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“Spontaneous Chirality Evolved at the Au–Ag Interface in Plasmonic Nanorods”. Sa J, Hu N, Heyvaert W, Van Gordon K, Li H, Wang L, Bals S, Liz-Marzán LM, Ni W, Chemistry of materials (2023). http://doi.org/10.1021/acs.chemmater.3c01044
Abstract: Chiral ligands are considered a required ingredient during the synthesis of dissymmetric plasmonic metal nanocrystals. The mechanism behind the generation of chiral structures involves the formation of high Miller index chiral facets, induced by the adsorption of such chiral ligands. We found however that, chirality can also evolve spontaneously, without the involvement of any chiral ligands, during the co-deposition of Au and Ag on Au nanorods. When using a specific Au/Ag ratio, phase segregation of the two metals leads to an interface within the obtained AuAg shell, which can be exposed by removing the Ag component via oxidative etching. Although a close-to-racemic mixture of chiral Au nanorods with right and left handedness is found in solution, electron tomography analysis evidences left- and righthanded helicities, both at the Au-Ag interface and at the exposed surface of Au NRs after Ag etching. The helicity profile of the NRs indicates dominating inclination angles in a range from 30° to 60°. Single-particle optical characterization also reveals random handedness in the plasmonic response of individual nanorods. We hypothesize that, the origin of chirality is related with symmetry breaking during the co-deposition of Au and Ag, through an initial perturbation in a small region on the Au-Ag interface that eventually leads to chiral segregation throughout the nanocrystal.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 8.6
DOI: 10.1021/acs.chemmater.3c01044
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“Incommensurate Modulations and Perovskite Growth in LaxSr2–xMnO4−δAffecting Solid Oxide Fuel Cell Conductivity”. Vandemeulebroucke D, Batuk M, Hajizadeh A, Wastiaux M, Roussel P, Hadermann J, Chemistry of Materials (2024). http://doi.org/10.1021/acs.chemmater.3c03199
Abstract: Ruddlesden-Popper La????Sr2−????MnO4−???? materials are interesting symmetric solid oxide
fuel cell electrodes due to their good redox stability, mixed ionic and electronic conducting behavior and thermal expansion that matches well with common electrolytes. In reducing environments – as at a solid oxide fuel cell anode – the x = 0.5 member, i.e. La0.5Sr1.5MnO4−????, has a much higher total conductivity than compounds with a different La/Sr ratio, although all those compositions have the same K2NiF4-type I4/mmm structure. The origin for this conductivity difference is not yet known in literature. Now, a combination of in-situ and ex-situ 3D electron diffraction, high-resolution imaging, energy-dispersive X-ray analysis and electron energy-loss spectroscopy uncovered clear differences between x=0.25 and x=0.5 in the pristine structure, as well as in the transformations upon high-temperature reduction. In La0.5Sr1.5MnO4−????, Ruddlesden-Popper n=2 layer defects and an amorphous surface layer are present, but not in La0.25Sr1.75MnO4−????. After annealing at 700°C in 5% H2/Ar, La0.25Sr1.75MnO4−???? transforms to a tetragonal 2D incommensurately modulated structure with modulation vectors ⃗????1 = 0.2848(1) · (⃗????* +⃗????*) and ⃗????2 =0.2848(1) · (⃗????* – ⃗????*), whereas La0.5Sr1.5MnO4−???? only partially transforms to an orthorhombic 1D incommensurately modulated structure,
with ⃗???? = 0.318(2) · ⃗????*. Perovskite domains grow at the crystal edge at 700°C in 5%
H2 or vacuum, due to the higher La concentration on the surface compared to the bulk, which leads to a different thermodynamic equilibrium. Since it is known that a lower degree of oxygen vacancy ordering and a higher amount of perovskite blocks enhance oxygen mobility, those differences in defect structure and structural transformation upon reduction, might all contribute to the higher conductivity of La0.5Sr1.5MnO4−???? in solid oxide fuel cell anode conditions compared to other La/Sr ratios.
Keywords: A1 Journal Article; Electron Microscopy for Materials Science (EMAT) ;
Impact Factor: 8.6
DOI: 10.1021/acs.chemmater.3c03199
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“Mechanism of Nitrogen Fixation by Nitrogenase: The Next Stage”. Hoffman BM, Lukoyanov D, Yang Z-Y, Dean DR, Seefeldt LC, Chemical Reviews 114, 4041 (2014). http://doi.org/10.1021/cr400641x
Abstract: Ammonia is a crucial nutrient used for plant growth and as a building block in pharmaceutical and chemical industry, produced via nitrogen fixation of the ubiquitous atmospheric N2. Current industrial ammonia production relies heavily on fossil resources, but a lot of work is put into developing non-fossil based pathways. Among these is the use of nonequilibrium plasma. In this work, we investigated water vapor as H source for nitrogen fixation into NH3 by non-equilibrium plasma. The highest selectivity towards NH3 was observed with low amounts of added H2O vapor, but the highest production rate was reached at high H2O vapor.
