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Full-Text Articles in Chemical Engineering
Using Sputter Deposition To Increase Co Tolerance In A Proton-Exchange Membrane Fuel Cell, Andrew T. Haug, Ralph E. White, John W. Weidner, Wayne Huang, Steven Shi, Narender Rana, Stephan Grunow, Timothy C. Stoner, Alain E. Kaloyeros
Using Sputter Deposition To Increase Co Tolerance In A Proton-Exchange Membrane Fuel Cell, Andrew T. Haug, Ralph E. White, John W. Weidner, Wayne Huang, Steven Shi, Narender Rana, Stephan Grunow, Timothy C. Stoner, Alain E. Kaloyeros
Faculty Publications
Placing a layer of Ru atop a Pt anode increases the carbon monoxide tolerance of proton-exchange membrane fuel cells when oxygen is added to the fuel stream. Sputter-deposited Ru filter anodes composed of a single Ru layer and three Ru layers separated by Nafion-carbon ink, respectively, were compared to Pt, Pt:Ru alloy, and an ink-based Ru filter anodes. The amount of Pt in each anode was 0.15 mg/cm2 and the amount of Ru in each Ru-containing anode was 0.080 mg/cm2. For an anode feed consisting of hydrogen, 200 ppm CO, and 2% O2 (in the form …
Study Of Sn-Coated Graphite As Anode Material For Secondary Lithium-Ion Batteries, Basker Veeraraghavan, Anand Durairajan, Bala Haran, Branko N. Popov, Ronald Guidotti
Study Of Sn-Coated Graphite As Anode Material For Secondary Lithium-Ion Batteries, Basker Veeraraghavan, Anand Durairajan, Bala Haran, Branko N. Popov, Ronald Guidotti
Faculty Publications
Tin-graphite composites have been developed as an alternate anode material for Li-ion batteries using an autocatalytic deposition technique. The specific discharge capacity, coulombic efficiency, rate capability behavior, and cycle life of Sn-C composites has been studied using a variety of electrochemical methods. The amount of tin loading and the heating temperature have a significant effect on the composite performance. The synthesis conditions and Sn loading on graphite have been optimized to obtain the maximum reversible capacity for the composite electrode. Heating the composite converts it from amorphous to crystalline form. Apart from higher capacity, Sn-graphite composites possesses higher coulombic efficiency, …
Modeling The Effects Of Electrode Composition And Pore Structure On The Performance Of Electrochemical Capacitors, Changqing Lin, Branko N. Popov, Harry J. Ploehn
Modeling The Effects Of Electrode Composition And Pore Structure On The Performance Of Electrochemical Capacitors, Changqing Lin, Branko N. Popov, Harry J. Ploehn
Faculty Publications
This work presents a mathematical model for charge/discharge of electrochemical capacitors that explicitly accounts for particle-packing effects in a composite electrochemical capacitor consisting of hydrous RuO2 nanoparticles dispersed within porous activated carbon. The model is also used to investigate the effect of nonuniform distributions of salt in the electrolyte phase of the electrode in the context of dilute solution theory. We use the model to compare the performance of capacitors with electrodes made from different activated carbons and to investigate the effects of varying carbon content and discharge current density. Even at low discharge current density, concentration polarization in …
Modeling The Effects Of Electrode Composition And Pore Structure On The Performance Of Electrochemical Capacitors, Changqing Lin, Branko N. Popov, Harry J. Ploehn
Modeling The Effects Of Electrode Composition And Pore Structure On The Performance Of Electrochemical Capacitors, Changqing Lin, Branko N. Popov, Harry J. Ploehn
Faculty Publications
This work presents a mathematical model for charge/discharge of electrochemical capacitors that explicitly accounts for particle-packing effects in a composite electrochemical capacitor consisting of hydrous RuO2 nanoparticles dispersed within porous activated carbon. The model is also used to investigate the effect of nonuniform distributions of salt in the electrolyte phase of the electrode in the context of dilute solution theory. We use the model to compare the performance of capacitors with electrodes made from different activated carbons and to investigate the effects of varying carbon content and discharge current density. Even at low discharge current density, concentration polarization in …
Modeling Of A Nickel-Hydrogen Cell: Phase Reactions In The Nickel Active Material, B. Wu, Ralph E. White
Modeling Of A Nickel-Hydrogen Cell: Phase Reactions In The Nickel Active Material, B. Wu, Ralph E. White
Faculty Publications
No abstract provided.
