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Gupta, A.; Baron, G.V.; Perreault, P.; Lenaerts, S.; Ciocarlan, R.-G.; Cool, P.; Mileo, P.G.M.; Rogge, S.; Van Speybroeck, V.; Watson, G.; Van Der Voort, P.; Houlleberghs, M.; Breynaert, E.; Martens, J.; Denayer, J.F.M. |
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Title |
Hydrogen clathrates : next generation hydrogen storage materials |
Type |
A1 Journal article |
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Year |
2021 |
Publication |
Energy Storage Materials |
Abbreviated Journal |
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Volume |
41 |
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Pages |
69-107 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Extensive research has been carried on the molecular adsorption in high surface area materials such as carbonaceous materials and MOFs as well as atomic bonded hydrogen in metals and alloys. Clathrates stand among the ones to be recently suggested for hydrogen storage. Although, the simulations predict lower capacity than the expected by the DOE norms, the additional benefits of clathrates such as low production and operational cost, fully reversible reaction, environmentally benign nature, low risk of flammability make them one of the most promising materials to be explored in the next decade. The inherent ability to tailor the properties of clathrates using techniques such as addition of promoter molecules, use of porous supports and formation of novel reverse micelles morphology provide immense scope customisation and growth. As rapidly evolving materials, clathrates promise to get as close as possible in the search of “holy grail” of hydrogen storage. This review aims to provide the audience with the background of the current developments in the solid-state hydrogen storage materials, with a special focus on the hydrogen clathrates. The in-depth analysis of the hydrogen clathrates will be provided beginning from their discovery, various additives utilised to enhance their thermodynamic and kinetic properties, challenges in the characterisation of hydrogen in clathrates, theoretical developments to justify the experimental findings and the upscaling opportunities presented by this system. The review will present state of the art in the field and also provide a global picture for the path forward. |
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Wos |
000685118300009 |
Publication Date |
2021-06-08 |
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ISSN |
2405-8297 |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Times cited |
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Open Access |
OpenAccess |
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Most recent IF: NA |
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Call Number |
UA @ admin @ c:irua:178744 |
Serial |
8045 |
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Author |
Van Everbroeck, T.; Wu, J.; Arenas-Esteban, D.; Ciocarlan, R.-G.; Mertens, M.; Bals, S.; Dujardin, C.; Granger, P.; Seftel, E.M.; Cool, P. |
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Title |
ZnAl layered double hydroxide based catalysts (with Cu, Mn, Ti) used as noble metal-free three-way catalysts |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Applied clay science |
Abbreviated Journal |
Appl Clay Sci |
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Volume |
217 |
Issue |
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Pages |
106390 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA) |
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Wos |
000795870100004 |
Publication Date |
2022-01-02 |
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Edition |
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ISSN |
0169-1317 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.6 |
Times cited |
6 |
Open Access |
OpenAccess |
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Notes |
The authors acknowledge financial support by theEuropean Union’s Horizon 2020 Project Partial-PGMs (H2020-NMP-686086). R-G C. and P.C. acknowledge the FWO-Flanders (project no. G038215N) for financial support. S⋅B and D.A.E thank the financial support of the European Research Council (ERC-CoG-2019 815128). The authors are grateful to Johnson Matthey, UK, for supplying the commercial benchmark catalysts; realnano; sygmaSB |
Approved |
Most recent IF: 5.6 |
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Call Number |
EMAT @ emat @c:irua:186956 |
Serial |
6955 |
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Author |
Pacquets, L.; Van den Hoek, J.; Arenas Esteban, D.; Ciocarlan, R.-G.; Cool, P.; Baert, K.; Hauffman, T.; Daems, N.; Bals, S.; Breugelmans, T. |
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Title |
Use of nanoscale carbon layers on Ag-based gas diffusion electrodes to promote CO production |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
ACS applied nano materials |
Abbreviated Journal |
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Volume |
5 |
Issue |
6 |
Pages |
7723-7732 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT) |
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Abstract |
A promising strategy for the inhibition of the hydrogen evolution reaction along with the stabilization of the electrocatalyst in electrochemical CO2 reduction cells involves the application of a nanoscale amorphous carbon layer on top of the active catalyst layer in a gas diffusion electrode. Without modifying the chemical nature of the electrocatalyst itself, these amorphous carbon layers lead to the stabilization of the electrocatalyst, and a significant improvement with respect to the inhibition of the hydrogen evolution reaction was also obtained. The faradaic efficiencies of hydrogen could be reduced from 31.4 to 2.1% after 1 h of electrolysis with a 5 nm thick carbon layer. Furthermore, the impact of the carbon layer thickness (5–30 nm) on this inhibiting effect was investigated. We determined an optimal thickness of 15 nm where the hydrogen evolution reaction was inhibited and a decent stability was obtained. Next, a thickness of 15 nm was selected for durability measurements. Interestingly, these durability measurements revealed the beneficial impact of the carbon layer already after 6 h by suppressing the hydrogen evolution such that an increase of only 37.9% exists compared to 56.9% without the use of an additional carbon layer, which is an improvement of 150%. Since carbon is only applied afterward, it reveals its great potential in terms of electrocatalysis in general. |