Keywords: A1 Journal Article; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
DOI: 10.1021/cr400641x
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“DFT Study of Synergistic Catalysis of the Water-Gas-Shift Reaction on Cu-Au Bimetallic Surfaces”. Saqlain MA, Hussain A, Siddiq DM, Leenaerts O, Leitão AA, ChemCatChem 8, 1208 (2016). http://doi.org/10.1002/cctc.201501312
Abstract: The water-gas-shift reaction (WGSR) is an important industrial process that can be significantly enhanced at suitable catalyst surfaces. In this work, we investigate the catalytic behavior of metallic Cu(1 0 0) and bimetallic Cu–Au(1 0 0) surfaces. With density functional theory calculations, the variation in the Gibbs free energy (ΔG°), the activation barriers, and the rate constants for the WGSR are calculated. The variation in ΔG° for water dissociation shows that the process is spontaneous up to 520 K on the bimetallic surface and up to 229 K on the Cu(1 0 0) surface. The calculated rate constants for the process also show that the bimetallic surface is much more reactive than the Cu(1 0 0) surface. The calculated pressure–temperature phase diagram for water dissociation shows that the partial pressure of H2O required for water dissociation on the bimetallic surface is substantially lower than that on the Cu(1 0 0) surface at all the studied temperatures. Additionally, the calculations demonstrate that the kinetics of the water-gas-shift reaction is dominated by redox processes on both the surfaces.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 4.803
Times cited: 8
DOI: 10.1002/cctc.201501312
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“Pd/Lewis acid synergy in macroporous Pd@Na-ZSM-5 for enhancing selective conversion of biomass”. Liu J-W, Wu S-M, Wang L-Y, Tian G, Qin Y, Wu J-X, Zhao X-F, Zhang Y-X, Chang G-G, Wu L, Zhang Y-X, Li Z-F, Guo C-Y, Janiak C, Lenaerts S, Yang X-Y, Chemcatchem , 1 (2020). http://doi.org/10.1002/CCTC.202000868
Abstract: Pd nanometal particles encapsulated in macroporous Na-ZSM-5 with only Lewis acid sites have been successfully synthesized by a steam-thermal approach. The synergistic effect of Pd and Lewis acid sites have been investigated for significant enhancement of the catalytic selectivity towards furfural alcohol in furfural hydroconversion.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.5
Times cited: 1
DOI: 10.1002/CCTC.202000868
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“Waste-derived copper-lead electrocatalysts for CO₂, reduction”. Yang S, An H, Anastasiadou D, Xu W, Wu L, Wang H, de Ruiter J, Arnouts S, Figueiredo MC, Bals S, Altantzis T, van der Stam W, Weckhuysen BM, ChemCatChem 14, e202200754 (2022). http://doi.org/10.1002/CCTC.202200754
Abstract: It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO(2)R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non-renewable metal resources, which hampers their large-scale implementation. Here, we report the preparation of bimetallic copper-lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X-ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu-0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano-shape relationship between eCO(2)R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 4.5
Times cited: 7
DOI: 10.1002/CCTC.202200754
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“Study of hydrogen peroxide reactions on manganese oxides as a tool to decode the oxygen reduction reaction mechanism”. Ryabova AS, Bonnefont A, Zagrebin P, Poux T, Sena RP, Hadermann J, Abakumov AM, Kerangueven G, Istomin SY, Antipov EV, Tsirlina GA, Savinova ER, ChemElectroChem 3, 1667 (2016). http://doi.org/10.1002/CELC.201600236
Abstract: Hydrogen peroxide has been detected as a reaction intermediate in the electrochemical oxygen reduction reaction (ORR) on transition-metal oxides and other electrode materials. In this work, we studied the electrocatalytic and catalytic reactions of hydrogen peroxide on a set of Mn oxides, Mn2O3, MnOOH, LaMnO3, MnO2, and Mn3O4, that adopt different crystal structures to shed light on the mechanism of the ORR on these materials. We then combined experiment with kinetic modeling with the objective to correlate the differences in the ORR activity to the kinetics of the elementary reaction steps, and we uncovered the importance of structural and compositional factors in the catalytic activity of the Mn oxides. We concluded that the exceptional activity of Mn2O3 in the ORR is due to its high catalytic activity both in the reduction of oxygen to hydrogen peroxide and in the decomposition of the latter, and furthermore, we proposed a tentative link between crystal structure and reactivity.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.136
Times cited: 20
DOI: 10.1002/CELC.201600236
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“Attaching redox proteins onto electrode surfaces by bis-silane”. Trashin S, De Jong M, Meynen V, Dewilde S, De Wael K, ChemElectroChem 3, 1035 (2016). http://doi.org/10.1002/CELC.201600021
Abstract: Immobilization of redox proteins on electrode surfaces is of special interest for mechanistic studies and applications because of a well-controlled redox state of protein molecules by a polarized electrode and fast electron transfer kinetics, free from diffusion limitation. Here, bis-organosilane (1,2-bis(trimethoxysilyl)ethane) was applied as a fresh solution in a pH 7 phosphate buffer without use of any organic solvent, sol-gel or mesoporous bulk matrix. A short aging period of 30 minutes before deposition on the electrodes was optimal for the immobilization of proteins. Three redox proteins (cytochrome c, neuroglobin and GLB-12) were confined to the gold surface of electrodes with high coverages and stability, indicating that the suggested technique is simple, efficient and generic in nature.
