TY - JOUR
T1 - Carbon coated LaFe0.92Pd0.08O3 composites for catalytic transfer hydrogenation
T2 - Balance in the ability of substrates adsorption and conversion
AU - Wang, Bowen
AU - Zhang, Nan
AU - Xiao, Ping
AU - Zhang, Jian
AU - Carabineiro, Sónia A. C.
AU - Zhu, Junjiang
N1 - Funding Information:
Financial support provided by the National Natural Science Foundation of China (Nos. 42277485, 21976141, and 22102123), the Department of Science and Technology of Hubei Province (No. 2021CFA034), the Department of Education of Hubei Province (Nos. T2020011 and Q20211712), and the Opening Project of Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing & Finishing (Nos. STRZ202202 and STRZ202101) is gratefully acknowledged. S. A.C. C. acknowledges Fundaãço para a Ciência e a Tecnologia (FCT), Portuqal for Scientific Employment Stimulus-Institutional Call (CEEC-INST/00102/2018), and Associate Laboratory for Green Chemistry-LAQV financed by national funds from FCT/MCTES (UIDB/50006/2020 and UIDP/5006/2020).
Publisher Copyright:
© 2023, Tsinghua University Press.
PY - 2024/5
Y1 - 2024/5
N2 - Catalytic transfer hydrogenation (CTH) is a green and efficient pathway for selective hydrogenation of unsaturated aldehydes and ketones. However, managing the abilities of solid catalysts to adsorb substrates and to convert them into desired products is a challenging task. Herein, we report the synthesis of carbon coated LaFe0.92Pd0.08O3 composites (LFPO-8@C) for CTH of benzaldehyde (BzH) into benzyl alcohol (BzOH), using isopropanol (IPA) as hydrogen source. The coating with carbon improves the ability to adsorb/transfer reactants from solution to active sites, and the doping of Pd2+ at Fe3+ site strengthens the ability of LaFeO3 to convert BzH into BzOH. A balanced point between them (i.e., abilities to adsorb BzH and to convert BzH into BzOH) is obtained at LFPO-8@C, which exhibits a BzOH formation rate of 3.88 mmol⋅ggat-1⋅h-1 at 180 °C for 3 h, which is 1.50 and 2.72 times faster than those of LFPO-8 and LaFeO3@C. A reaction mechanism is proposed, in which the acidic sites (e.g., Fe4+, oxygen vacancy) are used for the activation of C=O bond of BzH and O–H bond of IPA, and the basic sites (e.g., lattice oxygen) for the activation of α–H (O–H) bond of IPA.[Figure not available: see fulltext.].
AB - Catalytic transfer hydrogenation (CTH) is a green and efficient pathway for selective hydrogenation of unsaturated aldehydes and ketones. However, managing the abilities of solid catalysts to adsorb substrates and to convert them into desired products is a challenging task. Herein, we report the synthesis of carbon coated LaFe0.92Pd0.08O3 composites (LFPO-8@C) for CTH of benzaldehyde (BzH) into benzyl alcohol (BzOH), using isopropanol (IPA) as hydrogen source. The coating with carbon improves the ability to adsorb/transfer reactants from solution to active sites, and the doping of Pd2+ at Fe3+ site strengthens the ability of LaFeO3 to convert BzH into BzOH. A balanced point between them (i.e., abilities to adsorb BzH and to convert BzH into BzOH) is obtained at LFPO-8@C, which exhibits a BzOH formation rate of 3.88 mmol⋅ggat-1⋅h-1 at 180 °C for 3 h, which is 1.50 and 2.72 times faster than those of LFPO-8 and LaFeO3@C. A reaction mechanism is proposed, in which the acidic sites (e.g., Fe4+, oxygen vacancy) are used for the activation of C=O bond of BzH and O–H bond of IPA, and the basic sites (e.g., lattice oxygen) for the activation of α–H (O–H) bond of IPA.[Figure not available: see fulltext.].
KW - catalytic transfer hydrogenation
KW - isopropanol
KW - LaFePdO
KW - porous carbon
KW - reaction mechanism
UR - http://www.scopus.com/inward/record.url?scp=85177475715&partnerID=8YFLogxK
U2 - 10.1007/s12274-023-6282-x
DO - 10.1007/s12274-023-6282-x
M3 - Article
AN - SCOPUS:85177475715
SN - 1998-0124
VL - 17
SP - 3724
EP - 3732
JO - Nano Research
JF - Nano Research
IS - 5
ER -