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Author Van Daele, K.; Balalta, D.; Hoekx, S.; Jacops, R.; Daems, N.; Altantzis, T.; Pant, D.; Breugelmans, T.
Title Synergy or Antagonism? Exploring the Interplay of SnO2and an N-OMC Carbon Capture Medium for the Electrochemical CO2Reduction toward Formate Type A1 Journal Article
Year 2024 Publication ACS Applied Energy Materials Abbreviated Journal ACS Appl. Energy Mater.
Volume 7 Issue 13 Pages 5517-5527
Keywords A1 Journal Article; nitrogen-doped ordered mesoporous carbon, SnO2, degradation pathways, electrochemical CO2 reduction, formate; Electron Microscopy for Materials Science (EMAT) ;
Abstract Closing the anthropogenic carbon cycle by means of the sustainable electrochemical CO2 reduction (eCO2R) toward formate (FA) is a promising strategy for CO2 abatement, clearing the path toward a carbon neutral future. Currently, three possible reaction pathways have been identified for the eCO2R toward FA, all of which are initiated by the adsorption of CO2 on the electrocatalyst’s surface. Therefore, a possible strategy to enhance the availability of CO2 near the active sites is to combine an active electrocatalyst material (here, SnO2) with a known carbon capture medium (here, nitrogen-doped ordered mesoporous carbon (N-OMC)). SnO2 was introduced in situ during the N-OMC synthesis, yielding SnO2-N-OMCs. We approached the state of the art for Sn-based N-doped carbon electrocatalysts in terms of performance under industrially relevant currents with an average FEFA of 59% for SnO2-N-OMC (6) and 61% for SnO2-N-OMC (2). Moreover, the SnO2-N-OMC electrocatalysts require a low overpotential, courtesy of the N-OMC support, compared to the state of the art, for the selective conversion of CO2 toward FA at the industrially relevant current density of 100 mA cm–2. Additionally, the 24 h stability of the best performing SnO2-N-OMC electrocatalysts is explored, and pulverization/agglomeration and in situ SnO2 reduction are identified as major degradation pathways, allowing future research to be steered more accurately toward more stable Sn-based electrocatalysts for the eCO2R toward FA. An optimal combination of both the SnO2 species and the N-OMC carbon capture medium could result in a synergistic effect, especially when utilization of the N-OMC support material is optimized to morphologically stabilize the SnO2 active species.
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Language Wos (down) https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=brocade2&SrcAuth=WosAPI&KeyUT=WOS:001253 Publication Date 2024-07-08
Series Editor Series Title Abbreviated Series Title
Series Volume Series Issue Edition
ISSN 2574-0962 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 6.4 Times cited Open Access
Notes K.V.D. received financial support through a PhD fellowship strategic basic research (1S83320N) from the Research Foundation Flanders (FWO). Additionally, this project received funding in the framework of the Catalisti cluster SBO project CO2PERATE (“All renewable CCU based on formic acid integrated in an industrial micro-grid”), with financial support of VLAIO (Flemish Agency for Innovation and Entrepreneurship) (UA & VITO). Furthermore, this research was supported by the Interreg 2 Seas-program 2014–2020, cofunded by the European Regional Development Fund under subsidy contract no. E2C 2S03-019 (UA & VITO). D.B. and D.P. acknowledge the support from European Union’s Horizon 2020 MSCA-ITN programme under grant agreement no. 955650 (CATCHY). S.H. is financially supported through a PhD fellowship strategic basic research (1S42623N) from the Research Foundation Flanders (FWO). R.J. received financial support of the federal Energy Transition Fund by FPS Economy. T.A. acknowledges funding from the University of Antwerp Research fund (BOF). We acknowledge Prof. Tom Hauffman and Kitty Baert from the Electrochemical and Surface Engineering research group (SURF) at the VUB (Vrije Universiteit Brussel) for the XPS measurements, Prof. Christophe Vande Velde from the Intelligence in Processes, Advanced Catalysts and Solvents (iPRACS, UAntwerp) research group for the XRD analysis, and Prof. Pegie Cool, Prof. Vera Meynen, and Radu-George Ciocarlan from the Laboratory of Adsorption and Catalysis (LADCA, UAntwerp) for the nitrogen physisorption and Raman spectroscopy measurements. Approved Most recent IF: 6.4; 2024 IF: NA
Call Number EMAT @ emat @c:irua:206409 Serial 9261
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Author Li, C.; Tardajos, A.P.; Wang, D.; Choukroun, D.; Van Daele, K.; Breugelmans, T.; Bals, S.