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation)
Impact Factor: 4.136
Times cited: 4
DOI: 10.1002/CELC.201600021
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“Towards developing a screening strategy for ecstasy : revealing the electrochemical profile”. Thiruvottriyur Shanmugam S, Van Echelpoel R, Boeye G, Eliaerts J, Samanipour M, Ching HYV, Florea A, Van Doorslaer S, Van Durme F, Samyn N, Parrilla M, De Wael K, Chemelectrochem 8, 4826 (2021). http://doi.org/10.1002/CELC.202101198
Abstract: This article describes the development of an electrochemical screening strategy for 3,4-methylenedioxymethamphetamine (MDMA), the regular psychoactive compound in ecstasy (XTC) pills. We have investigated the specific electrochemical profile of MDMA and its electro-oxidation mechanisms at disposable graphite screen-printed electrodes. We have proved that the formation of a radical cation and subsequent reactions are indeed responsible for the electrode surface passivation, as evidenced by using electron paramagnetic resonance spectroscopy and electrochemistry. Thereafter, pure cutting agents and MDMA as well as simulated binary mixtures of compounds with MDMA were subjected to square wave voltammetry at pH 7 to understand the characteristic electrochemical profile. An additional measurement at pH 12 was able to resolve false positives and negatives occurring at pH 7. Finally, validation of the screening strategy was done by measuring a set of ecstasy street samples. Overall, our proposed electrochemical screening strategy has been demonstrated for the rapid, sensitive, and selective detection of MDMA, resolving most of the false positives and negatives given by the traditional Marquis color tests, thus exhibiting remarkable promises for the on-site screening of MDMA.
Keywords: A1 Journal article; AXES (Antwerp X-ray Analysis, Electrochemistry and Speciation); Organic synthesis (ORSY); Applied Electrochemistry & Catalysis (ELCAT); Antwerp Electrochemical and Analytical Sciences Lab (A-Sense Lab)
Impact Factor: 4.136
DOI: 10.1002/CELC.202101198
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“Inhibiting recombination to improve the performance of plasma-based CO2 conversion”. Wang K, Ceulemans S, Zhang H, Tsonev I, Zhang Y, Long Y, Fang M, Li X, Yan J, Bogaerts A, Chemical Engineering Journal 481, 148684 (2024). http://doi.org/10.1016/j.cej.2024.148684
Abstract: Warm plasma offers a promising route for CO2 splitting into valuable CO, yet recombination reactions of CO with oxygen, forming again CO2, have recently emerged as critical limitation. This study combines experiments and fluid dynamics + chemical kinetics modelling to comprehensively analyse the recombination reactions upon CO2 splitting in an atmospheric plasmatron. We introduce an innovative in-situ gas sampling technique, enabling 2D spatial mapping of gas product compositions and temperatures, experimentally confirming for the first time the substantial limiting effect of CO recombination reactions in the afterglow region. Our results show that the CO mole fraction at a 5 L/min flow rate drops significantly from 11.9 % at a vertical distance of z = 20 mm in the afterglow region to 8.6 % at z = 40 mm. We constructed a comprehensive 2D model that allows for spatial reaction rates analysis incorporating crucial reactions, and we validated it to kinetically elucidate this phenomenon. CO2 +M⇌O+CO+M and CO2 +O⇌CO+O2 are the dominant reactions, with the forward reactions prevailing in the plasma region and the backward reactions becoming prominent in the afterglow region. These results allow us to propose an afterglow quenching strategy for performance enhancement, which is further demonstrated through a meticulously developed plasmatron reactor with two-stage cooling. Our approach substantially increases the CO2 conversion (e.g., from 6.6 % to 19.5 % at 3 L/min flow rate) and energy efficiency (from 13.5 % to 28.5 %, again at 3 L/min) and significantly shortens the startup time (from ~ 150 s to 25 s). Our study underscores the critical role of inhibiting recombination reactions in plasma-based CO2 conversion and offers new avenues for performance enhancement.