Modeling Lithium Intercalation In A Porous Carbon Electrode, Gerardine G. Botte, Ralph E. White
Modeling Lithium Intercalation In A Porous Carbon Electrode, Gerardine G. Botte, Ralph E. White
Faculty Publications
No abstract provided.
Proton Diffusion In Nickel Hydroxide: Prediction Of Active Material Utilization, Sathya Motupally, Christopher C. Streinz, John W. Weidner
Proton Diffusion In Nickel Hydroxide: Prediction Of Active Material Utilization, Sathya Motupally, Christopher C. Streinz, John W. Weidner
Faculty Publications
Galvanostatic charge and discharge experiments reveal that the active material in nickel electrodes cannot be fully accessed at high currents or for thick films. It has been proposed that the utilization of the active material is controlled by the diffusion rate of protons through the film. This hypothesis is supported by the good agreement between mathematical simulations of material utilization and experimental data over a range of charge and discharge currents and film thicknesses. Furthermore, the fraction of material utilized is larger on charge than on discharge. The asymmetry on charge and discharge is due to a diffusion coefficient that …
Electrochemical Investigations Of Cobalt-Doped Limn2O4 As Cathode Material For Lithium-Ion Batteries, P. Arora, Branko Popov, Ralph E. White
Electrochemical Investigations Of Cobalt-Doped Limn2O4 As Cathode Material For Lithium-Ion Batteries, P. Arora, Branko Popov, Ralph E. White
Faculty Publications
A wide range (y = 0.05–0.33) of Co-doped LiCoyMn2–yO4 spinels were synthesized and electrochemically characterized. These Co-doped spinels showed improved specific capacity and capacity retention over pure spinels. Electrochemical impedance spectroscopy and the linear polarization resistance technique were used to determine the transport and electrochemical kinetic parameters of Co-doped spinels. The presence of Co in the spinel inhibits the passivation process occurring on the surface of the cathode. Also, Co increases the exchange current density and facilitates the charge-transfer reaction of the active material. The lower self-discharge observed for Co-doped spinels was attributed …
Theoretical Analysis Of Metal Hydride Electrodes: Studies On Equilibrium Potential And Exchange Current Density, Bala S. Haran, Branko N. Popov, Ralph E. White
Theoretical Analysis Of Metal Hydride Electrodes: Studies On Equilibrium Potential And Exchange Current Density, Bala S. Haran, Branko N. Popov, Ralph E. White
Faculty Publications
A theoretical model for the metal hydride electrode has been developed assuming that hydrogen diffusion in the alloy and charge-transfer at the surface control the discharge process. Theoretical equations for the dependence of equilibrium potential and exchange current density on the surface hydrogen concentration have been derived. These parameters have been used to correlate experimental data with the theoretical electrode discharge model. Analysis of both the experimental and theoretical discharge curves reveals a potential plateau determined by the magnitude of the interactions between the hydrogen in the alloy and the unhydrided metal. Neglecting these hydrogen-metal site interactions results in simulations …
The Role Of Oxygen At The Second Discharge Plateau Of Nickel Hydroxide, Sathya Motupally, Mukul Jain, Venkat Srinivasan, John W. Weidner
The Role Of Oxygen At The Second Discharge Plateau Of Nickel Hydroxide, Sathya Motupally, Mukul Jain, Venkat Srinivasan, John W. Weidner
Faculty Publications
It was shown that the appearance of a secondary discharge plateau approximately 400 mV below the primary plateau can result from the reduction of oxygen. During the galvanostatic discharge of planar nickel-hydroxide films at room temperature and in 3 weight percent KOH solutions, the second discharge plateau was observed only in the presence of dissolved oxygen in the electrolyte. When the solution was deoxygenated, no residual capacity could be extracted from the films even at low discharge rates or from overcharged films. In addition, the duration of the second plateau is inversely proportional to the square of the discharge current, …
The Effect Of Particle Size On The Discharge Performance Of A Nickel-Metal Hydride Cell, Jussi M. Heikonen, Harry J. Ploehn, Ralph E. White
The Effect Of Particle Size On The Discharge Performance Of A Nickel-Metal Hydride Cell, Jussi M. Heikonen, Harry J. Ploehn, Ralph E. White
Faculty Publications
We investigate the effect of particle size on the discharge performance of a nickel-metal hydride cell with a mathematical model. Electrodes with uniform as well as with nonuniform particle sizes are studied. With uniform particle size, the dependence of the particle-to-particle resistance on the particle size is taken into account. The optimal particle size depends on the discharge rate. Moreover, we show that under certain conditions it is advantageous to use a nonuniform particle size. In general, the higher the discharge current density, the more the particle size affects the electrode performance.
