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At least 289 records · Page 16

Targeted synthesis and reaction mechanism discussion of Mo 2 C based insertion-type electrodes for advanced pseudocapacitors

Mo 2 C is one of the few compounds that possess good electronic conductivity. Meanwhile, it possesses a natural 1D zigzag tunnel structure that is ideally suited for fast ion diffusion. Here, an effective approach is demonstrated for fabrication of structurally stable N-doped Mo 2 C/C nanobelts. They demonstrate high and fast energy storage ability with initial capacitances of 1139 C g -1 at 1 mV s-1, 151 C g -1 at an extremely high scan rate of 2000 mV s -1 and 208 C g -1 at a discharge current density of 200 A g -1 . After electrochemical activation of cycling, the capacity is continuously enhanced and much higher capacitances of 2523 C g -1 at 1 mV s -1 and 1403 C g -1 at 50 A g -1 are achieved after 15,000 cycles at 50 mV s -1 . Using the power law, it is evaluated that a surface-controlled capacitive process makes the main contribution to the capacity, which is over 90% when the scan rates are higher than 10 mV s -1 and still high as 73% at 1 mV s -1 . From in situ synchrotron XRD, it is found that there is a negligible change in the crystal structure and volume during charging/discharging, reflecting an insertion-type charge storage mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electrochemical reduction of europium(iii) using tetra- n -octyl diglycolamide functionalized ordered mesoporous carbon microelectrodes

This work investigates the one-electron reduction of Eu(III) to Eu(II) with ordered mesoporous carbon (OMC) in cavity microelectrode (CME) systems. OMC materials with and without tetra-n-octyl diglycolamide (TODGA) functionalization were subjected to voltammetric measurements and compared with commercial carbon black Vulcan® XC-72. The electrochemical reduction of solution Eu(III) with unfunctionalized OMC, XC-72, and TODGA-functionalized OMC—both within the electrode matrix and on the electrode surface—is reported. The complexation of Eu(III) by TODGA-functionalized OMC prior to electrode preparation incorporates Eu(III) as part of the bulk electrode matrix. Under these conditions, the high capacitance obscures the Eu(III)/Eu(II) redox couple. A signal emerges above the background (capacitive) currents when 2-octanol is added to the TODGA-functionalized OMC as a wetting agent. In contrast, surface Eu(III)–TODGA complexation, when Eu(III) contacts the electrode surface exclusively after electrode preparation, provides a strong response. The addition of 2-octanol to TODGA reduces the capacitance of the electrode and narrows the Eu(III)/Eu(II) redox peak widths. In conclusion, the desorption by reductive stripping of Eu(II) was demonstrated using a 2-octanol modified TODGA OMC CME, opening the possibility for selective separation of Eu from adjacent trivalent lanthanides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermal stability of antiferroelectric-like Al:HfO 2 thin films with TiN or Pt electrodes

HfO 2 -based antiferroelectric-like thin films are increasingly being considered for commercial devices. However, even with initial promise, the temperature sensitivity of electrical properties such as loss tangent and leakage current remains unreported. 50 nm thick, 4 at. % Al-doped HfO 2 thin films were synthesized via atomic layer deposition with both top and bottom electrodes being TiN or Pt. A study of their capacitance vs temperature showed that the Pt/Al:HfO 2 /Pt had a relative dielectric permittivity of 23.30 ± 0.06 at room temperature with a temperature coefficient of capacitance (TCC) of 78 ± 86 ppm/°C, while the TiN/Al:HfO 2 /TiN had a relative dielectric permittivity of 32.28 ± 0.14 at room temperature with a TCC of 322 ± 41 ppm/°C. The capacitance of both devices varied less than 6% over 1 to 1000 kHz from –125 to 125 °C. Both capacitors maintained loss tangents under 0.03 and leakage current densities of 10 –9 –10 –7 A/cm 2 between –125 and 125 °C. The TiN/Al:HfO 2 /TiN capacitor maintained an energy storage density (ESD) of 18.17 ± 0.79 J/cm 3 at an efficiency of 51.79% ± 2.75% over the –125 to 125 °C range. The Pt/Al:HfO 2 /Pt capacitor also maintained a stable ESD of 9.83 ± 0.26 J/cm 3 with an efficiency of 62.87% ± 3.00% over the same temperature range. Finally, such low losses in both capacitors along with their thermal stability make antiferroelectric-like, Al-doped HfO 2 thin films a promising material for temperature-stable microelectronics.