Keywords: A1 Journal Article; Plasma-based CO2 splitting Recombination reactions In-situ gas sampling Fluid dynamics modeling Kinetics modeling Afterglow quenching; Plasma, laser ablation and surface modeling Antwerp (PLASMANT) ;
Impact Factor: 15.1
DOI: 10.1016/j.cej.2024.148684
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“Facile morphology-controlled synthesis of organolead iodide perovskite nanocrystals using binary capping agents”. Debroye E, Yuan H, Bladt E, Baekelant W, Van der Auweraer M, Hofkens J, Bals S, Roeffaers MBJ, ChemNanoMat : chemistry of nanomaterials for energy, biology and more 3, 223 (2017). http://doi.org/10.1002/CNMA.201700006
Abstract: Controlling the morphology of organolead halide perovskite crystals is crucial to a fundamental understanding of the materials and to tune their properties for device applications. Here, we report a facile solution-based method for morphology-controlled synthesis of rod-like and plate-like organolead halide perovskite nanocrystals using binary capping agents. The morphology control is likely due to an interplay between surface binding kinetics of the two capping agents at different crystal facets. By high-resolution scanning transmission electron microscopy, we show that the obtained nanocrystals are monocrystalline. Moreover, long photoluminescence decay times of the nanocrystals indicate long charge diffusion lengths and low trap/defect densities. Our results pave the way for large-scale solution synthesis of organolead halide perovskite nanocrystals with controlled morphology for future device applications.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 2.937
Times cited: 19
DOI: 10.1002/CNMA.201700006
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“Tunable nitrogen-doped carbon nanoparticles from tannic acid and urea and their potential for sustainable soots”. Berthold T, Castro CR, Winter M, Hoerpel G, Kurttepeli M, Bals S, Antonietti M, Fechler N, ChemNanoMat : chemistry of nanomaterials for energy, biology and more 3, 311 (2017). http://doi.org/10.1002/CNMA.201700051
Abstract: Nano-sized nitrogen-doped carbon spheres are synthesized from two cheap, readily available and sustainable precursors: tannic acid and urea. In combination with a polymer structuring agent, nitrogen content, sphere size and the surface (up to 400 m(2)g(-1)) can be conveniently tuned by the precursor ratio, temperature and structuring agent content. Because the chosen precursors allow simple oven synthesis and avoid harsh conditions, this carbon nanosphere platform offers a more sustainable alternative to classical soots, for example, as printing pigments or conduction soots. The carbon spheres are demonstrated to be a promising as conductive carbon additive in anode materials for lithium ion batteries.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 2.937
Times cited: 14
DOI: 10.1002/CNMA.201700051
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“Catalytic Nox reduction with simultaneous dioxin and furan oxidation”. Goemans M, Clarysse P, Joannès J, de Clercq P, Lenaerts S, Matthys K, Boels K, Chemosphere 54, 1357 (2004). http://doi.org/10.1016/S0045-6535(03)00255-8
Abstract: The engineering, construction, performance and running costs of a catalytic flue gas cleaning component in the low dust area of a municipal waste incinerator is discussed. For this purpose, the case study of a Flemish incineration plant is presented, covering the history, the design procedure of the catalyst, relevant process data and the financial aspects. A reliable PCDD/F-destruction by means of oxidation by the catalyst to typical values of 0.001 ng TEQ/Nm3 has been demonstrated. At the same time, NOx− and CO-emissions are reduced by 90% and 20% to about 50 mg/Nm3 and below 10 mg/Nm3, respectively.
Keywords: A1 Journal article
Impact Factor: 4.208
DOI: 10.1016/S0045-6535(03)00255-8
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“Catalytic Nox reduction with simultaneous dioxin and furan oxidation”. Goemans M, Clarysse P, Joannès J, de Clercq P, Lenaerts S, Matthys K, Boels K, Chemosphere 50, 489 (2003). http://doi.org/10.1016/S0045-6535(02)00554-4
Abstract: The engineering, construction, performance and running costs of a catalytic flue gas cleaning component in the low dust area of a municipal waste incinerator is discussed. For this purpose, the case study of a Flemish incineration plant is presented, covering the history, the design procedure of the catalyst, relevant process data and the financial aspects. A reliable PCDD/F-destruction by means of oxidation by the catalyst to typical values of 0.001 ng TEQ/N m3 has been demonstrated. At the same time, NOx- and CO-emissions are reduced by 90% and 20% to about 50 mg/N m3 and below 10 mg/N m3, respectively.
Keywords: A1 Journal article
Impact Factor: 4.208
DOI: 10.1016/S0045-6535(02)00554-4
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“Two-stage anaerobic membrane bioreactor for co-treatment of food waste and kitchen wastewater for biogas production and nutrients recovery”. Le T-S, Nguyen P-D, Ngo HH, Bui X-T, Dang B-T, Diels L, Bui H-H, Nguyen M-T, Le Quang D-T, Chemosphere 309, 136537 (2022). http://doi.org/10.1016/J.CHEMOSPHERE.2022.136537
Abstract: Co-digestion of organic waste and wastewater is receiving increased attention as a plausible waste management approach toward energy recovery. However, traditional anaerobic processes for co-digestion are particularly susceptible to severe organic loading rates (OLRs) under long-term treatment. To enhance technological feasi-bility, this work presented a two-stage Anaerobic Membrane Bioreactor (2 S-AnMBR) composed of a hydrolysis reactor (HR) followed by an anaerobic membrane bioreactor (AnMBR) for long-term co-digestion of food waste and kitchen wastewater. The OLRs were expanded from 4.5, 5.6, and 6.9 kg COD m- 3 d-1 to optimize biogas yield, nitrogen recovery, and membrane fouling at ambient temperatures of 25-32 degrees C. Results showed that specific methane production of UASB was 249 +/- 7 L CH4 kg-1 CODremoved at the OLR of 6.9 kg TCOD m- 3 d-1. Total Chemical Oxygen Demand (TCOD) loss by hydrolysis was 21.6% of the input TCOD load at the hydraulic retention time (HRT) of 2 days. However, low total volatile fatty acid concentrations were found in the AnMBR, indicating that a sufficiently high hydrolysis efficiency could be accomplished with a short HRT. Furthermore, using AnMBR structure consisting of an Upflow Anaerobic Sludge Blanket Reactor (UASB) followed by a side -stream ultrafiltration membrane alleviated cake membrane fouling. The wasted digestate from the AnMBR comprised 42-47% Total Kjeldahl Nitrogen (TKN) and 57-68% total phosphorous loading, making it suitable for use in soil amendments or fertilizers. Finally, the predominance of fine particles (D10 = 0.8 mu m) in the ultra -filtration membrane housing (UFMH) could lead to a faster increase in trans-membrane pressure during the filtration process.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 8.8
