3D printed catalytic reactors for aerobic selective oxidation of benzyl alcohol into benzaldehyde in continuous multiphase flow

被引:17
作者
Jacquot, Clement [1 ,2 ]
Middelkoop, Vesna [2 ]
Koeckritz, Angela [3 ]
Pohar, Andrej
Bienert, Regina [3 ]
Kellici, Suela [5 ]
Baragau, Ioan-Alexandru [5 ]
Venezia, Baldassarre [4 ]
Gavriilidis, Asterios [4 ]
Likozar, Blaz [6 ]
Beale, Andrew M. [1 ,7 ]
机构
[1] UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England
[2] VITO, Flemish Inst Technol Res, Sustainable Mat Management, Boeretang 200, B-2400 Mol, Belgium
[3] LIKAT, Leibniz Inst Katalyse, Albert Einstein Str 29A, D-18059 Rostock, Germany
[4] UCL, Dept Chem Engn, Torrington Pl, London WC1E 7JE, England
[5] London South Bank Univ, Sch Engn, 103 Borough Rd, London SE1 0AA, England
[6] Natl Inst Chem, Hajdrihova 19,POB 660, SI-1001 Ljubljana, Slovenia
[7] Rutherford Appleton Lab, Res Complex Harwell, Didcot OX11 0FA, Oxon, England
关键词
Continuous flow reactor; Heterogeneous catalysis; 3D printed catalysts; Benzyl alcohol oxidation; Alcohol aerobic oxidation; HETEROGENEOUS COPPER; KINETIC-MODELS; OXYGEN; WATER;
D O I
10.1016/j.susmat.2021.e00329
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this work, novel, patterned monolithic reactors were devised to explore more efficient routes for reactant conversion in order to investigate their potential to replace the packed bed and batch reactors conventionally employed in chemical industries. Well-defined bimetallic formulations were developed to substitute platinum group metals and critical raw materials such as palladium and cobalt, at least in part, by less active, but more sustainable and cost-effective metals such as earth-abundant iron. FePd and FeCo based monoliths were 3D printed and stacked in a continuous flow tubular reactor for testing the selective oxidation of benzyl alcohol (BA) into benzaldehyde (BZ) under mild conditions (80-100 degrees C and atmospheric pressure). The novel monolithic reactors were evaluated against current state-of-the-art reactor technologies, conventional packed bed and batch reactors. The FeCo- and FePd-Al2O3-supported monolithic catalyst beds showed higher conversion and TOF than their packed bed counterparts under the same operating conditions, revealing the impact of the novel design on both regular geometry and composition. What is of particular interest in the catalytic measurements shown is that the combined stacking of two monoliths in a flow reactor, Al2O3-supported Fe and GO-supported FePd catalysts, can significantly improve the performance with an increase in TOF of up to 90% in comparison to their FePd analogues. Mathematical modelling was used to obtain additional insights into the physical and chemical processes governing the rate of BA conversion. It was found that due to the flow regime inside the microchannels, an axial dispersion model was appropriate, which allowed for mapping the concentration profiles of the reactants and products within the respective monolith geometries.
引用
收藏
页数:12
相关论文
共 45 条
[1]   Development of a continuous flow reactor for pharmaceuticals using catalytic monoliths: Pt/C selective oxidation of benzyl alcohol [J].
Al Badran, F. ;
Awdry, S. ;
Kolaczkowski, S. T. .
CATALYSIS TODAY, 2013, 216 :229-239
[2]   Green synthesis of Pd@graphene nanocomposite: Catalyst for the selective oxidation of alcohols [J].
Al-Marri, Abdulhadi H. ;
Khan, Merajuddin ;
Shaik, Mohammed Rafi ;
Mohri, Nils ;
Adil, Syed Farooq ;
Kuniyil, Mufsir ;
Alkhathlan, Hamad Z. ;
Al-Warthan, Abdulrahman ;
Tremel, Wolfgang ;
Tahir, Muhammad Nawaz ;
Khan, Mujeeb ;
Siddiqui, Mohammed Rafiq H. .
ARABIAN JOURNAL OF CHEMISTRY, 2016, 9 (06) :835-845
[3]  
[Anonymous], 2015, CHEM ENG TRANS, P1369, DOI [10.3303/CET1545229, DOI 10.3303/CET1545229]
[4]   An efficient and recyclable 3D printed α-Al2O3 catalyst for the multicomponent assembly of bioactive heterocycles [J].
Azuaje, Jhonny ;
Tubio, Carmen R. ;
Escalante, Luz ;
Gomez, Monica ;
Guitian, Francisco ;
Coelho, Alberto ;
Caamano, Olga ;
Gil, Alvaro ;
Sotelo, Eddy .
APPLIED CATALYSIS A-GENERAL, 2017, 530 :203-210
[5]   Selective oxidation of alcohols in a continuous multifunctional reactor: Ruthenium oxide catalysed oxidation of benzyl alcohol [J].
Bavykin, DV ;
Lapkin, AA ;
Kolaczkowski, ST ;
Plucinski, PK .
APPLIED CATALYSIS A-GENERAL, 2005, 288 (1-2) :175-184
[6]   Highly selective oxidation of benzyl alcohol catalyzed by new peripherally tetra-substituted Fe(II) and Co(II) phthalocyanines [J].
Cakir, Volkan ;
Saka, Ece Tugba ;
Biyiklioglu, Zekeriya ;
Kantekin, Halit .
SYNTHETIC METALS, 2014, 197 :233-239
[7]   Copper, copper oxide nanoparticles and copper complexes supported on mesoporous SBA-15 as catalysts in the selective oxidation of benzyl alcohol in aqueous phase [J].
Cruz, Paula ;
Perez, Yolanda ;
del Hierro, Isabel ;
Fajardo, Mariano .
MICROPOROUS AND MESOPOROUS MATERIALS, 2016, 220 :136-147
[8]   Oxidation of benzyl alcohols to aldehydes and ketones under air in water using a polymer supported palladium catalyst [J].
Dell'Anna, Maria Michela ;
Mali, Matilda ;
Mastrorilli, Piero ;
Cotugno, Pietro ;
Monopoli, Antonio .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2014, 386 :114-119
[9]   Kinetic modelling of benzyl alcohol selective oxidation in aqueous mixtures of nitric and sulfuric acids [J].
Di Somma, I. ;
Russo, D. ;
Andreozzi, R. ;
Marotta, R. ;
Guido, S. .
CHEMICAL ENGINEERING JOURNAL, 2017, 308 :738-744
[10]   Three-Dimensional Printing in Catalysis: Combining 3D Heterogeneous Copper and Palladium Catalysts for Multicatalytic Multicomponent Reactions [J].
Diaz-Marta, Antonio S. ;
Tubio, Carmen R. ;
Carbajales, Carlos ;
Fernandez, Carmen ;
Escalante, Luz ;
Sotelo, Eddy ;
Guitian, Francisco ;
Laura Barrio, V. ;
Gil, Alvaro ;
Coelho, Alberto .
ACS CATALYSIS, 2018, 8 (01) :392-404