36 MATERIALS SCIENCE↗

Strong-coupling quantum dot microscope

Here, we report the development and fabrication of a novel cryogenic instrument, a scanning quantum dot microscope (SQDM), capable of positioning a quantum dot to within tunneling range of a sample surface. The microscope is strong-coupling in the sense that electron wavefunctions in the quantum dot can directly overlap with electron wavefunctions in the sample, in contrast to probes based on electric-field coupling. The SQDM consists of a sharp glass probe with two asymmetric electrodes leading to an aluminum quantum dot at the apex. One electrode is capacitively coupled to the quantum dot, while the other lead is connected to the dot via a tunneling junction. A charge sensing circuit constructed from a high-electron-mobility transistor is attached to the capacitance lead to measure the charge state of the dot. The last key feature of the design is a tilted-apex geometry. This design feature, in conjunction with the capacitive sensing scheme, results in a robust quantum-dot probe capable of operating within angstrom distances of the sample surface while protecting the single tunnel junction responsible for electron transport onto the quantum dot. We demonstrate that our instrument can detect single-electron tunneling events and can also be operated as a standard scanning tunneling microscope capable of nanometer-scale resolution of the surface topography.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Correcting impedance measurements for background parasitics to characterize circuit components in cryogenic environments

Predictable circuit response is a critical prerequisite for accurate electronic measurements. Here, we describe a powerful yet straightforward experimental method and analysis model that utilizes an affordable LCR meter in conjunction with an in situ parasitic-impedance background-correction procedure to measure the temperature-dependent impedance (magnitude and phase) of up to ten individual passive circuit elements in a single cryostat run. We show how the model unambiguously identified a ∼20× drop in capacitance for 22 μF 5XR multilayer ceramic capacitors cooled from 300 K to 360 mK in an environment with a parasitic capacitance of ∼300 pF. The same experimental procedure, based on a simple two-wire measurement, was also used to measure 10 and 22 pF thin-film capacitors and 100 MΩ thick-film resistors. The results showed that the resistor values increased by up to an order of magnitude when the devices were cooled from 300 K to 360 mK. Most importantly, we showed that the simple data-acquisition method, coupled with our analysis model, enabled the measurement of component parasitics, and effectively extended the accuracy of a commercial LCR meter beyond its manufacturer-guaranteed values for a wide range of measurement frequencies. We also showed that, in the current configuration, our simple approach is limited to a capacitance accuracy of ∼10 pF.

Carpenter, R. J. [Santa Clara Univ., Santa Clara, ↗

Transport signatures of phase fluctuations in superconducting qubits

Abstract Josephson junctions supply the nonlinear inductance element in superconducting qubits. In the widely used transmon configuration, where the junction is shunted by a large capacitor, the low charging energy minimizes the sensitivity of the qubit to charge noise while maintaining the necessary anharmonicity to qubit states. We report here low-frequency transport measurements on small standalone junctions and identically fabricated capacitively-shunted junctions that show two distinct features normally attributed to small capacitance junctions near zero bias: reduced switching currents and prominent finite resistance associated with phase diffusion in the current–voltage characteristic. Our transport data reveals the existence of phase fluctuations in transmons arising from intrinsic junction capacitance.

Wisne, M. (ORCID:0009000610684209)↗

Merged-Element Transmon

Transmon qubits are ubiquitous in the pursuit of quantum computing using superconducting circuits. However, they have some drawbacks that still need to be addressed. Most importantly, the scalability of transmons is limited by the large device footprint needed to reduce the participation of the lossy capacitive parts of the circuit. In this work, we investigate and evaluate losses in an alternative device geometry, namely, the merged-element transmon (mergemon). To this end, we replace the large external shunt capacitor of a traditional transmon with the intrinsic capacitance of a Josephson junction and achieve an approximately 100 times reduction in qubit dimensions. We report the implementation of the mergemon using a sputtered Nb–amorphous-Si–Nb trilayer film. In an experiment below 10 mK, the frequency of the readout resonator, capacitively coupled to the mergemon, exhibits a qubit-state-dependent shift in the low-power regime. The device also demonstrates the single-photon and multiphoton transitions that represent a weakly anharmonic system in two-tone spectroscopy. The transition spectra are explained well with master-equation simulations. Here, a participation-ratio analysis identifies the dielectric loss of the amorphous-Si tunnel barrier and its interfaces as the dominant source for qubit relaxation. We expect the mergemon to achieve high coherence for relatively small device dimensions when implemented with a low-loss, epitaxially grown, and lattice-matched trilayer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Modeling the Impacts of Material Properties on Oscillatory Neuron Behavior