DOI: 10.1016/J.CHEMOSPHERE.2022.136537
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“ZnO nanorod arrays by plasma-enhanced CVD for light-activated functional applications”. Bekermann D, Gasparotto A, Barreca D, Devi A, Fischer RA, Kete M, Štangar UL, Lebedev OI, Maccato C, Tondello E, Van Tendeloo G, ChemPhysChem : a European journal of chemical physics and physical chemistry 11, 2337 (2010). http://doi.org/10.1002/cphc.201000333
Abstract: Switch of the surface properties: Supported ZnO nanorod arrays with tailored roughness and aspect ratios are successfully synthesized by plasma-enhanced chemical vapor deposition. Such nanostructures exhibit significant superhydrophilic and photocatalytic properties tunable as a function of their morphological organization (see picture). This renders them promising building blocks for the fabrication of stimuli-responsive materials.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.075
Times cited: 38
DOI: 10.1002/cphc.201000333
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“Quantum-Transport Characteristics of a p-n Junction on Single-Layer TiS3”. Iyikanat F, Senger RT, Peeters FM, Sahin H, ChemPhysChem : a European journal of chemical physics and physical chemistry 17, 3985 (2016). http://doi.org/10.1002/CPHC.201600751
Abstract: By using density functional theory and non-equilibrium Green's function-based methods, we investigated the electronic and transport properties of a TiS3 monolayer p-n junction. We constructed a lateral p-n junction on a TiS3 monolayer using Li and F adatoms. An applied bias voltage caused significant variability in the electronic and transport properties of the TiS3 p-n junction. In addition, the spin-dependent current-volt-age characteristics of the constructed TiS3 p-n junction were analyzed. Important device characteristics were found, such as negative differential resistance and rectifying diode behaviors for spin-polarized currents in the TiS3 p-n junction. These prominent conduction properties of the TiS3 p-n junction offer remarkable opportunities for the design of nanoelectronic devices based on a recently synthesized single-layered material.
Keywords: A1 Journal article; Condensed Matter Theory (CMT)
Impact Factor: 3.075
Times cited: 12
DOI: 10.1002/CPHC.201600751
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“Photocatalytic removal of soot : unravelling of the reaction mechanism by EPR and in situ FTIR spectroscopy”. Smits M, Ling Y, Lenaerts S, Van Doorslaer S, ChemPhysChem : a European journal of chemical physics and physical chemistry 13, 4251 (2012). http://doi.org/10.1002/CPHC.201200674
Abstract: Photocatalytic soot oxidation is studied on P25 TiO2 as an important model reaction for self-cleaning processes by means of electron paramagnetic resonance (EPR) and Fourier transform infrared (FTIR) spectroscopy. Contacting of carbon black with P25 leads on the one hand to a reduction of the local dioxygen concentration in the powder. On the other hand, the weakly adsorbed radicals on the carbon particles are likely to act as alternative traps for the photogenerated conduction-band electrons. We find furthermore that the presence of dioxygen and oxygen-related radicals is vital for the photocatalytic soot degradation. The complete oxidation of soot to CO2 is evidenced by in situ FTIR spectroscopy, no intermediate CO is detected during the photocatalytic process.
Keywords: A1 Journal article; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3.075
Times cited: 9
DOI: 10.1002/CPHC.201200674
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“Fluorescent nanodiamonds with bioorthogonally reactive protein-resistant polymeric coatings”. Rehor I, Mackova H, Filippov SK, Kucka J, Proks V, Slegerova J, Turner S, Van Tendeloo G, Ledvina M, Hruby M, Cigler P;, ChemPlusChem 79, 21 (2014). http://doi.org/10.1002/cplu.201300339
Abstract: The novel synthesis of a polymeric interface grown from the surface of bright fluorescent nanodiamonds is reported. The polymer enables bioorthogonal attachment of various molecules by click chemistry; the particles are resistant to nonspecific protein adsorption and show outstanding colloidal stability in buffers and biological media. The coating fully preserves the unique optical properties of the nitrogen-vacancy centers that are crucial for bioimaging and sensoric applications.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 2.797
Times cited: 34
DOI: 10.1002/cplu.201300339
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“Design of Ru-zeolites for hydrogen-free production of conjugated linoleic acid”. Philippaerts A, Goossens S, Vermandel W, Tromp M, Turner S, Geboers J, Van Tendeloo G, Jacobs PA, Sels BF, Chemsuschem 4, 757 (2011). http://doi.org/10.1002/cssc.201100015
Abstract: While conjugated vegetable oils are currently used as additives in the drying agents of oils and paints, they are also attractive molecules for making bio-plastics. Moreover, conjugated oils will soon be accepted as nutritional additives for functional food products. While current manufacture of conjugated vegetable oils or conjugated linoleic acids (CLAs) uses a homogeneous base as isomerisation catalyst, a heterogeneous alternative is not available today. This contribution presents the direct production of CLAs over Ru supported on different zeolites, varying in topology (ZSM-5, BETA, Y), Si/Al ratio and countercation (H+, Na+, Cs+). Ru/Cs-USY, with a Si/Al ratio of 40, was identified as the most active and selective catalyst for isomerisation of methyl linoleate (cis-9,cis-12 (C18:2)) to CLA at 165 °C. Interestingly, no hydrogen pre-treatment of the catalyst or addition of hydrogen donors is required to achieve industrially relevant isomerisation productivities, namely, 0.7 g of CLA per litre of solvent per minute. Moreover, the biologically most active CLA isomers, namely, cis-9,trans-11, trans-10,cis-12 and trans-9,trans-11, were the main products, especially at low catalyst concentrations. Ex situ physicochemical characterisation with CO chemisorption, extended X-ray absorption fine structure measurements, transmission electron microscopy analysis, and temperature-programmed oxidation reveals the presence of highly dispersed RuO2 species in Ru/Cs-USY(40).
