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Register a new userElectrolytic Conversion of Bicarbonate into CO in a Flow Cell
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Electrochemical CO2 reduction offers a method to use renewable electricity to convert CO2 into CO and other carbon-based chemical building blocks. While nearly all studies rely on a CO2 feed, we show herein that aqueous bicarbonate solutions can also be electrochemically converted into CO gas at meaningful rates in a flow cell. We achieved this result in a flow cell containing a bipolar membrane (BPM) and a silver nanoparticle catalyst on a porous carbon support. Electrolysis upon a N2-saturated 3.0-M potassium bicarbonate electrolyte solution yields CO with a faradaic efficiency (F.E.CO) of 81% at 25 mA cm-2 and 37% at 100 mA cm-2. This output is comparable to the analogous experiment where the electrolyte is saturated with gaseous CO2 (faradaic efficiency for CO is 78% at 25 mA cm-2 and 35% at 100 mA cm-2). The H+ flux from the BPM is critical to this chemistry in that it reacts with the bicarbonate feed to generate CO2, which is then reduced to CO at the gas diffusion electrode. These results are important in that they show that the addition of gaseous CO2 to bicarbonate electrolytes is not necessary in order to obtain reduced carbon products with a flow cell architecture. This process offers a means of using electrolysis to bypass the thermally-intensive step of extracting CO2 from bicarbonate solutions generated in carbon capture schemes.
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Organic molecular hole-transport materials (HTMs) are appealing for the scalable manufacture of perovskite solar cells (PSCs) because they are easier to reproducibly prepare in high purity than polymeric and inorganic HTMs. There is also a need to construct PSCs without dopants and additives to avoid formidable engineering and stability issues. We report here a power conversion efficiency (PCE) of 20.6% with a molecular HTM in an inverted (p-i-n) PSC without any dopants or interlayers. This new benchmark was made possible by the discovery that annealing a spiro-based dopant-free HTM (denoted DFH) containing redox-active triphenyl amine (TPA) units undergoes preferential molecular organization normal to the substrate. This structural order, governed by the strong intermolecular interactions of the DFH dioxane groups, affords high intrinsic hole mobility (1x10-3 cm2 V-1 s-1). Annealing films of DFH also enables the growth of large perovskite grains (up to 2 um) that minimize charge recombination in the PSC. DFH can also be isolated at a fraction of the cost of any other organic HTM.
Following some recent unexpected hints of neutron production in setups like high-voltage atmospheric discharges and plasma discharges in electrolytic cells, we present a measurement of the neutron flux in a configuration similar to the latter. We use two different types of neutron detectors, poly-allyl-diglicol-carbonate (PADC, aka CR-39) tracers and Indium disks. At 95% C.L. we provide an upper limit of 1.5 neutrons cm^-2 s^-1 for the thermal neutron flux at ~5 cm from the center of the cell. Allowing for a higher energy neutron component the largest allowed flux is 64 neutrons cm^-2 s^-1. This upper limit is two orders of magnitude smaller than what previously claimed in an electrolytic cell plasma discharge experiment. Furthermore the behavior of the CR-39 is discussed to point our possible sources of spurious signals.
Generator-collector experiments offer insights into the mechanisms of electrochemical reactions by correlating the product and generator currents. Most commonly, these experiments are performed using a rotating ring-disk electrode (RRDE). We developed a double electrode flow cell (DEFC) with exchangeable generator and detector electrodes where the electrode width equals the channel width. Commonalities and differences between the RRDE and DEFC are discussed based on analytical solutions, numerical simulations and measurements of the ferri-/ferrocyanide redox couple on Pt electrodes in a potassium chloride electrolyte. The analytical solutions agree with the measurements using electrode widths of 5 and 2 mm. Yet, we find an unexpected dependence on the exponent of the width so that wider electrodes cannot be analysed using the conventional analytical solution. In contrast, all the investigated electrodes show a collection efficiency of close to 35.4% above a minimum rotation speed or flow rate, where the narrowest electrode is most accurate at the cost of precision and the widest electrode the least accurate but most precise. Our DEFC with exchangeable electrodes is an attractive alternative to commercial RRDEs due to the flexibility to optimize the electrode materials and geometry for the desired reaction.
Our recent paper on the Search for Neutron Flux Generation in a Plasma Discharge Electrolytic Cell [1] has as main goal the validation of the experiment in Ref.[2]. As a follow-up, Ref.[3] moves a set of objections on our procedure and presents argumentations on why the experiments should not yield the same results. We collect here additional material and calculations that contribute to understanding the observed discrepancies. Furthermore we prove that the absence of signals from Indium activation detectors reported also for the experiment of Ref.[2] is a clear indication that neutron production does not occur. [1] R.Faccini et al arXiv:1310.4749 [2] D.Cirillo et al, Key Engineering Materials 495, 104 (2012). [3] A.Widom et al. arXiv:1311.2447
A one dimensional (1-D), isothermal model for a direct methanol fuel cell (DMFC) is presented. This model accounts for the kinetics of the multi-step methanol oxidation reaction at the anode. Diffusion and crossover of methanol are modeled and the mixed potential of the oxygen cathode due to methanol crossover is included. Kinetic and diffusional parameters are estimated by comparing the model to data from a 25 cm2 DMFC. This semi-analytical model can be solved rapidly so that it is suitable for inclusion in real-time system level DMFC simulations.
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