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.
引用
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页数:12
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共 81 条
[1]   An efficient microwave-assisted chelation (MWAC) post-synthetic modification method to produce hierarchical Y zeolites [J].
Abdulridha, Samer ;
Zhang, Rongxin ;
Xu, Shaojun ;
Tedstone, Aleksander ;
Ou, Xiaoxia ;
Gong, Jiacheng ;
Mao, Boyang ;
Frogley, Mark ;
Bawn, Carlo ;
Zhou, Zhaoxia ;
Zhang, Xinran ;
Chansai, Sarayute ;
Holmes, Stuart M. ;
Hardacre, Christopher ;
Garforth, Arthur A. ;
Yang, Sihai ;
Jiao, Yilai ;
Fan, Xiaolei .
MICROPOROUS AND MESOPOROUS MATERIALS, 2021, 311
[2]   Integration of chemical catalysis with extractive fermentation to produce fuels [J].
Anbarasan, Pazhamalai ;
Baer, Zachary C. ;
Sreekumar, Sanil ;
Gross, Elad ;
Binder, Joseph B. ;
Blanch, Harvey W. ;
Clark, Douglas S. ;
Toste, F. Dean .
NATURE, 2012, 491 (7423) :235-239
[3]   Selective Decarboxylation of Fatty Acids Catalyzed by Pd-Supported Hierarchical ZSM-5 Zeolite [J].
Arroyo, Marta ;
Briones, Laura ;
Hernando, Hector ;
Escola, Jose M. ;
Serrano, David P. .
ENERGY & FUELS, 2021, 35 (21) :17167-17181
[4]   Heteroaggregation and Selective Deposition for the Fine Design of Nanoarchitectured Bifunctional Catalysts: Application to Hydroisomerization [J].
Ben Moussa, Olfa ;
Tinat, Lionel ;
Jin, Xiaojing ;
Baaziz, Walid ;
Durupthy, Olivier ;
Sayag, Celine ;
Blanchard, Juliette .
ACS CATALYSIS, 2018, 8 (07) :6071-6078
[5]   Domino Reaction Catalyzed by Zeolites with BrOnsted and Lewis Acid Sites for the Production of -Valerolactone from Furfural [J].
Bui, Linh ;
Luo, Helen ;
Gunther, William R. ;
Roman-Leshkov, Yuriy .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (31) :8022-8025
[6]   Al-modified Pd@mSiO2 core-shell catalysts for the selective hydrodeoxygenation of fatty acid esters: Influence of catalyst structure and Al atoms incorporation [J].
Cao, Xincheng ;
Zhao, Jiaping ;
Long, Feng ;
Zhang, Xiaolei ;
Xu, Junming ;
Jiang, Jianchun .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2022, 305
[7]   EFFECTS OF DIFFUSION ON FREE PRECESSION IN NUCLEAR MAGNETIC RESONANCE EXPERIMENTS [J].
CARR, HY ;
PURCELL, EM .
PHYSICAL REVIEW, 1954, 94 (03) :630-638
[8]   The effect of textural properties on the hydrogenation of succinic acid using palladium incorporated mesoporous supports [J].
Chung, Sang-Ho ;
Park, Young-Moo ;
Kim, Min-Sung ;
Lee, Kwan-Young .
CATALYSIS TODAY, 2012, 185 (01) :205-210
[9]   Heterogeneous Catalysis for Tandem Reactions [J].
Climent, Maria J. ;
Corma, Avelino ;
Iborra, Sara ;
Sabater, Maria J. .
ACS CATALYSIS, 2014, 4 (03) :870-891
[10]   Heterogeneous Catalysts for the One-Pot Synthesis of Chemicals and Fine Chemicals [J].
Climent, Maria J. ;
Corma, Avelino ;
Iborra, Sara .
CHEMICAL REVIEWS, 2011, 111 (02) :1072-1133