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Cooperative defect-enriched SiO2 for oxygen activation and organic dehydrogenation
Saputera W.H.a,b, Tahini H.A.c, Lovell E.C.a, Tan T.H.a, Rawal A.a, Aguey-Zinsou K.-F.a, Friedmann D.a,d, Smith S.C.c, Amal R.a, Scott J.a
a Particles and Catalysis Research Group, School of Chemical Engineering, The University of New South Wales, Sydney, 2052, Australia
b Department of Chemical Engineering, Institut Teknologi Bandung, Bandung, 40132, Indonesia
c Integrated Materials Design Laboratory, Research School of Physics and Engineering, The Australian National University, Canberra, 2601, Australia
d School of Chemistry, RMIT, Melbourne, 3000, Australia
[vc_row][vc_column][vc_row_inner][vc_column_inner][vc_separator css=”.vc_custom_1624529070653{padding-top: 30px !important;padding-bottom: 30px !important;}”][/vc_column_inner][/vc_row_inner][vc_row_inner layout=”boxed”][vc_column_inner width=”3/4″ css=”.vc_custom_1624695412187{border-right-width: 1px !important;border-right-color: #dddddd !important;border-right-style: solid !important;border-radius: 1px !important;}”][vc_empty_space][megatron_heading title=”Abstract” size=”size-sm” text_align=”text-left”][vc_column_text]© 2019 Elsevier Inc.Tailoring oxide functionalities via defect engineering is an effective approach in many advanced materials. Here we report that introducing defect sites in SiO2 via sequential hydrogenation and UV light pre-treatment steps can invoke synergism for oxygen activation and organic dehydrogenation under ambient conditions in the absence of light. The hydrogenation step is proposed to break Si–O–Si bonds to give an E′δ center – silanol pair. UV light pre-treatment then serves to dehydroxylate the silanol group to give a non-bridging oxygen hole centers (NBOHC). The two defect sites work in harmony to activate oxygen and in turn oxidize formic acid. First-principles calculations indicated that UV light pre-treatment lowered the energy barrier for oxygen activation and formic acid decomposition on the defect sites. Re-illuminating the used SiO2 led to partial recovery of the defect sites and hence oxidation performance. The study demonstrates the capacity for generating synergistic defects in simple metal oxides as an effective way to enhance performance for oxidation processes.[/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”Author keywords” size=”size-sm” text_align=”text-left”][vc_column_text]Advanced materials,Effective approaches,First-principles calculation,Formic acid decompositions,Nonbridging oxygen hole center,Oxygen activations,Pre-Treatment,SiO2[/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”Indexed keywords” size=”size-sm” text_align=”text-left”][vc_column_text]Defects,Dehydrogenation,E′δ center,Non-bridging oxygen hole center (NBOHC),Oxygen activation,SiO2,UV light pre-treatment[/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”Funding details” size=”size-sm” text_align=”text-left”][vc_column_text][{‘$’: ‘The work was supported by the Australian Research Council under The Laureate Fellowship Scheme – FL140100081 . W.H. Saputera thanks the Indonesia Endowment Fund for Education (LPDP), Republic of Indonesia for his personal PhD fellowship. The authors would like to acknowledge the UNSW Mark Wainwright Analytical Center for their assistance with XPS, TEM, FTIR, XRD, NMR and EPR measurements and analyses. This research was also undertaken with the assistance of computational resources provided by the Australian Government through National Computational Infrastructure (NCI) under the National Computational Merit Allocation Scheme.’}, {‘$’: ‘The work was supported by the Australian Research Council under The Laureate Fellowship Scheme ? FL140100081. W.H. Saputera thanks the Indonesia Endowment Fund for Education (LPDP), Republic of Indonesia for his personal PhD fellowship. The authors would like to acknowledge the UNSW Mark Wainwright Analytical Center for their assistance with XPS, TEM, FTIR, XRD, NMR and EPR measurements and analyses. This research was also undertaken with the assistance of computational resources provided by the Australian Government through National Computational Infrastructure (NCI) under the National Computational Merit Allocation Scheme.’}][/vc_column_text][vc_empty_space][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][vc_empty_space][megatron_heading title=”DOI” size=”size-sm” text_align=”text-left”][vc_column_text]https://doi.org/10.1016/j.jcat.2019.07.006[/vc_column_text][/vc_column_inner][vc_column_inner width=”1/4″][vc_column_text]Widget Plumx[/vc_column_text][/vc_column_inner][/vc_row_inner][/vc_column][/vc_row][vc_row][vc_column][vc_separator css=”.vc_custom_1624528584150{padding-top: 25px !important;padding-bottom: 25px !important;}”][/vc_column][/vc_row]