Pulse Cycle Research Articles

High-performance ferroelectric field-effect transistors with ultra-thin indium tin oxide channels for flexible and transparent electronics

With the development of wearable devices and hafnium-based ferroelectrics (FE), there is an increasing demand for high-performance flexible ferroelectric memories. However, developing ferroelectric memories that simultaneously exhibit good flexibility and significant performance has proven challenging. Here, we developed a high-performance flexible field-effect transistor (FeFET) device with a thermal budget of less than 400 °C by integrating Zr-doped HfO2 (HZO) and ultra-thin indium tin oxide (ITO). The proposed FeFET has a large memory window (MW) of 2.78 V, a high current on/off ratio (ION/IOFF) of over 108, and high endurance up to 2×107 cycles. In addition, the FeFETs under different bending conditions exhibit excellent neuromorphic properties. The device exhibits excellent bending reliability over 5×105 pulse cycles at a bending radius of 5 mm. The efficient integration of hafnium-based ferroelectric materials with promising ultrathin channel materials (ITO) offers unique opportunities to enable high-performance back-end-of-line (BEOL) compatible wearable FeFETs for edge intelligence applications.

Blind source separation for decomposing X-ray pulsar profiles

Accretion-powered X-ray pulsars offer a unique opportunity to study physics under extreme conditions. To fully exploit this potential, the interrelated problems of modelling radiative transport and the dynamical structure of the accretion flow must, however, be solved. This task is challenging both from a theoretical and observational point of view and is further complicated by a lack of direct correspondence between the properties of emission emerging from the neutron star and observed far away from it. In general, a mixture of emission from both poles of the neutron star viewed from different angles is indeed observed at some or even all phases of the pulse cycle. It is essential, therefore, to reconstruct the contributions of each pole to the observed flux in order to test and refine models describing the formation of the spectra and pulse profiles of X-ray pulsars. In this paper we propose a novel data-driven approach to address this problem using the pulse-to-pulse variability in the observed flux, and demonstrate its application to RXTE observations of the bright persistent X-ray pulsar Cen X-3. We then discuss the comparison of our results with previous work attempting to solve the same problem and how they can be qualitatively interpreted in the framework of a toy model describing emission from the poles of a neutron star.

Modeling and experimental comparison of pulsed-DC driven low-pressure plasma discharge in a metal tube

High-voltage pulsed-DC can be used to deposit films on the inner surfaces of tubes and pipes. However, the characteristics of the plasma discharge in the tubes and mechanisms of film deposition are not well understood. In this study, a discharge is formed in a metal tube inserted with a coaxial anode by microsecond (μs) pulsed power to explore the influence of the pulse parameters on the plasma characteristics, including the temporal and spatial evolution near the tube walls experimentally and by simulation. The discharge waveform is monitored by a voltage-current probe to analyze the impact of the electrical characteristics on the plasma. The plasma properties are diagnosed by a Langmuir probe and numerically calculated by the fluid model. The source voltage and current jointly influence the plasma density and electron temperature, and secondary electron emission by energetic ion bombardment affects not only the distribution of electron density measured by the probe, but also the temporal distribution during the pulse-on and pulse-off time. The electron temperature varies conversely with the density from the plasma zone to the cathode suggesting the typical glow discharge in the pulsed-DC tube. Secondary electron emission is created at a higher discharge frequency, and a sustained plasma between pulse cycles appears to be produced at a higher frequency. The results impart information about the pulsed-DC driven plasma discharge at low pressure as well as the role energetic ions play on the cathode and elucidate the mechanisms of plasma deposition on the interior tube wall.

Fast Electrodeposition of MXene/PDA Composites for High‐Performance Bioelectronic Interfaces: An In Vitro Evaluation

AbstractBioelectrode is critical to many biomedical researches. However, traditional materials (typically noble metals) and manufacturing techniques limit the large‐scale production of bioelectrodes. Herein, a fast electrochemical approach is proposed to deposit versatile MXene/polydopamine (PDA) composites on a metalized substrate. PDA coating can improve the adhesion between MXene and the substrate, while MXene provides rough surfaces with unique micro/nanostructure and outstanding electrical/optical/thermal performance. The impedance of the as‐prepared bioelectrode at 1 kHz is down to 8.48 Ω cm2. The corresponding cathodic charge storage capacity (CSCc) and charge injection capacity (CIC) are up to ≈250 and 6.59 mC cm−2 respectively, much superior to that of bare Pt and other conventional material‐based electrodes. The MXene/PDA composites also demonstrate robust stability under continuous electrostimulation for 1 × 108 pulse cycles and 1000 CV cycles. Moreover, MXene/PDA composites show a high and rapid photothermal response. Photoelectrochemical activity is also observed with high photocurrent, ≈40 folds larger than that of bare Pt. The utility of this new electrode in ascorbic acid sensing is demonstrated. Excellent biocompatibility is verified via neuron adhesion test and viability assay.

