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Energy Conversion and Management
journal homepage: www.elsevier.com/locate/enconman
Green and sustainable methanol production from CO
2
over magnetized
FeeCu/core–shell and infiltrate mesoporous silica-aluminosilicates
Wasakon Umchoo
a,b
, Chuleehat Sriakkarin
a,b
, Waleeporn Donphai
a,b,
⁎
,
Chompunuch Warakulwit
b
, Yingyot Poo-arporn
c
, Pongsakorn Jantaratana
d
, Thongthai Witoon
a,b
,
Metta Chareonpanich
a,b,
⁎
a
KU-Green Catalysts Group, Center of Excellence on Petrochemical and Materials Technology, Department of Chemical Engineering, Faculty of Engineering, Kasetsart
University, Bangkok 10900, Thailand
b
NANOTEC Center for Nanoscale Materials Design for Green Nanotechnology and Center for Advanced Studies in Nanotechnology for Chemical, Food and Agricultural
Industries, KU Institute for Advanced Studies, Kasetsart University, Bangkok 10900, Thailand
c
Synchrotron Light Research Institute, Nakhon Ratchasima 30000, Thailand
d
Department of Physics, Faculty of Science, Kasetsart University, Bangkok 10900, Thailand
ARTICLE INFO
Keywords:
FeeCu catalyst
Mesoporous silica-aluminosilicate
Core-shell structure
Infiltrate structure
CO
2
hydrogenation
External magnetic field
ABSTRACT
In this present work, green and efficient utilization concepts in the form of the use of an external magnetic field
have been applied to improve catalytic performance in CO
2
hydrogenation. The 10Fee10Cu catalysts with two
types of supports, core–shell and infiltrate mesoporous silica-aluminosilicate materials, were applied under
external magnetic fields of different intensities (0, 20.8 mT, 27.7 mT) and orientations (north-to-south (N–S),
south-to-north (S–N) directions). It was found that a magnetic field considerably enhanced both CO
2
conversion
and methanol and DME selectivities. The highest CO
2
conversion was obtained over 10Fee10Cu/infiltrate
catalyst under the magnetic field conditions of 27.7 mT and 4N–S direction at 260 °C (conversion was 1.5 times
greater than that without a magnetic field). Under such conditions and at 240 °C, the highest methanol and DME
space time yields were obtained, with results 1.8–1.9 times higher than those of without a magnetic field. These
excellent performances could be ascribed to the superior adsorption of CO
2
and H
2
reactant gas molecules over
the surface of magnetized catalysts under external magnetic field. This leads to the advantages of the catalyzed
CO
2
hydrogenation–decreases in the operating temperature and simultaneous reduction in CO
2
emission to the
atmosphere. This therefore facilitates a carbon-neutral route of CO
2
utilization.
1. Introduction
Over the past decades, increases in carbon dioxide (CO
2
) emissions
have directly affected climate change and global warming [1–3]. These
large amounts of CO
2
come from human activities, combustion of coal
and fossil fuels as energy sources for industries, electricity production,
and transportation [1,2,4]. Indeed the carbon dioxide concentration in
the atmosphere has consequently risen from ∼280 ppm before the in-
dustrial revolution to ∼410 ppm in 2017, and is further predicted to
reach ∼570 ppm by the end of the century [5,6]. Consequently, utili-
zation of CO
2
to produce value-added chemicals, fuels, and alternative
energy can potentially minimize and improve global warming and cli-
mate change problems [2,4,7].
The development of emerging green technologies with environ-
mental sustainability has become an important issue. Among other
methods for CO
2
utilization, CO
2
hydrogenation reaction is one of the
most effective ways to approach the environmentally friendly synthesis
of sustainable chemicals and fuels [4,5,7,8]. It has been found that
methanol, dimethyl ether (DME), and chemical feedstock can be pro-
duced using a low reaction temperature and low pressure through this
hydrogenation reaction [7–10]. The drawback due to low methanol and
DME productions, the secondary reaction to carbon monoxide (CO) and
methane (CH
4
) was still significantly observed.
In order to improve methanol and DME selectivities, an external
magnetic field is of a great interest to be applied to a conventional
reactor. An external magnetic field has been successfully applied in
various processes especially a fluidized bed reactor––as a tool to control
movement of magnetic particles, eliminate slugging and channeling,
and reduce agglomeration of magnetic particles [11–13]. However,
there is little available research regarding the direct effect of external
https://doi.org/10.1016/j.enconman.2017.12.101
Received 26 October 2017; Received in revised form 20 December 2017; Accepted 31 December 2017
⁎
Corresponding authors at: KU-Green Catalysts Group, Center of Excellence on Petrochemical and Materials Technology, Department of Chemical Engineering, Faculty of Engineering,
Kasetsart University, Bangkok 10900, Thailand.
E-mail addresses: fengwod@ku.ac.th (W. Donphai), fengmtc@ku.ac.th (M. Chareonpanich).
Energy Conversion and Management 159 (2018) 342–352
0196-8904/ © 2018 Elsevier Ltd. All rights reserved.
T