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- ItemMicrowave plasma discharges for biomass pretreatment: Degradation of a sodium carboxymethyl cellulose model(New York, NY : American Inst. of Physics, 2020) Honnorat, B.; Brüser, V.; Kolb, J.F.Biogas production is an important component of an environmentally benign renewable energy strategy. However, the cost-effectiveness of biogas production from biomass is limited by the presence of polymeric structures, which are recalcitrant to digestion by bacteria. Therefore, pretreatments must often be applied prior to anaerobic fermentation to increase yields of biogas. Many physico-chemical pretreatments have a high energy demand and are generally costly. An alternative could be the ignition of a plasma directly in the biomass substrate. The reactive species that are generated by plasma-liquid interactions, such as hydroxyl radicals and hydrogen peroxides, could contribute significantly to the disintegration of cell walls and the breakage of poorly digestible polymers. With respect to economic, processing, and other potential benefits, a microwave instigated and sustained plasma was investigated. A microwave circuit transmitted 2-kW pulses into a recirculated sodium carboxymethyl cellulose solution, which mimicked the rheological properties of biomass. Each microwave pulse had a duration of 12.5 ms and caused the ignition of a discharge after a vapor bubble had formed. Microwaves were absorbed in the process with an efficiency of ∼97%. Slow-motion imaging showed the development of the discharge. The plasma discharges provoked a decrease in the viscosity, probably caused by the shortening of polymer chains of the cellulose derivative. The decrease in viscosity by itself could reduce processing costs and promotes bacterial activity in actual biomass. The results demonstrate the potential of microwave in-liquid plasma discharges for the pretreatment of biomass. © 2020 Author(s).
- ItemHigh-Resolution Inkjet Printing of Quantum Dot Light-Emitting Microdiode Arrays(Weinheim : Wiley-VCH Verlag, 2020) Yang, P.; Zhang, L.; Kang, D.J.; Strahl, R.; Kraus, T.The direct printing of microscale quantum dot light-emitting diodes (QLEDs) is a cost-effective alternative to the placement of pre-formed LEDs. The quality of printed QLEDs currently is limited by nonuniformities in droplet formation, wetting, and drying during inkjet printing. Here, optimal ink formulation which can suppress nonuniformities at the pixel and array levels is demonstrated. A solvent mixture is used to tune the ejected droplet size, ensure wetting, and provoke Marangoni flows that prevent coffee stain rings. Arrays of green QLED devices are printed at a resolution of 500 pixels in.−1 with a maximum luminance of ≈3000 cd m−2 and a peak current efficiency of 2.8 cd A−1. The resulting array quality is sufficient to print displays at state-of-the-art resolutions.
- ItemTaking some heat off the NDCs? The limited potential of additional short-lived climate forcers’ mitigation(Dordrecht [u.a.] : Springer Science + Business Media B.V, 2019) Harmsen, Mathijs; Fricko, Oliver; Hilaire, Jérôme; van Vuuren, Detlef P.; Drouet, Laurent; Durand-Lasserve, Olivier; Fujimori, Shinichiro; Keramidas, Kimon; Klimont, Zbigniew; Luderer, Gunnar; Aleluia Reis, Lara; Riahi, Keywan; Sano, Fuminori; Smith, Steven J.Several studies have shown that the greenhouse gas reduction resulting from the current nationally determined contributions (NDCs) will not be enough to meet the overall targets of the Paris Climate Agreement. It has been suggested that more ambition mitigations of short-lived climate forcer (SLCF) emissions could potentially be a way to reduce the risk of overshooting the 1.5 or 2 °C target in a cost-effective way. In this study, we employ eight state-of-the-art integrated assessment models (IAMs) to examine the global temperature effects of ambitious reductions of methane, black and organic carbon, and hydrofluorocarbon emissions. The SLCFs measures considered are found to add significantly to the effect of the NDCs on short-term global mean temperature (GMT) (in the year 2040: − 0.03 to − 0.15 °C) and on reducing the short-term rate-of-change (by − 2 to 15%), but only a small effect on reducing the maximum temperature change before 2100. This, because later in the century under assumed ambitious climate policy, SLCF mitigation is maximized, either directly or indirectly due to changes in the energy system. All three SLCF groups can contribute to achieving GMT changes. © 2019, The Author(s).