Governing Equations For Transport In Porous Electrodes, Pauline De Vidts, Ralph E. White
Governing Equations For Transport In Porous Electrodes, Pauline De Vidts, Ralph E. White
Faculty Publications
No abstract provided.
Electrowinning Of Nonnoble Metals With Simultaneous Hydrogen Evolution At Flow-Through Porous Electrodes Iii. Time Effects, Mahmoud M. Saleh, John W Weidner, Bahgat E. El-Anadouli, Badr G. Ateya
Electrowinning Of Nonnoble Metals With Simultaneous Hydrogen Evolution At Flow-Through Porous Electrodes Iii. Time Effects, Mahmoud M. Saleh, John W Weidner, Bahgat E. El-Anadouli, Badr G. Ateya
Faculty Publications
The electrowinning of zinc from a recirculating alkaline zincate solution at a flow-through porous electrode was investigated. Experimental results were obtained to test the predictions of a mathematical model. The effects of electrolyte flow rate, cell current, and electrode thickness on the concentration-time relations and coulombic efficiency-time relations were studied. The experimental results show that the highest recovery rate was obtained at both high flow rates and cell currents. There is, however, a practical limit for increasing both the cell current and the electrolyte flow rate. Reasonable agreement between the model predictions and experimental results was obtained. A case study …
An Electrochemical Route For Making Porous Nickel Oxide Electrochemical Capacitors, Venkat Srinivasan, John W. Weidner
An Electrochemical Route For Making Porous Nickel Oxide Electrochemical Capacitors, Venkat Srinivasan, John W. Weidner
Faculty Publications
Porous nickel oxide films were prepared by electrochemically precipitating nickel hydroxide and heating the hydroxide in air at 300°C. The resulting nickel oxide films behave as an electrochemical capacitor with a specific capacitance of 59 F/g electrode material. These nickel oxide films maintain high utilization at high rates of discharge (i.e., high power density) and have excellent cycle life. Porous cobalt oxide films were also synthesized. Although the specific capacitances of these films are approximately one-fifth that of the nickel oxide films, the results demonstrate the versatility of fabricating a wide range of porous metal oxide films using …
Anodic Oxidation Of Ethylenediaminetetraacetic Acid On Platinum Electrode In Alkaline Medium, S. N. R. Pakalapati, Branko N. Popov, Ralph E. White
Anodic Oxidation Of Ethylenediaminetetraacetic Acid On Platinum Electrode In Alkaline Medium, S. N. R. Pakalapati, Branko N. Popov, Ralph E. White
Faculty Publications
The anodic oxidation of ethylenediaminetetraacetic acid (EDTA) was studied in alkaline medium on a smooth platinum electrode. Bulk electrolysis indicated that stable organic intermediates (formaldehyde and glyoxal) are formed during the oxidation of EDTA and that complete oxidation to CO2 can be achieved. The proposed pathway suggests that the acetate groups in EDTA are initially oxidized, generating formaldehyde and ethylenediamine. The rest potential of EDTA (0.066 to 0.164 V vs. Hg/HgO) was observed to be higher than for other organic species. In alkaline medium, very little EDTA oxidation was found to occur on bare platinum. Limiting-current behavior due to …
Anomalous Codeposition Of Fe-Ni Alloys And Fe-Ni-Sio2 Composites Under Potentiostatic Conditions, M. Ramasubramanian, S. N. Popova, Branko N. Popov, Ralph E. White, K. M. Yin
Anomalous Codeposition Of Fe-Ni Alloys And Fe-Ni-Sio2 Composites Under Potentiostatic Conditions, M. Ramasubramanian, S. N. Popova, Branko N. Popov, Ralph E. White, K. M. Yin
Faculty Publications
A mathematical model has been developed to describe the electrodeposition of Fe-Ni alloys and Fe-Ni-SiO2 composites under potentiostatic conditions. This model can be used to predict the polarization behavior, partial current densities, and alloy composition of each of the components as a function of the applied potential. Fe-Ni-SiO2 samples were deposited on platinum rotating disk electrodes from sulfate electrolytes under potentiostatic conditions, and the results obtained were compared to the model. The model predictions were found to agree well with the experimental observations for the Fe-Ni and Fe-Ni-SiO2 systems.
