 9PL, England
[7] Univ Manchester, Dept Mat, Manchester M13 9PL, England
[8] Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
[9] Diamond Light Source, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England
[10] Univ Manchester Harwell, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England
[11] Rutherford Appleton Lab, UK Catalysis Hub, Harwell OX11 0FA, Oxon, England
[12] Zhejiang Univ, Inst Wenzhou, Wenzhou 325006, Peoples R China
基金:
英国工程与自然科学研究理事会;
中国国家自然科学基金;
关键词:
BIFUNCTIONAL CATALYSTS;
SELECTIVE CONVERSION;
GAMMA-VALEROLACTONE;
PALMITIC ACID;
SUCCINIC ACID;
HYDROGENATION;
PALLADIUM;
ZEOLITES;
ALCOHOL;
NANOPARTICLES;
D O I:
10.1038/s41467-024-51925-2
中图分类号:
O [数理科学和化学];
P [天文学、地球科学];
Q [生物科学];
N [自然科学总论];
学科分类号:
07 ;
0710 ;
09 ;
摘要:
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 moldodecane molPd-1 h-1) and selectivity (C12:C11 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. Hierarchical ZSM-5 boosts fatty acid hydrodeoxygenation by compartmentalization of catalytic sites. Separating acid sites within micropores and metal nanoparticles in mesopores provides control over the reaction and reduces unwanted side reactions.
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页数:12
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