- ItemGeneral and selective synthesis of primary amines using Ni-based homogeneous catalysts(Cambridge : RSC, 2020) Murugesan, Kathiravan; Wei, Zhihong; Chandrashekhar, Vishwas G.; Jiao, Haijun; Beller, Matthias; Jagadeesh, Rajenahally V.The development of base metal catalysts for industrially relevant amination and hydrogenation reactions by applying abundant and atom economical reagents continues to be important for the cost-effective and sustainable synthesis of amines which represent highly essential chemicals. In particular, the synthesis of primary amines is of central importance because these compounds serve as key precursors and central intermediates to produce value-added fine and bulk chemicals as well as pharmaceuticals, agrochemicals and materials. Here we report a Ni-triphos complex as the first Ni-based homogeneous catalyst for both reductive amination of carbonyl compounds with ammonia and hydrogenation of nitroarenes to prepare all kinds of primary amines. Remarkably, this Ni-complex enabled the synthesis of functionalized and structurally diverse benzylic, heterocyclic and aliphatic linear and branched primary amines as well as aromatic primary amines starting from inexpensive and easily accessible carbonyl compounds (aldehydes and ketones) and nitroarenes using ammonia and molecular hydrogen. This Ni-catalyzed reductive amination methodology has been applied for the amination of more complex pharmaceuticals and steroid derivatives. Detailed DFT computations have been performed for the Ni-triphos based reductive amination reaction, and they revealed that the overall reaction has an inner-sphere mechanism with H2metathesis as the rate-determining step. © The Royal Society of Chemistry 2020.
- ItemThe role of methane in future climate strategies: mitigation potentials and climate impacts(Dordrecht [u.a.] : Springer Science + Business Media B.V, 2019) Harmsen, Mathijs; Mathijs, Detlef P.; Bodirsky, Benjamin Leon; Chateau, Jean; Durand-Lasserve, Olivier; Drouet, Laurent; Fricko, Oliver; Fujimori, Shinichiro; Gernaat, David E.H.J.; Hanaoka, Tatsuya; Hilaire, Jérôme; Keramidas, Kimon; Luderer, Gunnar; Moura, Maria Cecilia P.; Sano, Fuminori; Smith, Steven J.; Wada, KenichiThis study examines model-specific assumptions and projections of methane (CH4) emissions in deep mitigation scenarios generated by integrated assessment models (IAMs). For this, scenarios of nine models are compared in terms of sectoral and regional CH4 emission reduction strategies, as well as resulting climate impacts. The models’ projected reduction potentials are compared to sector and technology-specific reduction potentials found in literature. Significant cost-effective and non-climate policy related reductions are projected in the reference case (10–36% compared to a “frozen emission factor” scenario in 2100). Still, compared to 2010, CH4 emissions are expected to rise steadily by 9–72% (up to 412 to 654 Mt CH4/year). Ambitious CO2 reduction measures could by themselves lead to a reduction of CH4 emissions due to a reduction of fossil fuels (22–48% compared to the reference case in 2100). However, direct CH4 mitigation is crucial and more effective in bringing down CH4 (50–74% compared to the reference case). Given the limited reduction potential, agriculture CH4 emissions are projected to constitute an increasingly larger share of total anthropogenic CH4 emissions in mitigation scenarios. Enteric fermentation in ruminants is in that respect by far the largest mitigation bottleneck later in the century with a projected 40–78% of total remaining CH4 emissions in 2100 in a strong (2 °C) climate policy case. © 2019, The Author(s).
- ItemConstruction of cost-effective bimetallic nanoparticles on titanium carbides as a superb catalyst for promoting hydrolysis of ammonia borane(London : RSC Publishing, 2018) Guo, Zhangwei; Liu, Tong; Wang, Qingtao; Gao, GuanhuiBimetallic cost-effective CoNi nanoparticles (NPs) are conveniently supported on titanium carbides (MXene) by a simple one-step wet-chemical method. The synthesized CoNi/MXene catalysts are characterized by XPS, TEM, STEM-HAADF and ICP-AES. The as-prepared CoNi NPs with a size of 2.8 nm are well dispersed on the MXene surface. It is found that among the CoNi bimetallic system, Co0.7Ni0.3 shows the best performance toward catalyzing ammonia borane (AB) decomposition with a turnover frequency value of 87.6 molH2 molcat−1 min−1 at 50 °C. The remarkable catalytic performance is attributed to the mild affiliation of MXene to NPs, which not only stabilizes NPs to maintain a good dispersion but also leaves sufficient surface active sites to facilitate the catalytic reaction.