Title A simple method to clean ligand contamination on TEM grids Type A1 Journal article
Year 2021 Publication Ultramicroscopy Abbreviated Journal Ultramicroscopy
Volume 221 Issue Pages 113195
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Colloidal nanoparticles (NPs) including nanowires and nanosheets made by chemical methods involve many organic ligands. When the structure of NPs is investigated via transmission electron microscopy (TEM), the organic ligands act as a source for e-beam induced deposition and this causes substantial build-up of carbon layers in the investigated areas, which is typically referred to as “contamination” in the eld of electron mi- croscopy. This contamination is often more severe for scanning TEM, a technique that is based on a focused electron beam and hence higher electron dose rate. In this paper, we report a simple and effective method to clean drop-cast TEM grids that contain NPs with ligands. Using a combination of activated carbon and ethanol, this method effectively reduces the amount of ligands on TEM grids, and therefore greatly improves the quality of electron microscopy images and subsequent analytical measurements. This ef cient and facile method can be helpful during electron microscopy investigation of different kinds of nanomaterials that suffer from ligand- induced contamination.
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Language Wos (down) 000612539600002 Publication Date 0000-00-00
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ISSN 0304-3991 ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor 2.843 Times cited 10 Open Access OpenAccess
Notes This research was funded by the University Antwerp GOA project (ID 33928). DW acknowledges an Individual Fellowship funded by the Marie Sklodowska-Curie Actions (MSCA) in Horizon 2020 program (grant 894254 SuprAtom). Approved Most recent IF: 2.843
Call Number EMAT @ emat @c:irua:174947 Serial 6666
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Author Daems, N.; De Mot, B.; Choukroun, D.; Van Daele, K.; Li, C.; Hubin, A.; Bals, S.; Hereijgers, J.; Breugelmans, T.
Title Nickel-containing N-doped carbon as effective electrocatalysts for the reduction of CO2 to CO in a continuous-flow electrolyzer Type A1 Journal article
Year 2019 Publication Sustainable energy & fuels Abbreviated Journal
Volume 4 Issue 4 Pages 1296-1311
Keywords A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Abstract Nickel-containing N-doped carbons were synthesized for the electrochemical reduction of CO2 to CO, which is a promising approach to reduce the atmospheric CO2 levels and its negative impact on the environment. Unfortunately, poor performance (activity, selectivity and/or stability) is still a major hurdle for the economical implementation of this type of materials. The electrocatalysts were prepared through an easily up-scalable and easily tunable method based on the pyrolysis of Ni-containing N-doped carbons. Ni–N–AC–B1 synthesized with a high relative amount of nitrogen and nickel with respect to carbon, was identified as the most promising candidate for this reaction based on its partial CO current density (4.2 mA cm−2), its overpotential (0.57 V) and its faradaic efficiency to CO (>99%). This results in unprecedented values for the current density per g active sites (690 A g−1 active sites). Combined with its decent stability and its high performance in an actual electrolyzer setup, this makes it a promising candidate for the electrochemical reduction of CO2 to CO on a larger scale. Finally, the evaluation of this kind of material in a flow-cell setup has been limited and to the best of our knowledge never included an evaluation of several crucial parameters (e.g. electrolyte type, anode composition and membrane type) and is an essential investigation in the move towards up-scaling and ultimately industrial application of this technique. This study resulted in an optimal cell configuration, consisting of Pt as an anode, Fumatech® as the membrane and 1 M KHCO3 and 2 M KOH as catholyte and anolyte, respectively. In conclusion, this research offers a unique combination of electrocatalyst development and reactor optimization.
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Language Wos (down) 000518690900030 Publication Date 2019-12-20
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ISSN ISBN Additional Links UA library record; WoS full record; WoS citing articles
Impact Factor Times cited 14 Open Access OpenAccess
Notes ; The authors acknowledge sponsoring from the research foundation of Flanders (FWO) in the frame of a post-doctoral grant (12Y3919N – ND). J. Hereijgers was supported through a postdoctoral fellowship (28761) of the Research Foundation Flanders (FWO). This project was co-funded by the Interreg 2 Seas-Program 2014-2020, co-.nanced by the European Fund for Regional Development in the frame of subsidiary contract nr 2S03-019. This work was further performed in the framework of the Catalisti cluster SBO project CO2PERATE (“All renewable CCU based on formic acid integrated in an industrial microgrid”), with the.nancial support of VLAIO (Flemish Agency for Innovation and Entrepreneurship). This project.nally received funding from the European Research Council (ERC Consolidator Grant 815128, REALNANO). We thank Karen Leyssens for helping with the N<INF>2</INF> physisorption measurements and Kitty Baert (VUB) for analyzing the samples with XPS and Raman. ; sygma Approved Most recent IF: NA
Call Number UA @ admin @ c:irua:165482 Serial 6311
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