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 24
DOI: 10.1002/cssc.201100015
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“Selective bifunctional catalytic conversion of cellulose over reshaped ni particles at the tip of carbon nanofibers”. Van de Vyver S, Geboers J, Dusselier M, Schepers H, Vosch T, Zhang L, Van Tendeloo G, Jacobs PA, Sels BF, Chemsuschem 3, 698 (2010). http://doi.org/10.1002/cssc.201000087
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 136
DOI: 10.1002/cssc.201000087
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“Selective nickel-catalyzed conversion of model and lignin-derived phenolic compounds to cyclohexanone-based polymer building blocks”. Schutyser W, Van den Bosch S, Dijkmans J, Turner S, Meledina M, Van Tendeloo G, Debecker DP, Sels BF, Chemsuschem 8, 1805 (2015). http://doi.org/10.1002/cssc.201403375
Abstract: Valorization of lignin is essential for the economics of future lignocellulosic biorefineries. Lignin is converted into novel polymer building blocks through four steps: catalytic hydroprocessing of softwood to form 4-alkylguaiacols, their conversion into 4-alkylcyclohexanols, followed by dehydrogenation to form cyclohexanones, and Baeyer-Villiger oxidation to give caprolactones. The formation of alkylated cyclohexanols is one of the most difficult steps in the series. A liquid-phase process in the presence of nickel on CeO2 or ZrO2 catalysts is demonstrated herein to give the highest cyclohexanol yields. The catalytic reaction with 4-alkylguaiacols follows two parallel pathways with comparable rates: 1) ring hydrogenation with the formation of the corresponding alkylated 2-methoxycyclohexanol, and 2) demethoxylation to form 4-alkylphenol. Although subsequent phenol to cyclohexanol conversion is fast, the rate is limited for the removal of the methoxy group from 2-methoxycyclohexanol. Overall, this last reaction is the rate-limiting step and requires a sufficient temperature (> 250 degrees C) to overcome the energy barrier. Substrate reactivity (with respect to the type of alkyl chain) and details of the catalyst properties (nickel loading and nickel particle size) on the reaction rates are reported in detail for the Ni/CeO2 catalyst. The best Ni/CeO2 catalyst reaches 4-alkylcyclohexanol yields over 80 %, is even able to convert real softwood-derived guaiacol mixtures and can be reused in subsequent experiments. A proof of principle of the projected cascade conversion of lignocellulose feedstock entirely into caprolactone is demonstrated by using Cu/ZrO2 for the dehydrogenation step to produce the resultant cyclohexanones (approximate to 80%) and tin-containing beta zeolite to form 4-alkyl-e-caprolactones in high yields, according to a Baeyer-Villiger-type oxidation with H2O2.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 7.226
Times cited: 71
DOI: 10.1002/cssc.201403375
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“The Chemical Route to a Carbon Dioxide Neutral World”. Martens JA, Bogaerts A, De Kimpe N, Jacobs PA, Marin GB, Rabaey K, Saeys M, Verhelst S, Chemsuschem 10, 1039 (2017). http://doi.org/10.1002/cssc.201601051
Abstract: Excessive CO2 emissions in the atmosphere from anthropogenic activity can be divided into point sources and diffuse sources. The capture of CO2 from flue gases of large industrial installations and its conversion into fuels and chemicals with fast catalytic processes seems technically possible. Some emerging technologies are already being demonstrated on an industrial scale. Others are still being tested on a laboratory or pilot scale. These emerging chemical technologies can be implemented in a time window ranging from 5 to 20 years. The massive amounts of energy needed for capturing processes and the conversion of CO2 should come from low-carbon energy sources, such as tidal, geothermal, and nuclear energy, but also, mainly, from the sun. Synthetic methane gas that can be formed from CO2 and hydrogen gas is an attractive renewable energy carrier with an existing distribution system. Methanol offers advantages as a liquid fuel and is also a building block for the chemical industry. CO2 emissions from diffuse sources is a difficult problem to solve, particularly for CO2 emissions from road, water, and air transport, but steady progress in the development of technology for capturing CO2 from air is being made. It is impossible to ban carbon from the entire energy
supply of mankind with the current technological knowledge, but a transition to a mixed carbon–hydrogen economy can reduce net CO2 emissions and ultimately lead to a CO2-neutral world.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 75
DOI: 10.1002/cssc.201601051
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“Gliding Arc Plasmatron: Providing an Alternative Method for Carbon Dioxide Conversion”. Ramakers M, Trenchev G, Heijkers S, Wang W, Bogaerts A, Chemsuschem 10, 2642 (2017). http://doi.org/10.1002/cssc.201700589
Abstract: Low-temperature plasmas are gaining a lot of interest for environmental and energy applications. A large research field in these applications is the conversion of CO2 into chemicals and fuels. Since CO2 is a very stable molecule, a key performance indicator for the research on plasma-based CO2 conversion is the energy efficiency. Until now, the energy efficiency in atmospheric plasma reactors is quite low, and therefore we employ here a novel type of plasma reactor, the gliding arc plasmatron (GAP). This paper provides a detailed experimental and computational study of the CO2 conversion, as well as the energy cost and efficiency in a GAP. A comparison with thermal conversion, other plasma types and other novel CO2 conversion technologies is made to find out whether this novel plasma reactor can provide a significant contribution to the much-needed efficient conversion of CO2. From these comparisons it becomes evident that our results are less than a factor of two away from being cost competitive and already outperform several other new technologies. Furthermore, we indicate how the performance of the GAP can still be improved by further exploiting its non-equilibrium character. Hence, it is clear that the GAP is very promising for CO2 conversion.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 42
