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
收藏
页数:12
相关论文
共 81 条
[51]   Heterogeneous and homogeneous catalysis for the hydrogenation of carboxylic acid derivatives: history, advances and future directions [J].
Pritchard, James ;
Filonenko, Georgy A. ;
van Putten, Robbert ;
Hensen, Emiel J. M. ;
Pidko, Evgeny A. .
CHEMICAL SOCIETY REVIEWS, 2015, 44 (11) :3808-3833
[52]   A novel laboratory-based hard X-ray photoelectron spectroscopy system [J].
Regoutz, Anna ;
Mascheck, Manfred ;
Wiell, Tomas ;
Eriksson, Susanna K. ;
Liljenberg, Cristopher ;
Tetzner, Kornelius ;
Williamson, Benjamin A. D. ;
Scanlon, David O. ;
Palmgren, Paul .
REVIEW OF SCIENTIFIC INSTRUMENTS, 2018, 89 (07)
[53]   Bifunctional Catalysts for Upgrading of Biomass-Derived Oxygenates: A Review [J].
Robinson, Allison M. ;
Hensley, Jesse E. ;
Medlin, J. Will .
ACS CATALYSIS, 2016, 6 (08) :5026-5043
[54]   Nuclear spin relaxation as a probe of zeolite acidity: a combined NMR and TPD investigation of pyridine in HZSM-5 [J].
Robinson, Neil ;
Brauer, Pierre ;
York, Andrew P. E. ;
D'Agostino, Carmine .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2021, 23 (33) :17752-17760
[55]   Non-sulphide zeolite catalyst for bio-jet-fuel conversion [J].
Shahinuzzaman, M. ;
Yaakob, Zahira ;
Ahmed, Yunus .
RENEWABLE & SUSTAINABLE ENERGY REVIEWS, 2017, 77 :1375-1384
[56]   Pd/Nb2O5/SiO2 Catalyst for the Direct Hydrodeoxygenation of Biomass-Related Compounds to Liquid Alkanes under Mild Conditions [J].
Shao, Yi ;
Xia, Qineng ;
Liu, Xiaohui ;
Lu, Guanzhong ;
Wang, Yanqin .
CHEMSUSCHEM, 2015, 8 (10) :1761-1767
[57]   Recent progress on upgrading of bio-oil to hydrocarbons over metal/zeolite bifunctional catalysts [J].
Shi, Yanchun ;
Xing, Enhui ;
Wu, Kejing ;
Wang, Jianlong ;
Yang, Mingde ;
Wu, Yulong .
CATALYSIS SCIENCE & TECHNOLOGY, 2017, 7 (12) :2385-2415
[58]   Upgrading of palmitic acid to iso-alkanes over bi-functional Mo/ZSM-22 catalysts [J].
Shi, Yanchun ;
Cao, Yaya ;
Duan, Yanan ;
Chen, Hao ;
Chen, Yu ;
Yang, Mingde ;
Wu, Yulong .
GREEN CHEMISTRY, 2016, 18 (17) :4633-4648
[59]   Calculations of electron inelastic mean free paths. X. Data for 41 elemental solids over the 50eV to 200keV range with the relativistic full Penn algorithm [J].
Shinotsuka, H. ;
Tanuma, S. ;
Powell, C. J. ;
Penn, D. R. .
SURFACE AND INTERFACE ANALYSIS, 2015, 47 (09) :871-888
[60]   Efficient conversion of levulinic acid or furfuryl alcohol into alkyl levulinates catalyzed by heteropoly acid and ZrO2 bifunctionalized organosilica nanotubes [J].
Song, Daiyu ;
An, Sai ;
Sun, Yingnan ;
Guo, Yihang .
JOURNAL OF CATALYSIS, 2016, 333 :184-199