Surface morphology evolution mechanisms of pulse laser polishing mold steel

In this study, high-frequency nanosecond pulse laser was conducted on mold steel surfaces for solving surface defects during polishing processes. The influence of different single-pulse energy densities on surface roughness was carefully investigated through technical experiments, with the lowest roughness obtained at 2.5 J/cm2. A computational fluid dynamics (CFD) model was developed to simulate the evolution of surface morphology at different energy densities. The applicability of the model was successfully verified by comparative experiments and simulative results. The evaporation threshold for nanosecond pulse laser polishing was found to be between 2.5 and 3.0 J/cm2. The introduction of evaporation and increased temperature gradients accelerate the flow of the melt pool, thereby leading to a shift in the driving force for fluid velocity. The short pulse cycle can create a continuous melt pool that moves with the laser beam, resulting in surface flattening along the scanning path. Under a large number of overlapping pulses, the surface over melting (SOM) mechanism dominated the morphology evolution of the molten pool. Significant findings demonstrated that pulse laser-induced heat accumulated to melt the peaks and valleys of the initial surface, while convective flow reduced the height difference of the melt pool. It can provide a new insight into surface roughness improvement of metals through nanosecond pulse laser polishing.

Thermal-hydraulic study of the EU-DEMO Helium Cooled Pebble Bed Breeding Blanket Primary Heat Transport System

The European DEMO reactor will work under normal operating conditions in accordance with a pulsed duty cycle. However unplanned and planned transients of plasma overpower may occur compromising the integrity of its plasma-facing components structures. Consequently, adopting appropriate tools is essential to accurately and consistently model the thermal-hydraulic response of the involved cooling systems under both normal operating conditions and accidental events. Given this background, the University of Palermo, in collaboration with EUROfusion, started a research work to study the thermal-hydraulic behaviour of the Primary Heat Transport System (PHTS) of the Helium Cooled Pebble Bed Breeding Blanket (HCPB BB) of the DEMO device under steady-state and transient conditions. The activity has been performed adopting a computational approach, employing the thermal-hydraulic system code TRACE version 5.0 patch 6. The key point of the work has been the code-to-code benchmark with the outcomes previously obtained with the RELAP5-3D code, to estimate the impact of the physical models, numerical resolution schemes and modelling techniques adopted on the predictive capabilities of the system codes considered. The models and the analysis results are presented and critically discussed herein.

Ultrasound assisted efficient separation of lithium from brine with a composite polyether sulfone-ionic liquid membrane.

Green, selective and efficient extraction of lithium as one of the most important components for energy storages with ultrasound-assisted membrane separation of lithium from brine, which contains alkali metal chlorides, is conducted using a composite membrane. The composite membrane is formed by sealing a supported ionic liquid membrane (consisting of 1-alkyl-3-methylimidazolium hexafluorophosphate ([RMIM][PF6]) + TBP) with a polyethersulfone (PES) membrane and a PVC thin film membrane. The aim of the study is to optimize the separation process for the selective extraction of lithium from alkali metals. Various parameters, including membrane composition, feed concentration, and ultrasonic conditions, are adjusted to identify the best operating conditions. The results reveal that a membrane containing xIL = 0.5 of [MOIM][PF6] exhibits higher selectivity compared to other membranes studied. The flux of lithium initially increases with shorter sonication times, but it decreases as the duration of ultrasonic irradiation is prolonged. The optimal frequency for the ultrasonic treatment, which matches the bulk modulus of the membrane, is approximately 250 kHz. Higher frequencies result in higher flux and selectivity in lithium separation; besides, optimizing the amplitude and pulse cycle of the ultrasound at 75% leads to increased flux. Moreover, higher flux and selectivity (percentage of lithium with respect to the all of the ion flux) are achieved when separating lithium from alkali metal chlorides at higher feed concentrations, ranging from 250 ppm to 1000 ppm. The selectivity is influenced by the hydrophobicity, which depends on the behavior of the ionic liquid membrane. The process is promising for the future of the lithium mining from brine.