A Model For The Galvanostatic Deposition Of Nickel Hydroxide, Mahesh Murthy, Gowri S. Nagarajan, John W. Weidner, John W. Van Zee
A Model For The Galvanostatic Deposition Of Nickel Hydroxide, Mahesh Murthy, Gowri S. Nagarajan, John W. Weidner, John W. Van Zee
Faculty Publications
A mathematical model is presented for the galvanostatic deposition of Ni(OH)2 films in stagnant Ni(NO3)2 solutions. The objective is to quantify the anomalous deposition behavior reported previously in which the utilization of the electrochemically generated OH– species decreased drastically as the concentration of Ni(NO3)2 increased beyond 0.1 M. For example as the Ni(NO3)2 concentration increased from 0.1 to 2.0 M, the deposition rate decreased by a factor of ten at 2.5 mA/cm2. At this high ratio of concentration to current density, a comparison with Faraday's …
Electrochemical Determination Of The Diffusion Coefficient Of Hydrogen Through An Lani4.25Al0.75 Electrode In Alkaline Aqueous Solution, G. Zheng, Branko N. Popov, Ralph E. White
Electrochemical Determination Of The Diffusion Coefficient Of Hydrogen Through An Lani4.25Al0.75 Electrode In Alkaline Aqueous Solution, G. Zheng, Branko N. Popov, Ralph E. White
Faculty Publications
Theconstant potential and constant current discharge techniques were used todetermine the hydrogen diffusion coefficients in an LaNi4.25Al0.75 electrode. The valuesobtained were 2.97 × 10–11 and 3.30 × 10–11 cm2/s, respectively. The advantages and disadvantages of these two techniques are discussed.
Electrochemical Determination Of The Diffusion Coefficient Of Hydrogen Through An Lani4.25Al0.75 Electrode In Alkaline Aqueous Solution, G. Zheng, Branko N. Popov, Ralph E. White
Electrochemical Determination Of The Diffusion Coefficient Of Hydrogen Through An Lani4.25Al0.75 Electrode In Alkaline Aqueous Solution, G. Zheng, Branko N. Popov, Ralph E. White
Faculty Publications
The constant potential and constant current discharge techniques were used to determine the hydrogen diffusion coefficients in an LaNi4.25Al0.75 electrode. The values obtained were 2.97 × 10–11 and 3.30 × 10–11 cm2/s, respectively. The advantages and disadvantages of these two techniques are discussed.
Mathematical Modeling Of The Formation Of Calcareous Deposits On Cathodically Protected Steel In Seawater, J. F. Yan, T. V. Nguyen, Ralph E. White, R. B. Griffin
Mathematical Modeling Of The Formation Of Calcareous Deposits On Cathodically Protected Steel In Seawater, J. F. Yan, T. V. Nguyen, Ralph E. White, R. B. Griffin
Faculty Publications
A first principle mathematical model of the formation of calcareous deposits on a cathodically protected steel rotatingdisk electrode in seawater is presented. The model includes equations which transport phenomena, electrochemical reactions,precipitation reactions, and a homogeneous reaction involved in the formation of calcareous deposits on an electrodesurface. Predicted concentration profiles show that a high concentration of OH– ions on the electrode surface leads to the formation of calcareous deposits. The calcareous deposits contain mostly CaCO3, but the initial deposits are predicted to contain more Mg(OH)2 than CaCO3. The predicted calcareous deposits on the electrode surface …
Galvanostatic Pulse And Pulse Reverse Plating Of Nickel-Iron Alloys From Electrolytes Containing Organic Compounds On A Rotating Disk Electrode, Branko N. Popov, Ken-Ming Yin, Ralph E. White
Galvanostatic Pulse And Pulse Reverse Plating Of Nickel-Iron Alloys From Electrolytes Containing Organic Compounds On A Rotating Disk Electrode, Branko N. Popov, Ken-Ming Yin, Ralph E. White
Faculty Publications
Linear sweep voltammetry, galvanostatic pulse, and pulse reverse techniques were used to study the plating of nickel-iron alloys in the presence of organic additives. The effects of pulse current densities, ip, reverse current densities, ir, rotation speed of disk electrode, and the presence of organic additives on deposition of nickel-iron alloys are evaluated. The observed phenomena can be explained by the concentration depletion of reactants (or products), and the surface coverage of the additives on the electrode. A new formulation of the plating bath is defined.