DOI: 10.1002/cssc.201700589
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“Dry Reforming of Methane in a Gliding Arc Plasmatron: Towards a Better Understanding of the Plasma Chemistry”. Cleiren E, Heijkers S, Ramakers M, Bogaerts A, Chemsuschem 10, 4025 (2017). http://doi.org/10.1002/cssc.201701274
Abstract: Dry reforming of methane (DRM) in a gliding arc plasmatron is studied for different CH4 fractions in the mixture. The CO2 and CH4 conversions reach their highest values of approximately 18 and 10%, respectively, at 25% CH4 in the gas mixture, corresponding to an overall energy cost of 10 kJ L@1 (or 2.5 eV per molecule) and an energy efficiency of 66%. CO and H2 are the major products, with the formation of smaller fractions of C2Hx (x=2, 4, or 6) compounds and H2O. A chemical kinetics model is used to investigate the underlying chemical processes. The calculated CO2 and CH4 conversion and the energy efficiency are in good agreement with the experimental data. The model calculations reveal that the reaction of CO2 (mainly at vibrationally excited levels) with H radicals is mainly responsible for
the CO2 conversion, especially at higher CH4 fractions in the mixture, which explains why the CO2 conversion increases with increasing CH4 fraction. The main process responsible for CH4 conversion is the reaction with OH radicals. The excellent energy efficiency can be explained by the non-equilibrium character of the plasma, in which the electrons mainly activate the gas molecules, and by the important role of the vibrational kinetics of CO2. The results demonstrate that a gliding arc plasmatron is very promising for DRM.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 7.226
Times cited: 23
DOI: 10.1002/cssc.201701274
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“Harvesting hydrogen gas from air pollutants with an un-biased gas phase photo-electrochemical cell”. Verbruggen SW, Van Hal M, Bosserez T, Rongé, J, Hauchecorne B, Martens JA, Lenaerts S, Chemsuschem 10, 1413 (2017). http://doi.org/10.1002/CSSC.201601806
Abstract: The concept of an all-gas-phase photo-electrochemical cell (PEC) producing hydrogen gas from volatile organic contaminated gas and light is presented. Without applying any external bias, organic contaminants are degraded and hydrogen gas is produced in separate electrode compartments. The system works most efficiently with organic pollutants in inert carrier gas. In the presence of oxygen gas, the cell performs less efficiently but still significant photocurrents are generated, showing the cell can be run on organic contaminated air. The purpose of this study is to demonstrate new application opportunities of PEC technology and to encourage further advancement toward photo-electrochemical remediation of air pollution with the attractive feature of simultaneous energy recovery and pollution abatement.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 7.226
Times cited: 6
DOI: 10.1002/CSSC.201601806
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“Modeling the physicochemical properties of natural deep eutectic solvents : a review”. Kovács A, Billen P, Cornet I, Wijnants M, Neyts EC, Chemsuschem 13, 3789 (2020). http://doi.org/10.1002/CSSC.202000286
Abstract: Natural deep eutectic solvents (NADES) are mixtures of naturally derived compounds with a significantly decreased melting point due to the specific interactions among the constituents. NADES have benign properties (low volatility, flammability, toxicity, cost) and tailorable physicochemical properties (by altering the type and molar ratio of constituents), hence they are often considered as a green alternative to common organic solvents. Modeling the relation between their composition and properties is crucial though, both for understanding and predicting their behavior. Several efforts were done to this end, yet this review aims at structuring the present knowledge as an outline for future research. First, we reviewed the key properties of NADES and relate them to their structure based on the available experimental data. Second, we reviewed available modeling methods applicable to NADES. At the molecular level, density functional theory and molecular dynamics allow interpreting density differences and vibrational spectra, and computation of interaction energies. Additionally, properties at the level of the bulk media can be explained and predicted by semi-empirical methods based on ab initio methods (COSMO-RS) and equation of state models (PC-SAFT). Finally, methods based on large datasets are discussed; models based on group contribution methods and machine learning. A combination of bulk media and dataset modeling allows qualitative prediction and interpretation of phase equilibria properties on the one hand, and quantitative prediction of melting point, density, viscosity, surface tension and refractive indices on the other hand. In our view, multiscale modeling, combining the molecular and macroscale methods, will strongly enhance the predictability of NADES properties and their interaction with solutes, yielding truly tailorable solvents to accommodate (bio)chemical reactions.