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Wos |
000818507900001 |
Publication Date |
2022-05-19 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2574-0970 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.9 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
L.P. was supported through a Ph.D. fellowship strategic basic research (1S56920N) of the Research Foundation-Flanders (FWO). S.B. acknowledges financial support from ERC Consolidator Grant Number 815128 REALNANO. This research was financed by the Research Council of the University of Antwerp (BOF-GOA 33928). P.C. and R.-G.C. acknowledge financial support by FWO Flanders (project no. G038215N). The authors recognize the contribution of S. Pourbabak and T. Derez for the assistance with the Ag and carbon coating, Indah Prihatiningtyas and Bart Van der Bruggen for the assistance with the contact angle measurements, Daniel Choukroun for the use of the in-house-made hybrid flow cell, and Stijn Van den Broeck for his assistance with the FIB measurements. |
Approved |
Most recent IF: 5.9 |
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Call Number |
UA @ admin @ c:irua:188887 |
Serial |
7099 |
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Author |
Volders, J.; Elen, K.; Raes, A.; Ninakanti, R.; Kelchtermans, A.-S.; Sastre, F.; Hardy, A.; Cool, P.; Verbruggen, S.W.; Buskens, P.; Van Bael, M.K. |
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Title |
Sunlight-powered reverse water gas shift reaction catalysed by plasmonic Au/TiO₂ nanocatalysts : effects of Au particle size on the activity and selectivity |
Type |
A1 Journal article |
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Year |
2022 |
Publication |
Nanomaterials |
Abbreviated Journal |
Nanomaterials-Basel |
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Volume |
12 |
Issue |
23 |
Pages |
4153-13 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
This study reports the low temperature and low pressure conversion (up to 160 °C, p = 3.5 bar) of CO2 and H2 to CO using plasmonic Au/TiO2 nanocatalysts and mildly concentrated artificial sunlight as the sole energy source (up to 13.9 kW·m-2 = 13.9 suns). To distinguish between photothermal and non-thermal contributors, we investigated the impact of the Au nanoparticle size and light intensity on the activity and selectivity of the catalyst. A comparative study between P25 TiO2-supported Au nanocatalysts of a size of 6 nm and 16 nm displayed a 15 times higher activity for the smaller particles, which can only partially be attributed to the higher Au surface area. Other factors that may play a role are e.g., the electronic contact between Au and TiO2 and the ratio between plasmonic absorption and scattering. Both catalysts displayed ≥84% selectivity for CO (side product is CH4). Furthermore, we demonstrated that the catalytic activity of Au/TiO2 increases exponentially with increasing light intensity, which indicated the presence of a photothermal contributor. In dark, however, both Au/TiO2 catalysts solely produced CH4 at the same catalyst bed temperature (160 °C). We propose that the difference in selectivity is caused by the promotion of CO desorption through charge transfer of plasmon generated charges (as a non-thermal contributor). |
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Wos |
000896093900001 |
Publication Date |
2022-11-24 |
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Edition |
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ISSN |
2079-4991 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.3 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 5.3 |
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Call Number |
UA @ admin @ c:irua:191843 |
Serial |
7341 |
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Permanent link to this record |
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Author |
Ciocarlan, R.-G.; Blommaerts, N.; Lenaerts, S.; Cool, P.; Verbruggen, S.W. |
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Title |
Recent trends in plasmon‐assisted photocatalytic CO₂ reduction |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Chemsuschem |
Abbreviated Journal |
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Volume |
16 |
Issue |
5 |
Pages |
e202201647-25 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Direct photocatalytic reduction of CO2 has become an highly active field of research. It is thus of utmost importance to maintain an overview of the various materials used to sustain this process, find common trends, and, in this way, eventually improve the current conversions and selectivities. In particular, CO2 photoreduction using plasmonic photocatalysts under solar light has gained tremendous attention, and a wide variety of materials has been developed to reduce CO2 towards more practical gases or liquid fuels (CH4, CO, CH3OH/CH3CH2OH) in this manner. This Review therefore aims at providing insights in current developments of photocatalysts consisting of only plasmonic nanoparticles and semiconductor materials. By classifying recent studies based on product selectivity, this Review aims to unravel common trends that can provide effective information on ways to improve the photoreduction yield or possible means to shift the selectivity towards desired products, thus generating new ideas for the way forward. |
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Wos |
000926901300001 |
Publication Date |
2023-01-10 |
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Abbreviated Series Title |
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Edition |
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ISSN |
1864-5631 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.4 |
Times cited |
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Open Access |
OpenAccess |
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Notes |
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Approved |