Impedance Analysis For Oxygen Reduction In A Lithium Carbonate Melt: Effects Of Partial Pressure Of Carbon Dioxide And Temperature, Bhasker B. Dave, Ralph E. White, Supramaniam Srinivasan, A. John Appleby
Impedance Analysis For Oxygen Reduction In A Lithium Carbonate Melt: Effects Of Partial Pressure Of Carbon Dioxide And Temperature, Bhasker B. Dave, Ralph E. White, Supramaniam Srinivasan, A. John Appleby
Faculty Publications
Effects of partial pressure of carbon dioxide and temperature on oxygen reduction kinetics on a gold electrode in a lithium carbonate melt were examined using electrochemical impedance spectroscopic (EIS) and linear sweep voltammetric techniques. The impedance spectra were analyzed by a complex nonlinear least squares method, using the Randles-Ershler equivalent circuit model, to determine the electrode-kinetic and the mass-transfer parameters such as the charge-transfer resistance and the Warburg coefficient. The cyclic voltammetric measurements indicated that the oxygen reduction process in lithium carbonate melt is "reversible" up to 200 mV/s. The product DC0 determined by cyclic voltammetry agreed well …
Mathematical Modeling Of A Primary Zinc/Air Battery, Z. Mao, Ralph E. White
Mathematical Modeling Of A Primary Zinc/Air Battery, Z. Mao, Ralph E. White
Faculty Publications
The mathematical model developed by Sunu and Bennion has been extended to include the separator, precipitation of both solid ZnO and K2Zn(OH)4, and the air electrode, and has been used to investigate the behavior of a primary Zn-Air battery with respect to battery design features. Predictions obtained from the model indicate that anode material utilizationis predominantly limited by depletion of the concentration of hydroxide ions. The effect of electrode thickness on anode material utilization is insignificant, whereas material loading per unit volume has a great effect on anode material utilization; a higher loading lowers both the …
Parameter Sensitivity And Optimization Predictions Of A Hydrogen/Oxygen Alkaline Fuel Cell Model, Michael C. Kimble, Ralph E. White
Parameter Sensitivity And Optimization Predictions Of A Hydrogen/Oxygen Alkaline Fuel Cell Model, Michael C. Kimble, Ralph E. White
Faculty Publications
A mathematical model is used to predict parameter sensitivities and optimal design parameters for a hydrogen/oxygen alkaline fuel cell. A sensitivity analysis of the various transport and electrode kinetic parameters indicates which parameters have the most influence on the predicted current density and over which range of potentials these parameters affect the fuel-cell performance the most. This information can be used to decide which parameters should be optimized or determined more accurately through further modeling or experimental studies. The effect of various design parameters on the limiting current density are investigated to determine if optimal values exist for the parameters. …
The Self-Discharge Of The Niooh/Ni(Oh)2 Electrode Constant Potential Study, Z. Mao, Ralph E. White
The Self-Discharge Of The Niooh/Ni(Oh)2 Electrode Constant Potential Study, Z. Mao, Ralph E. White
Faculty Publications
Hydrogen oxidation currents at a NiOOH/Ni(OH)2 electrode were measured directly at constant potentials for various hydrogen pressures and states of charge. It was found that the hydrogen oxidation current is linearly proportional to the hydrogen pressure at all electrode potentials and that the logarithm of the anodic current is a linear function of electrode potential. It was also found that hydrogen oxidation on the nickel substrate material was strongly inhibited by the presence of nickel hydroxide on the substrate surface. By comparing the currents for hydrogen oxidation and oxygen evolution on the NiOOH/Ni(OH)2 electrode and on a nickel …
Mathematical Modeling Of Cathodic Protection Using The Boundary Element Method With A Nonlinear Polarization Curve, J. F. Fan, S. N. R Pakalapati, T. V. Nguyen, Ralph E. White, R. B. Griffin
Mathematical Modeling Of Cathodic Protection Using The Boundary Element Method With A Nonlinear Polarization Curve, J. F. Fan, S. N. R Pakalapati, T. V. Nguyen, Ralph E. White, R. B. Griffin
Faculty Publications