In this study, neuromorphic computing, which mimics the functions of biological brains, offers improvements in both latency and energy efficiency over typical von Neumann computing architectures. Spiking neural networks can be especially power-efficient because they encode information temporally and can use more sparse electrical inputs. Here, we study the design of volatile memristors (variable resistors with memory) for neuronal devices, with particular consideration toward the feasibility of all-on-chip oscillation using built-in capacitance. We use circuit simulations to model the behavior of oscillator neurons with a range of realistic material properties. We find that energy inputs increase with insulating-phase resistivity, thermal conductivity, and device aspect ratio. However, we also find that the minimum capacitance needed for oscillation decreases with increasing insulating-phase resistivity, which opposes the constraints for power efficiency. Based on published data on NbO 2 , VO 2 , and EuNiO 3 , we find that existing materials can be engineered for all-on-chip spiking using their parasitic capacitance.

36 MATERIALS SCIENCE↗

Demonstration of Vertical 2T-nC FeRAM Hybrid Cell and Its Scalability for High-Density 3-D Ferroelectric Capacitor Memory

In this work, we present a comprehensive experimental and modeling study on the scaling of vertical 2T-nC ferroelectric random access memory (FeRAM) hybrid cells, comprising n metal-ferroelectric–metal (MFM) capacitors, to demonstrate a high-performance and high-density 3-D capacitor memory. Our contributions include: 1) successful process integration of vertical 2T-3C FeRAM cells by stacking MFM structures on top of Si CMOS transistors; 2) experimental validation of memory cell functionality, confirming the feasibility of the vertical 2T-nC FeRAM architecture; 3) an analysis of scaling effects on parasitic capacitance in densely integrated 3-D arrays, using 3-D technology computer-aided design (TCAD) simulations; 4) exploration of aggressive stacking of write bitlines (WBLs) to enhance memory density, where ferroelectric linear capacitance ( C FE ) enables self-boosted inhibition under the V W /2 scheme, but renders the V W /3 scheme ineffective due to intolerable write disturbances; and 5) assessment of horizontal scaling, revealing significant increases in read disturbances caused by interplane capacitance between adjacent WBLs ( C Z ). This work represents an early exploration into the potential of 2T-nC FeRAM as a scalable and efficient 3-D memory solution.

42 ENGINEERING↗

The Effect of Proton Conductivity of Fe–N–C–Based Cathode on PEM Fuel cell Performance

A model–based impedance spectroscopy is used to determine proton conductivity, oxygen transport parameter, double layer capacitance and oxygen reduction reaction (ORR) Tafel slope in the Fe–N–C cathode catalyst layer (CCL) of a PEM fuel cell. Experimental spectra of two cells differing by the membrane thickness only are processed using a physics–based model for PEMFC impedance. The spectra have been measured in the range of current densities from 25 to 800 mA cm -2 . The ORR Tafel slope of both the cells shows almost linear growth with the current density. In one of the cells, the CCL proton conductivity σp strongly decays at the current density of 100 mA cm -2 ; this decay is accompanied by the step growth of the double layer capacitance. Other minor variations of proton conductivity and double layer capacitance with the cell current occur also in a counterphase; presumed origin of this effect is discussed. The oxygen diffusion coefficient in the cathode exhibits explosive growth with the cell current. We attribute this effect to formation of temperature and pressure gradients in the CCL due to strongly non–uniform distribution of ORR rate in the electrode.

25 ENERGY STORAGE↗

Mechanistic Insights of Pore Contributions in Carbon Supercapacitors by Modified Step Potential Electrochemical Spectroscopy

Porous carbons are widely used as electrode materials for electrical double layer (EDL)-type supercapacitors. Differentiation of capacitance contributions from micropores and mesopores is important to understand porous carbon capacitive behavior. However, this remains challenging to accomplish. Here, we present an improved step potential electrochemical spectroscopy method to investigate the contributions to capacitance from hierarchical pores and redox processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Carbon Electrodes from Powder River Basin Coal Development of Competitive Supercapacitor Electrodes of Diverse Compositions from Coal Extract

