TY - JOUR
T1 - Tuning CO 2 conversion product selectivity of metal organic frameworks derived hybrid carbon photoelectrocatalytic reactors
AU - Maina, James W.
AU - Pozo-Gonzalo, Cristina
AU - Schütz, Jürg A.
AU - Wang, Jiangting
AU - Dumée, Ludovic F.
N1 - Funding Information:
The authors acknowledge the Australian Institute of Nuclear Science and Engineering (AINSE) for financial support, through Mr. James Maina AINSE postgraduate research award (PGRA), and acknowledge Australia’s Nuclear Science and Technology Organization (ANSTO) for RBS and PIXE beam time ( P 10990 ). L. F. DUMEE acknowledges the ARC DECRA scheme for his DE180100130 Fellowship. The authors also acknowledge Dr. Luke Grundy (CSIRO) for his assistance in gas chromatography, Mr. Guanghui Zhu (Georgia Institute of Technology) for his assistance in methane adsorption studies and Prof. Lingxue Kong for his support and advice.
Publisher Copyright:
© 2019 Elsevier Ltd
PY - 2019/7
Y1 - 2019/7
N2 - Photo/electrocatalytic conversion of carbon dioxide (CO 2 ), has potential to address the adverse environmental impact of global warming. However, it is challenging to control the reactions to yield a specific product, and most catalyst produce a mixture of product that may include methanol, carbon monoxide (CO), methane among others. Metal organic frameworks (MOFs) derived carbon catalysts have potential to facilitate selective CO 2 conversion, owing to their regular microporous structure, in addition to enhanced chemical stability and electrical conductivity as compared to the precursor MOFs. However, there are no established techniques for immobilizing these catalysts directly on the surface a conductive substrate, without the need of polymer adhesives. Here, MOF-derived hybrid carbon photoelectrocatalytic reactors were successfully fabricated on the surface of macroporous metal support, by direct carbonization of the metal supported MOF membranes. The carbonization resulted in a dramatic improvement in electrocatalytic performance, with samples carbonized at 700 °C producing up to 9 times higher methanol yield as compared to non-carbonized membranes. The product selectivity could also be tuned from methanol, to CO or a mixture of both, by switching between electrocatalysis and photocatalysis. This work opens route for the development of robust metal supported carbonized MOF-based catalysts, for energy conversion applications.
AB - Photo/electrocatalytic conversion of carbon dioxide (CO 2 ), has potential to address the adverse environmental impact of global warming. However, it is challenging to control the reactions to yield a specific product, and most catalyst produce a mixture of product that may include methanol, carbon monoxide (CO), methane among others. Metal organic frameworks (MOFs) derived carbon catalysts have potential to facilitate selective CO 2 conversion, owing to their regular microporous structure, in addition to enhanced chemical stability and electrical conductivity as compared to the precursor MOFs. However, there are no established techniques for immobilizing these catalysts directly on the surface a conductive substrate, without the need of polymer adhesives. Here, MOF-derived hybrid carbon photoelectrocatalytic reactors were successfully fabricated on the surface of macroporous metal support, by direct carbonization of the metal supported MOF membranes. The carbonization resulted in a dramatic improvement in electrocatalytic performance, with samples carbonized at 700 °C producing up to 9 times higher methanol yield as compared to non-carbonized membranes. The product selectivity could also be tuned from methanol, to CO or a mixture of both, by switching between electrocatalysis and photocatalysis. This work opens route for the development of robust metal supported carbonized MOF-based catalysts, for energy conversion applications.
KW - Carbonized MOFs
KW - CO adsorption
KW - CO conversion
KW - Metal organic frameworks (MOFs)
KW - Photoelectrocatalytic reactors
UR - http://www.scopus.com/inward/record.url?scp=85063338279&partnerID=8YFLogxK
U2 - 10.1016/j.carbon.2019.03.043
DO - 10.1016/j.carbon.2019.03.043
M3 - Article
AN - SCOPUS:85063338279
SN - 0008-6223
VL - 148
SP - 80
EP - 90
JO - Carbon
JF - Carbon
ER -