Exploring the Mechanism of Pulse Hydraulic Fracturing in Tight Reservoirs

Pulse hydraulic fracturing is capable of creating intricate seam networks for improved reservoir recovery, but its dynamic damage mechanism remains unclear, limiting its scientific guidance for fracturing construction. This study combined the statistical damage and viscoelastic models according to the D-P criterion and fluid flow continuity equation to establish a mathematical model of the fluid–solid coupling under pulsed hydraulic pressure. The finite element approach was used to investigate the dynamic response and damage accumulation law of tight reservoirs under various pulse parameters. The model’s correctness was verified with indoor triaxial pulse hydraulic fracturing studies, and the Changqing oilfield’s pulse hydraulic fracturing parameters were optimized. The results showed that the rock body around the borehole sustained dynamic damage when exposed to pulsed fluid pressure. The impact force increases with frequency; however, when the frequency is too high, the dynamic pore pressure cannot be stabilized. Consequently, the damage to the rock mass starts to increase and then progressively decreases with higher pulse frequencies. The ideal frequency was found to be 1 Hz. The rock body steadily accumulates damage as the number of pulses rises, increasing the damage value gradually. At the same frequency, the damage is higher for larger pulse amplitudes and ground stress differences, as well as a smaller modulus of elasticity. Pulse cycling reduces the rupture pressure by up to 26% compared to conventional hydraulic fracturing. Moreover, the Sine wave is 4–20% better than the triangle wave. The pulse damage mechanism and parameter optimization in this paper provide theoretical support for improving the effect of hydraulic fracture modification.

Design of Experiments for Optimizing Ultrasound-Assisted Extraction of Bioactive Compounds from Plant-Based Sources

Plant-based materials are an important source of bioactive compounds (BC) with interesting industrial applications. Therefore, adequate experimental strategies for maximizing their recovery yield are required. Among all procedures for extracting BC (maceration, Soxhlet, hydro-distillation, pulsed-electric field, enzyme, microwave, high hydrostatic pressure, and supercritical fluids), the ultrasound-assisted extraction (UAE) highlighted as an advanced, cost-efficient, eco-friendly, and sustainable alternative for recovering BC (polyphenols, flavonoids, anthocyanins, and carotenoids) from plant sources with higher yields. However, the UAE efficiency is influenced by several factors, including operational variables and extraction process (frequency, amplitude, ultrasonic power, pulse cycle, type of solvent, extraction time, solvent-to-solid ratio, pH, particle size, and temperature) that exert an impact on the molecular structures of targeted molecules, leading to variations in their biological properties. In this context, a diverse design of experiments (DOEs), including full or fractional factorial, Plackett–Burman, Box-Behnken, Central composite, Taguchi, Mixture, D-optimal, and Doehlert have been investigated alone and in combination to optimize the UAE of BC from plant-based materials, using the response surface methodology and mathematical models in a simple or multi-factorial/multi-response approach. The present review summarizes the advantages and limitations of the most common DOEs investigated to optimize the UAE of bioactive compounds from plant-based materials.

Analysis of physiological pulsating flow of fractional Maxwell fluid in a locally narrow artery

The purpose of this paper is to provide a novel reference for the early diagnosis and treatment of atherosclerosis. Two-dimensional governing equations of fractional-order Maxwell fluid flow in a local stenotic artery are established, taking real physiological pulsating blood flow at inlet into consideration. Drawing support from the finite difference method as well as the L1 formula, vorticity and stream functions are introduced to acquire numerical solutions for velocity, stream function, and pressure. The distribution of blood flow in narrowed arteries within a real physiological pulse cycle is discussed. Furthermore, the influences of the degree of stenosis δ, the stenosis length parameter L0, fractional order parameter α, and relaxation time λ on crucial medical indicators, including the time average of the wall shear stress, oscillatory shear index, relative residence time, and pressure distribution are revealed. The results show that the deceleration and reversal phases of real physiological pulsatile flow critically affect the progression of arterial stenosis, and increasing the fractional order parameter α weakens the development of stenosis, while increasing λ has the opposite effect. This study is expected to serve as a reference for formulating standards of key medical indicators in the early diagnosis of vascular stenosis.