The distributions of potential and current density around a cathodically protected pipeline in seawater were determined using the boundary element technique. A nonlinear polarization curve for a low carbon steel in artificial sea water was obtained from dc-potentiodynamic measurements and was fitted for use as the boundary condition on the pipe. The program was used to evaluate cases in which one or two aluminum sacrificial anodes are used to protect a low carbon steelpipe in seawater. The results show that the number of anodes, the sizes of the anodes, and the distance between the anodes and the cathode are of …
Current Distribution In A Horizon® Lead-Acid Battery During Discharge, Z. Mao, Ralph E. White, B. Jay
Current Distribution In A Horizon® Lead-Acid Battery During Discharge, Z. Mao, Ralph E. White, B. Jay
Faculty Publications
A simple mathematical model is presented and used to analyze the potential and current distributions in a HORIZON® sealed lead-acid battery. It was found that an increase in the thickness of an electrode would not enhance the discharge rate of that electrode; instead, it causes the transfer current distribution to be less uniform in the electrode. Also, the ohmic drop across the separator would decrease with a decrease in the thickness of the separator more rapidly when the thickness is small than when it is large. In addition, it was found that efficient high-capacity, high-rate electrodes must consider the electrode …
Electrochemical Characterization Of Electronically Conductive Polypyrrole On Cyclic Voltammograms, Taewhan Yeu, Ken-Ming Yin, Jose Carbajal, Ralph E. White
Electrochemical Characterization Of Electronically Conductive Polypyrrole On Cyclic Voltammograms, Taewhan Yeu, Ken-Ming Yin, Jose Carbajal, Ralph E. White
Faculty Publications
Experimental and theoretical cyclic voltammograms for electronically conducting polypyrrole film are obtained from the identical conditions and compared to each other to characterize electrochemical behavior of the polymer. A comparison of the simulated and experimental cyclic yoltammograms shows quantitative agreement. The profiles of the dependent variables show that the switching process is governed by the availability of the counter ion to the polypyrrole electrode and the amount of electroactive sites. Sensitivity analysis shows that the double layer effects have more influence in the cyclic voltammograms than the electrokinetic effects.
A Mathematical Model Of The Self-Discharge Of A Ni-H2 Battery, Z. Mao, Ralph E. White
A Mathematical Model Of The Self-Discharge Of A Ni-H2 Battery, Z. Mao, Ralph E. White
Faculty Publications
A simple mathematical model is presented and used to characterize the self-discharge of a nickel oxyhydroxide(NiOOH) electrode in a hydrogen environment. This model includes diffusion of dissolved hydrogen in an electrolyte film which covers a flooded electrode, electrochemical oxidation of hydrogen, reduction of nickel oxyhydroxide, and changes of surface area and of porosity of the electrode during the self-discharge process. Although the self-discharge process is complicated, the predictions of the model are consistent with experimental results reported in the literature, which include linear relationships between the logarithm of hydrogen pressure and time and between the logarithm of the capacity remaining …
A Mathematical Model Of A Hydrogen/Oxygen Alkaline Fuel Cell, Michael C. Kimble, Ralph E. White
A Mathematical Model Of A Hydrogen/Oxygen Alkaline Fuel Cell, Michael C. Kimble, Ralph E. White
Faculty Publications
A mathematical model of a hydrogen/oxygen alkaline fuel cell is presented that can be used to predict polarization behavior under various potential loads. The model describes the phenomena occurring in the solid, liquid, and gaseous phases of the anode, separator, and cathode regions, assuming a macrohomogeneous, three-phase porous electrode structure. The model calculates the spatial variation of the partial pressures of oxygen, hydrogen, and water vapor, dissolved oxygen and hydrogen concentrations, electrolyte concentration, and the solid- and solution-phase potential drops. By developing a complete model of the alkaline fuel cell, the interaction of the various transport and kinetic resistances can …