Recent demand for coal as a thermal energy source has decreased significantly and will likely continue to decrease as renewable sources of energy become more available and environmental concern and cost from burning coal makes it more costly than renewables. Given that Powder River Basin (PRB) coal in Wyoming has relatively low thermal energy, it is critical for Wyoming to employ coal in other capacities at the current energy transition period in history. Among many potential non-thermal applications, PRB coal can be utilized for membrane and electrode applications through the formation of carbon fibers. Coal-derived membranes can become low-cost, conductive membranes for use in electrodialysis separation processes. Carbon fiber derived electrodes have been shown be a cost-effective alternative to typical electrode materials that can meet or exceed the performance of current carbon electrode materials. In this talk, we demonstrate the manufacture of supercapacitor electrodes from Powder River Basin (PRB) coal-derived precursors. Specifically, PRB coal was treated in cheap solvents, partitioned into liquid extract and solid residue. An electropinning process has been developed that can convert either the liquid extract or the solid residue into carbon fiber mats. The electrospinning process is versatile with many tunable process parameters to achieve desirable physiochemical properties. For example, the coal residue can be manipulated by additional heat treatment, or by adding binders, salts, or surfactants to create a solution that can be electrospun into advanced carbon electrodes with desirable structural and surface properties. Similarly, some of the liquid extract (tar fraction) can be subsequently reacted with toluene diisocyanate to create resinous coal-derived polyurethane (PUs) as a spinnable ink. Carbon nanofiber mats made from our proprietary electrospinning process were further carbonized at temperature ranging from 700°C to 900°C before they are used as electrodes in supercapacitors. Galvanostatic charge-discharge (GCD) results show that the best performing PU fiber mats can deliver a specific capacitance of 604 F g -1 at the current density of 1 A g -1 . A carbon fiber mat from a different solvent extraction residue also delivered the specific capacitance of 508 F g -1 . These specific capacitance values are comparable to or better than commercial activated carbons, demonstrating the viability of manufacturing carbon nanofiber electrodes from coal without the use of a commercial polymer as binder in the spinning ink.

Cincotta, Robert↗

Photon-to-Digital Converters for Neutron Imaging Instruments (Final Report)

Oak Ridge National Laboratory (ORNL) collaborated with the Université de Sherbrooke (UdeS) to design a modular and scalable tile of innovative digital photodetectors called Photon-to-Digital Converters (PDC) and the required subsystems to demonstrate the feasibility of large area single-photon detectors to support high-resolution, depth-of-interaction, fast neutron radiography based on scintillation detectors. The goal is to demonstrate the advantages of using PDC over conventional Silicon Photomultiplier (SiPM) for neutron imaging systems. The basic building blocks of analog SiPM and PDC are Single-Photon Avalanche Photodiodes (SPAD). The main difference between conventional SiPMs and PDCs, is in the fact that analog SiPMs sum the charge produced by individual SPAD passively, while in PDCs each SPAD is read out individually by an active electronic circuit. Hence, PDCs provide a direct photon-to-bit conversion where a logic “1” means that there was a detection in a given SPAD. Conversely, an analog SiPM requires a sophisticated preamplifier (current amplifiers or transimpedance amplifier) followed by a shaping amplifier and an analog-to-digital converter. Moreover, since the charge from each SPAD varies slightly, the passive sum of the analog SiPM will have signal fluctuations for the same amount of photon detected. This is one of many issues that is completely eliminated by individual one-to-one SPAD read out in PDCs. The large area required for scintillator readouts for neutron imaging is such that the output capacitance of a large area of SiPM arrays is very high. This creates a burden on the signal-to-noise optimization with respect to the power budget. For PDC, the power consumption is dictated by rate of the incident photon flux, or in photon-starved environments, the dark noise rate of the SPAD array. In other words, the power consumption in the absence of events is extremely low. Hence, the power consumption of a PDC read out system is much lower than its analog counterpart. Further, the large SiPM capacitance may introduce signal distortions on the scintillator fast rise or decay time with undesired effects on timing and pulse shape discrimination. The problem is absent in PDCs, as their readout is independent on device capacitance. UdeS is the world leader in 3D vertical integration of frontside illuminated SPAD arrays over CMOS readouts. These capabilities allow future production of “3D PDC” with maximum photosensitive fill factor and electronic functionalities tailored to the application. UdeS' vast knowledge of SPADs and CMOS design made the team an ideal collaborator in the development of large area high-resolution fast neutron radiography.

42 ENGINEERING↗

Upcycling Linear Low-Density Polyethylene Waste into Graphene for High Mass Loading Supercapacitors

Polyethylene is notoriously difficult to upcycle because it decomposes into light gases at approximately 350-400 °C which prevents processing it at higher temperatures to convert it into electrode materials. We address this challenge by using an air-based, thermos-oxidative process, which heats linear low-density polyethylene (LLDPE) just below the decomposition point to initiate oxidation and cross-linking of LLDPE alkyl chains. These molecular transformations allow LLDPE to be graphenized at 950 °C without decomposing. The LLDPE-derived graphene (LLDPE-G) has a BET specific surface area up to 1,800 m2/g and Raman ID/IG ratio of 0.85. When used as electrode material for a symmetric supercapacitor with the 1 M H2SO4 electrolyte, LLDPE-G possesses an specific capacitance up to 175 F/g at mass loading of 20 mg/cm2, yielding an areal capacitance of 3.5 F/cm2. The cycling stability with capacitance demonstrates a retention of 95.8% after 100,000 cycles at high current density of 4.0 A/g.