Keywords: A1 Journal article; Engineering sciences. Technology; Intelligence in PRocesses, Advanced Catalysts and Solvents (iPRACS); Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT); Biochemical Wastewater Valorization & Engineering (BioWaVE)
Impact Factor: 8.4
DOI: 10.1002/CSSC.202000286
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“A techno-economic assessment of an algal-based biorefinery”. Thomassen G, Egiguren Vila U, Van Dael M, Lemmens B, Van Passel S, Clean Technologies And Environmental Policy 18, 1849 (2016). http://doi.org/10.1007/S10098-016-1159-2
Abstract: Economic and technological assessments have identified difficulties with the commercialization of bulk products from microalgae, like biofuels. To overcome these problems, a multi-product algal-based biorefinery has been proposed. This paper performs a techno-economic assessment of such a biorefinery. Four production pathways, ranging from a base case with commercial technologies to an improved case with innovative technologies, are analyzed. All region-specific parameters were adapted to Belgian conditions. Three scenarios result in techno-economically viable production plants. The most profitable scenario is the scenario which uses a specialized membrane for medium recycling and an open pond algae cultivation. Although the inclusion of a photobioreactor decreases the culture medium costs, the higher investment costs result in lower economic profits. The carotenoid content and price are identified as critical parameters. Furthermore, the economies of scale assumption for the photobioreactor is critical for the feasibility of this cultivation technology. The techno-economic assessment is an important methodology to guide and evaluate further improvements in research and shorten the time-to-market for innovative technologies in this field.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 3.331
Times cited: 24
DOI: 10.1007/S10098-016-1159-2
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“Cost-efficient emission abatement of energy and transportation technologies : mitigation costs and policy impacts for Belgium”. De Schepper E, Van Passel S, Lizin S, Achten WMJ, Van Acker K, Clean Technologies And Environmental Policy 16, 1107 (2014). http://doi.org/10.1007/S10098-014-0713-Z
Abstract: In the light of global warming, this paper develops a framework to compare energy and transportation technologies in terms of cost-efficient GHG emission reduction. We conduct a simultaneous assessment of economic and environmental performances through life cycle costing and life cycle assessment. To calculate the GHG mitigation cost, we create reference systems within the base scenario. Further, we extend the concept of the mitigation cost, allowing (i) comparision of technologies given a limited investment resource, and (ii) evaluation of the direct impact of policy measures by means of the subsidized mitigation cost. The framework is illustrated with a case of solar photovoltaics (PV), grid powered battery electric vehicles (BEVs), and solar powered BEVs for a Belgian small and medium sized enterprise. The study's conclusions are that the mitigation cost of solar PV is high, even though this is a mature technology. The emerging mass produced BEVs on the other hand are found to have a large potential for cost-efficient GHG mitigation as indicated by their low cost of mitigation. Finally, based on the subsidized mitigation cost, we conclude that the current financial stimuli for all three investigated technologies are excessive when compared to the CO2 market value under the EU Emission Trading Scheme.
Keywords: A1 Journal article; Economics; Engineering sciences. Technology; Engineering Management (ENM)
Impact Factor: 3.331
Times cited: 14
DOI: 10.1007/S10098-014-0713-Z
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“On the (ir)relevance of heatwaves in climate change impacts on European agriculture”. Fabri C, Moretti M, Van Passel S, Climatic Change 174, 16 (2022). http://doi.org/10.1007/S10584-022-03438-4
Abstract: The Ricardian model is a widely used approach based on cross-sectional regression analysis to estimate climate change impacts on agricultural productivity. Up until now, researchers have focused on the impacts of gradual changes in temperature and precipitation, even though climate change is known to encompass also changes in the severity and frequency of extreme weather events. This research investigates the impact of heatwaves on European agriculture, additional to the impact of average climate change. Using a dataset of more than 60,000 European farms, the study examines whether adding a measure for heatwaves to the Ricardian model influences its results. We find that heatwaves have a minor impact on agricultural productivity and that this impact is moderated by average temperature. In colder regions, farm productivity increases with the number of heatwave days. For warmer regions, land values decrease with heatwave frequency. Despite the moderating effect, the marginal effect of heatwave frequency, i.e. the percentage change in agricultural land values caused by one more heatwave day per year, is small in comparison to the effect of average temperature increases. Non-marginal effects are found to be relevant, but only in the case of increased heatwave frequency. According to our results, farms are not expected to suffer more from extreme weather than from mean climate change, as was claimed by several previous studies.
Keywords: A1 Journal article; Engineering Management (ENM)
Impact Factor: 4.8
DOI: 10.1007/S10584-022-03438-4
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