Most recent IF: 8.4; 2023 IF: 7.226 |
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Call Number |
UA @ admin @ c:irua:193633 |
Serial |
7335 |
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Permanent link to this record |
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Author |
Kummamuru, N.B.; Watson, G.; Ciocarlan, R.-G.; Verbruggen, S.W.; Cool, P.; Van Der Voort, P.; Perreault, P. |
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Title |
Accelerated methane storage in clathrate hydrates using mesoporous (Organo-) silica materials |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Fuel |
Abbreviated Journal |
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Volume |
354 |
Issue |
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Pages |
129403-129418 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Laboratory of adsorption and catalysis (LADCA); Sustainable Energy, Air and Water Technology (DuEL) |
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Abstract |
Methane (CH4) clathrate hydrates have gained much attention in the ever-growing search for novel energy storage methods; however, they are currently limited due to their poor water-to-hydrate conversions and slow formation kinetics. To surmount these bottlenecks, significant research has been centered on the design of novel methods (porous media). In this vein, the present work explores two hydrophobic mesoporous solids, an alkyl-grafted mesoporous silica (SBA-15 C8) and a periodic mesoporous organosilica (Ring-PMO), in their ability to promote CH4 clathrates. Both materials have shown to facilitate CH4 clathrate formation at mild operating conditions (6 MPa and 269–276 K). The study revealed that the maximal CH4 storage capacities are strongly linked to the critical/optimal quantity of water in the system which was determined to be at 130% and 200% of the pore volume for SBA-15 C8 and Ring-PMO, respectively. Up to 90% and 95% of the maximum water-to-hydrate conversions were achieved in 90 min at the lowest experimental temperature and critical water content for SBA-15 C8 and Ring-PMO, respectively. At these conditions, SBA-15 C8 and Ring-PMO showed a maximum gas uptake of 98.2 and 101.2 mmol CH4/mol H2O, respectively. Both the materials exhibited no chemical or morphological changes post-clathrate formations (characterized using FT-IR, N2 sorption, XRD, and TEM), inferring their viability as clathrate promoters for multiple cycles. An integrated multistep model was considered adequate for representing the hydrate crystallization kinetics and fits well with the experimental kinetic data with a low average absolute deviation in water-to-hydrate conversions among the three distinct kinetic models analyzed. Overall, the results from this study demonstrate hydrophobic porous materials as effective promoters of CH4 clathrates, which could make clathrate-based CH4 storage and transport technology industrially viable. |
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Wos |
001059413200001 |
Publication Date |
2023-08-07 |
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Edition |
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ISSN |
0016-2361 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.4 |
Times cited |
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Open Access |
Not_Open_Access: Available from 07.02.2024 |
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Notes |
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Approved |
Most recent IF: 7.4; 2023 IF: 4.601 |
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Call Number |
UA @ admin @ c:irua:197987 |
Serial |
8829 |
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Author |
Ndayirinde, C.; Gorbanev, Y.; Ciocarlan, R.-G.; De Meyer, R.; Smets, A.; Vlasov, E.; Bals, S.; Cool, P.; Bogaerts, A. |
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Title |
Plasma-catalytic ammonia synthesis : packed catalysts act as plasma modifiers |
Type |
A1 Journal article |
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Year |
2023 |
Publication |
Catalysis today |
Abbreviated Journal |
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Volume |
419 |
Issue |
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Pages |
114156-12 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
We studied the plasma-catalytic production of NH3 from H2 and N2 in a dielectric barrier discharge plasma reactor using five different Co-based catalysts supported on Al2O3, namely Co/Al2O3, CoCe/Al2O3, CoLa/Al2O3, CoCeLa/Al2O3 and CoCeMg/Al2O3. The catalysts were characterized via several techniques, including SEM-EDX, and their performance was compared. The best performing catalyst was found to be CoLa/Al2O3, but the dif-ferences in NH3 concentration, energy consumption and production rate between the different catalysts were limited under the same conditions (i.e. feed gas, flow rate and ratio, and applied power). At the same time, the plasma properties, such as the plasma power and current profile, varied significantly depending on the catalyst. Taken together, these findings suggest that in the production of NH3 by plasma catalysis, our catalysts act as plasma modifiers, i.e., they change the discharge properties and hence the gas phase plasma chemistry. Importantly, this effect dominates over the direct catalytic effect (as e.g. in thermal catalysis) defined by the chemistry on the catalyst surface. |
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Wos |
000987221300001 |
Publication Date |
2023-04-10 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0920-5861 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
5.3 |
Times cited |
3 |
Open Access |
OpenAccess |
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Notes |
This research was supported by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project) and the Methusalem project of the University of Antwerp. We also gratefully acknowledge the NH3-TPD analysis performed by Sander Bossier. |
Approved |
Most recent IF: 5.3; 2023 IF: 4.636 |
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Call Number |
UA @ admin @ c:irua:197268 |
Serial |
8917 |
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Permanent link to this record |