Gao, Yuan↗

Upcycling Linear Low-Density Polyethylene Waste into Graphene for High Mass Loading Supercapacitors

Upcycling plastic into advanced carbons, such as graphene and porous carbon, offers attractive options to manage waste streams by converting the plastic into carbon electrode materials for energy storage devices. Linear low density polyethylene (LLDPE) is firstly bulk-oxidized with a facile and scalable method and then carbonized and catalyticlly graphenized into porous graphene materials. The LLDPE derived graphene (LLDPE-G) has a BET specific surface area up to 1800 m2/g and Raman ID/IG ratio of 0.85. When used as electrode material for symmetric supercapacitor, LLDPE-G possesses outstanding specific capacitance and excellent areal capacitance. Moreover, LLDPE-G exhibits exceptional cycling stability with capacitance retention of 95.8% after 100,000 cycles. Last but not least, KCl is recycled and reused over 3 cycles with material quality and electrocapacitive performance of LLDPE-G retained and verified after each cycle.

Gao, Yuan↗

Upcycling Low Linear Density Polyethylene Waste into Turbostratic Graphene for High Mass Loading Supercapacitors

In this work, LLDPE was upcycled into a high quality turbostratic graphene using a pre-treatment step to oxidatively crosslink the polymer with the assistance of solid additives (KCl and K2CO3) that improve crosslinking by increasing the effective surface area of the polymer melt during processing. After this pretreatment step, the crosslinked polymer could then be carbonized and catalytically graphenized between 400-950 °C without complete decomposition of the material. The LLDPE derived graphene (LLDPE-G) obtained from this process has a Brunauer–Emmett–Teller (BET) specific surface area, up to 1800 m2g-1 and average Raman ID/IG and I2D/IG ratios of 0.85 and 0.57, respectively, indicating high quality graphene. When used as an electrode material in symmetric supercapacitors, LLDPE-G possesses an outstanding specific capacitance up to 175 Fg-1 at a mass loading of 20 mgcm-2, which is two times the commercial requirement, yielding an excellent areal capacitance of 3.5 Fcm-2. Moreover, LLDPE-G exhibits exceptional cycling stability with a capacitance retention of 95.8% after 100,000 cycles at a current density of 4.0 Ag-1. Additionally, the KCl and K2CO3 were recycled and reused over 3 complete cycles to make new LLDPE-G with the material quality and electrocapacitive performance retained and verified after each cycle. Our approach creates new opportunities for upcycling not only waste LLDPE but also other varieties of PE to high value graphene materials.

Gao, Yuan [NETL Site Support Contractor, National ↗

Evaluation of Three Types of Electric Field Sensors

On June 3-4, 2025, we evaluated three types of electric-field (E-field) sensors: capacitive electrodes, stainless-steel stakes, and porous pots - at two electromagnetic (EM) stations (PWBVI and PWAOF) on Aqueduct Mesa at the Nevada National Security Site. We compared calibrated time series and derived metrics including power spectral density, root-mean-square (RMS) amplitude, signal-to-noise ratio (SNR), and detectability of power line harmonics and Schumann resonance. The objective was to identify an alternative E field sensor with higher SNR than the existing capacitive electrodes. Our data demonstrates that stainless-steel electrodes perform best, with the highest SNR and the most consistent detection of power-line harmonics and Schumann resonance among the three sensor types; they may be used as a supplement to, or replacement for, the existing capacitive electrodes.

58 GEOSCIENCES↗

A review of transport models in charged porous electrodes

There is increased interest in many different processes based upon interactions between a charged solid surface and a liquid electrolyte. Energy storage in capacitive porous materials, ionic membranes, capacitive deionization (CDI) for water desalination, capacitive energy generation, removal of heavy ions from wastewater streams, and geophysical applications are some examples of these processes. Process development is driven by the production of porous materials with increasing surface area. Understanding of the physical phenomena occurring at the charged solid-electrolyte interface will significantly improve the design and development of more effective applied processes. The goal of this work is to critically review the current knowledge in the field. The focus is on concepts behind different models. We start by briefly presenting the classical electrical double layer (EDL) models in flat surfaces. Then, we discuss models for porous materials containing macro-, meso-, and micro-pores. Some of the current models for systems comprising two different pore sizes are also included. Finally, we discuss the concepts behind the most common models used for ionic transport and Faradaic processes in porous media. The latter models are used for simulation of electrosorption processes in porous media.

42 ENGINEERING↗