PCTS‐Controlled Synthesis of L10/L12‐Typed Pt‐Mn Intermetallics for Electrocatalytic Oxygen Reduction

AbstractPt‐based intermetallics are recognized as effective catalysts for oxygen reduction reaction (ORR) in fuel cells. However, the synthesis of intermetallics often requires prolonged annealing and the effect of different crystal structures on ORR still need to be investigated. Herein, L12‐Pt3Mn and L10‐PtMn intermetallics with Pt‐skin are rapidly synthesized through an emerging periodic carbothermal shock method to investigate their ORR‐activity difference. The formation of L12‐Pt3Mn and L10‐PtMn can be well‐controlled by the Pt/Mn feeding ratio, pulse cycles, and temperature. Electrocatalytic investigations show that L12‐Pt3Mn presents a more positive half‐wave potential (0.91 V vs RHE) and onset potential (1.02 V vs RHE) than those of L10‐PtMn. The mass activity and specific activity of L12‐Pt3Mn are respectively fourfold and threefold greater than those of L10‐PtMn. Theoretical calculations indicate that the L12‐Pt3Mn has a more substantial work function than L10‐PtMn, thereby conferring L12‐Pt3Mn with an increased electron density allocation for catalytic involvement. This electron confinement imparts L12‐Pt3Mn with a Pt d‐band center lower than that of L10‐PtMn, consequently attenuating the adsorption of strongly bonded *O intermediates during the rate‐determining step. This study not only employs a straightforward method for intermetallic preparation but also elucidates the discrepancies in ORR activity across intermetallics with distinct structures.

Electro-oxidation of persistent organic contaminants at graphene sponge electrodes using intermittent current

Borophene (Bph) and hexagonal boron nitride (hBN)-modified graphene sponge anode coupled to N-doped graphene sponge cathode were applied for electrochemical degradation of persistent organic contaminants using intermittent current. Three different ON-OFF pulse cycles were tested using low-conductivity supporting electrolyte in flow-through mode. Functionalization of the reduced graphene oxide (RGO) with Bph and hBN improved the ability of the double layer to store electrical charge, thus maintaining the generation of H2O2, O3, and ·OH even during the OFF cycles. Both anodes tested showed enhanced contaminant removal during shorter OFF periods (e.g. 52.5 s/52.s and 75 s/30 s ON/OFF), due to the improved retention of anode charge during the shorter OFF stages. Electrochemical removal of the target contaminants required 24 kWh m−3 in continuous current mode for both hBN-RGO and Bph-RGO anodes at 231 A/m−2, which was lowered to 11.7 and 13.5 kWh m−3 respectively, using ON-OFF pulse cycles. Electrochemical degradation pathways were elucidated in both systems using carbamazepine as a representative persistent contaminant. Flow-through reactors with both Bph- and hBN-RGO anodes removed ≥60 % of the target contaminants in a single pass using continuous current, whereas intermittent current led to somewhat decreased removal efficiencies (43–58 %) due to the scavenging effect of the wastewater matrix. Thus, halving the current ON time led to less than 20 % decrease in the removal efficiencies due to the capacitive properties of RGO. Given that switching to intermittent current decreased the energy consumption from 9.3 kWh m−3 to 4.4 kWh m−3 (Bph-RGO anode) and from 6.9 kWh m−3 to 3.6 kWh m−3 (hBN-RGO anode), higher removal of the target contaminants can be achieved by coupling sequential reactors in the intermittent current mode.

Enhancing polarization retention in BiFeO3 domain wall nanodevices through controlled space charge redistribution

Ferroelectric thin films with binary switchable polarization offer promising applications in domain wall (DW) memory. However, achieving reliable polarization retention in size-reduced devices remains challenging. In this study, we present a planar ferroelectric BiFeO3 DW nanodevice demonstrating stable polarization retention through electrical cycling. By precisely controlling the device size, including the width and gap of planar Pt electrodes, we observed a back-switching process in switched polarization within 20 min, as characterized by ex-situ piezoresponse force microscopy (PFM). To overcome this issue, long-time alternating voltage pulse cycling effectively suppressed the back-switching behavior, leading to symmetrized polarization coercive voltages of the device. PFM characterization further confirmed the persistence of the artificially created DW between the electrode pair. This improved polarization retention was attributed to the migration of mobile charged defects, such as oxygen vacancies, at the domain boundary. The presence of these defects generated a local built-in field, which screened the net polarization induced by the charged DW. Upon erasing the DW, the local built-in field gradually dissipated during opposite voltage poling, resulting in restored poor polarization retention and asymmetric coercive voltage in the nanodevices. This work presents a promising approach to utilize defect redistribution for stabilizing the switched polarization in the development of high-density ferroelectric DW memory.

