Highly Efficient N-Doped Carbon-Supported Subnanometer Cobalt-Zinc Bimetallic Catalysts for Decarbonylation of Fatty Acids into Long-Chain Olefins

被引:6
作者
Zhang, Zhenya [1 ,2 ]
Li, Bolong [1 ,2 ]
Wang, Jianghao [1 ,2 ]
Li, Jing [1 ,2 ]
Fu, Jie [1 ,2 ]
机构
[1] Zhejiang Univ, Coll Chem & Biol Engn, Key Lab Biomass Chem Engn, Minist Educ, Hangzhou 310058, Peoples R China
[2] Inst Zhejiang Univ Quzhou, Quzhou 324000, Zhejiang, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
renewable fatty acids; CoZn@NC catalysts; decarbonylativedehydration; long-chain olefins; inhibiting cracking; ALIPHATIC CARBOXYLIC-ACIDS; STEARIC-ACID; ALPHA-OLEFINS; DEOXYGENATION; HYDROCARBONS; DECARBOXYLATION; DEHYDRATION; CONVERSION; KINETICS; CRACKING;
D O I
10.1021/acssuschemeng.3c06906
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The quest for economical and efficient heterogeneous catalysts for the synthesis of long-chain alpha-olefins from biomass-derived fatty acids is of utmost significance. Regrettably, the generation of olefins by the dehydrative decarbonylation of fatty acids without the inclusion of additives is seldom documented. This scarcity is mostly attributed to the occurrence of competing decarboxylation and cracking processes. In this study, bimetallic CoZn@NC catalysts were prepared by decomposing ZIFs (CoZn) via a semisacrificial template-assisted strategy. The resulting CoZn@NC-900 catalysts are highly efficient and outperform Pt/C in stearic acid decarbonylation. In a batch reactor, these catalysts demonstrate 85.8% stearic acid conversion with up to 52.4% combined alkene yield at 350 C-degrees for 1 h. The binding of N and Co forms the active decarbonylation sites, while Zn promotes the formation of Co subnanoparticles through spatial segregation effects, effectively reducing the acidity of the catalyst and thus ultimately inhibiting C-C cracking. Moreover, the CoZn@NC catalysts showed good stability, and the catalytic decarbonylation activity was maintained after several consecutive uses. This work presents a cost-effective strategy for the efficient catalytic decarbonylation of carboxylic acids with the inhibition of C-C cracking and shows promise for enabling the production of high-value olefins from biomass sources.
引用
收藏
页码:1320 / 1332
页数:13
相关论文
共 65 条
[1]   Effects of Metal and Method Used for Synthesis of Supported Catalysts on Catalytic Performance in Olefin Production from Fatty Acids [J].
Berenblyum, A. S. ;
Kuznetsov, P. S. ;
Danyushevsky, V. Ya ;
Lazov, M. A. ;
Katsman, E. A. .
PETROLEUM CHEMISTRY, 2022, 62 (05) :552-560
[2]   Oils and Fats as Renewable Raw Materials in Chemistry [J].
Biermann, Ursula ;
Bornscheuer, Uwe ;
Meier, Michael A. R. ;
Metzger, Juergen O. ;
Schaefer, Hans J. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (17) :3854-3871
[3]   Investigation of the role of Nb on Pd-Zr-Zn catalyst in methanol steam reforming for hydrogen [J].
Cai, Fufeng ;
Lu, Peijing ;
Ibrahim, Jessica Juweriah ;
Fu, Yu ;
Zhang, Jun ;
Sun, Yuhan .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2019, 44 (23) :11717-11733
[4]   Tuning the Electronic Structure of CoO Nanowire Arrays by N-Doping for Efficient Hydrogen Evolution in Alkaline Solutions [J].
Cao, Maoqi ;
Li, Xiaofeng ;
Xiang, Dingding ;
Wu, Dawang ;
Sun, Sailan ;
Dai, Hongjing ;
Luo, Jun ;
Zou, Hongtao .
CATALYSTS, 2021, 11 (10)
[5]   Metal/Porous Carbon Composites for Heterogeneous Catalysis: Old Catalysts with Improved Performance Promoted by N-Doping [J].
Cao, Yueling ;
Mao, Shanjun ;
Li, Mingming ;
Chen, Yiqing ;
Wang, Yong .
ACS CATALYSIS, 2017, 7 (12) :8090-8112
[6]   Nitrogen-coordinated single-atom catalysts with manganese and cobalt sites for acidic oxygen reduction [J].
Chao, Guojie ;
Zhang, Yizhe ;
Zhang, Longsheng ;
Zong, Wei ;
Zhang, Nan ;
Xue, Tiantian ;
Fan, Wei ;
Liu, Tianxi ;
Xie, Yi .
JOURNAL OF MATERIALS CHEMISTRY A, 2022, 10 (11) :5930-5936
[7]   A Heterogeneous Catalyst for the Transformation of Fatty Acids to α-Olefins [J].
Chatterjee, Anamitra ;
Jensen, Vidar R. .
ACS CATALYSIS, 2017, 7 (04) :2543-2547
[8]   Palladium Precatalysts for Decarbonylative Dehydration of Fatty Acids to Linear Alpha Olefins [J].
Chatterjee, Anamitra ;
Eliasson, Sondre H. Hopen ;
Tornroos, Karl W. ;
Jensen, Vidar R. .
ACS CATALYSIS, 2016, 6 (11) :7784-7789
[9]  
Chieregato A., 2016, CHEM FUELS BIOBASED, P1, DOI [10.1002/9783527698202, DOI 10.1002/9783527698202]
[10]  
Dawes GJS, 2015, GREEN CHEM, V17, P3231, DOI [10.1039/C5GC00023H, 10.1039/c5gc00023h]