Ionotronic WS2 memtransistors for 6-bit storage and neuromorphic adaptation at high temperature

Inspired by massive parallelism, an increase in internet-of-things devices, robust computation, and Big-data, the upsurge research in building multi-bit mem-transistors is ever-augmenting with different materials, mechanisms, and state-of-the-art architectures. Herein, we demonstrate monolayer WS2-based functional mem-transistor devices which address nonvolatility and synaptic operations at high temperature. The ionotronic memory devices based on WS2 exhibit reverse hysteresis with memory windows larger than 25 V, and extinction ratio greater than 106. The mem-transistors show stable retention and endurance greater than 100 sweep cycles and 400 pulse cycles in addition to 6-bit (64 distinct nonvolatile storage levels) pulse-programmable memory features ranging over six orders of current magnitudes (10−12–10−6 A). The origin of the multi-bit states is attributed to the carrier dynamics under electrostatic doping fluctuations induced by mobile ions, which is illustrated by employing a fingerprint mechanism including band-bending pictures. The credibility of all the storage states is confirmed by obtaining reliable signal-to-noise ratios. We also demonstrate key neuromorphic behaviors, such as synaptic plasticity, near linear potentiation, and depression, rendering it suitable for successful implementation in high temperature neuromorphic computing. Furthermore, artificial neural network simulations based on the conductance weight update characteristics of the proposed ionotronic mem-transistors are performed to explore the potency for accurate image recognition. Our findings showcase a different class of thermally aided memories based on 2D semiconductors unlocking promising avenues for high temperature memory applications in demanding electronics and forthcoming neuromorphic computing technologies.

Enhancing diffuse correlation spectroscopy pulsatile cerebral blood flow signal with near-infrared spectroscopy photoplethysmography.

Combining near-infrared spectroscopy (NIRS) and diffuse correlation spectroscopy (DCS) allows for quantifying cerebral blood volume, flow, and oxygenation changes continuously and non-invasively. As recently shown, the DCS pulsatile cerebral blood flow index () can be used to quantify critical closing pressure (CrCP) and cerebrovascular resistance (). Although current DCS technology allows for reliable monitoring of the slow hemodynamic changes, resolving pulsatile blood flow at large source-detector separations, which is needed to ensure cerebral sensitivity, is challenging because of its low signal-to-noise ratio (SNR). Cardiac-gated averaging of several arterial pulse cycles is required to obtain a meaningful waveform. Taking advantage of the high SNR of NIRS, we demonstrate a method that uses the NIRS photoplethysmography (NIRS-PPG) pulsatile signal to model DCS , reducing the coefficient of variation of the recovered pulsatile waveform () and allowing for an unprecedented temporal resolution (266Hz) at a large source-detector separation (). In 10 healthy subjects, we verified the quality of the NIRS-PPG during common tasks, showing high fidelity against ( ). We recovered CrCP and at 0.25Hz, times faster than previously achieved with DCS. NIRS-PPG improves DCS SNR, reducing the number of gate-averaged heartbeats required to recover CrCP and .

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Copper (Cu) metal nanoparticles were deposited onto FTO glass using the electrodeposition method. The precursor used was CuSO4×5H2O with Na2SO4 as the inorganic additive. The formation of Cu was characterized using field emission scanning electron microscopy (FESEM), energy-dispersive X-ray spectroscopy (EDX), and X-ray diffraction (XRD). This study investigated the impacts of the electrodeposition method (direct electrodeposition vs. pulse electrodeposition), voltages (‑0.4 V and ‑0.8 V), electrodeposition time (60s to 900s) and pulse cycles (50 cycles to 300 cycles), and FTO etching (fixed to 20s etching) towards the morphology and adhesion of Cu deposited. The grain size and thickness of Cu deposited vary with deposition time and pulse cycles. The voltage of -0.4 V successfully deposits shiny, metallic brown Cu onto FTO glass. Meanwhile, the voltage of -0.8 V gives powdery brown Cu on the surface. In addition, compared to direct electrodeposition (DD), pulse electrodeposition (PD) provides a more compact and homogeneous coverage of Cu onto FTO glass. The tape-test results also indicate that FTO etching by electrolysis reduction can improve the adhesion strength between deposited thin Cu film and the FTO glass. This work demonstrates a facile electrodeposition technique with substrate etching as an effective deposition of Cu metal with the potential for application in a wide range of fields.

Enhanced Long‐Term Memory Properties of ZnO Nanoparticle‐Based Optical Synaptic Devices for Neuromorphic Computing

The enhancement of long‐term memory properties in optical synaptic devices based on ZnO nanoparticles (NPs) is investigated. High‐temperature annealing improves crystal quality and carrier mobility, leading to efficient carrier generation and transport. The annealed ZnO NPs exhibit increased band edge luminescence and reduced deep‐level emission. Their larger surface grain size decreases oxygen adsorption, resulting in enhanced desorption by photoexcited carriers during UV exposure. The annealed devices show higher excitatory postsynaptic currents (EPSCs) and slower decay rates after UV termination, indicating better long‐term memory. They also demonstrate accelerated learning processes with fewer pulse cycles required to reach 100% EPSC. Overall, this research highlights the significance of high‐temperature annealing for improving long‐term memory in ZnO NP‐based optical synaptic devices, offering insights for advanced memory devices.

Physical design and performance research of two counter-rotating T0 choppers for the multi-physics neutron diffractometer at China Spallation Neutron Source

The T0 chopper has the ability to remove the fast neutrons and high-energy gamma rays emitted at time zero of each pulse cycle. The multi-physics instrument of the China Spallation Neutron Source requires high epithermal neutron flux to obtain large momentum transfer, and the traditional single T0 chopper is a disadvantage for the transmission of epithermal neutrons in the long focusing guide. To solve this problem, the two counter-rotating T0 chopper design is proposed that can greatly improve the transmission efficiency of epithermal neutrons. The results of the beam experiment show that compared with the single T0 chopper operating at 50 Hz, the two counter-rotating T0 choppers at the same speed significantly improves the transmission efficiency of epithermal neutrons (especially the shorter wavelength neutrons). For example, when the two blades partially overlap, the transmission efficiencies of 0.05 Å, 0.1 Å, and 0.2 Å wavelength neutrons are increased by 9.4, 4.7, and 4.6 times, respectively, which fully proves that the two counter-rotating T0 chopper design is reasonable, and the experimental results are in line with expectations. The design and application of two counter-rotating T0 choppers at the China Spallation Neutron Source is the first example of this in the world and can be applied to neutron spectrometers with high epithermal neutron flux requirements, and can also be extended to fields such as the energy selection of high-energy particles.

Degradation of flat-tube solid oxide electrolytic stack for co-electrolysis of H2O and CO2 under pulsed current

The coupling of CO2 electrolysis and renewable energy storage is of great significance, especially to CO2 capture and utilization. In this work, the factors influencing the performance and degradation of flat-tube solid oxide electrolytic cell stack (SOEC stack) for CO2/H2O co-electrolysis under an intermittent pulsed current are investigated by inserting a voltage lead inside the SOEC stack to monitor the variations in the cell and stack voltages during the electrolysis process. The results show that after 64 pulsed electrolysis cycles (900 h), the average voltage degradation rate is about 0.018%/cycle at 50–250 mA/cm2, and the useful life is expected to reach more than 1100 cycles (10,000 h). The microstructural analysis shows that a SrCrO4 barrier layer is formed on the contact surface between the metal interconnect and the current collecting layer of the cell, which increases the interface resistance of the metal interconnect and the cell, resulting in the degradation of the electrolytic performance. This study provides useful information for improving the stability of the SOEC stack for CO2/H2O co-electrolysis.

Highly Efficient Electrochemical Oxidation of Carbamazepine Using a Novel Graphene Nanoplatelet-doped PbO2 Electrode: Characteristics, Efficiency, and Mechanism

A novel graphene nanoplatelet (GN)-doped PbO2 electrode was fabricated and utilized to pulse electrochemical oxidize carbamazepine (CBZ) in aquesous solution. The GN-PbO2 electrode differed from a pure PbO2 electrode in that it exhibited higher surface roughness, smaller particle size, larger specific surface area, greater oxidation peak current, smaller charge transfer resistance, and higher oxygen evolution potential. After electrolysis for 90 min, 94.74% of CBZ and 45.15% of chemical oxygen demand could be removed at an initial pH of 3, pulsed frequency of 3000 Hz, current density of 20 mA cm−2, and pulsed duty cycle of 50%. Additionally, the primary electrochemical oxidation mechanism at the GN-PbO2 anode was indirect radical oxidation and the degradation pathway of CBZ in pulsed electrochemical oxidation was investigated and clarified considering the identified intermediate products and theoretical computations. The results demonstrate that pulsed electrochemical oxidation based on GN-PbO2 electrodes is a promising approach to increasing the viability of pharmaceutical wastewater treatment by electrochemical technologies.