Lead Dioxide Electrode Research Articles

Three-dimensional-electrode Electrochemical Oxidation of Refractory Organic Matter in a Cold High-altitude Area: A Case Study of Dibutyl Phthalate

Qinghai has a high altitude, low average temperature and low oxygen concentration, but it has abundant power resources, so it has a good application prospect to use electrochemical oxidation to degrade refractory organic matter. In this study, a three-dimensional electrode electrochemical oxidation system was constructed with powdered activated carbon as the particle electrode, graphite as the anode and stainless steel as the cathode, and the electrochemical oxidation degradation effect of DBP simulated wastewater at high altitude was studied. When applying the system to the simulated wastewater, the maximum chemical oxygen demand (COD) removal rate reached 61.75% at a plate spacing of 5 cm, electrolyte and particle-electrode dosages of 12 g and 35 g, respectively, and an electrolytic voltage of 20 V. Electrolyte voltage is the most influential factor in the COD removal rate, followed by plate spacing, electrolyte dosage, and particle electrode dosage. The graphite electrode was confirmed to be higher-value than ruthenium–iridium, titanium mesh, and lead dioxide electrodes.

Photoelectrocatalysis degradation of P-aminophenol using PbO2-TiO2 heterojunction electrode: Catalytic, theoretical calculating and mechanism

To lengthen the lifetime and extend the potential commercial applications of lead dioxide electrode. Herein, PbO2–TiO2 heterostructured electrodes were fabricated via direct current electrodeposition and the surface of the electrode was characterized by electron microscopy (EDS), X-ray diffraction (XRD) and scanning electron microscopy (SEM). The PbO2–TiO2 heterostructure electrode could produce an obvious photocurrent under UV irradiation, indicating a photoelectrocatalytic reaction. The PbO2–TiO2 heterostructured electrode was examined using density functional theory calculations(DFT). Work function(WF) confirmed that the applied electric field is conducive to the movement of photoelectrons, which promotes the photoelectrocatalysis effect. The nudged elastic band(NEB) results showed that the PbO2–TiO2 heterostructure electrode can promote the formation of •OH by reducing the activation barrier. The PbO2–TiO2 electrode was used as an anode to treat P-aminophenol (PAP) wastewater simulated wastewater and real PAP wastewater via photoelectrocatalytic degradation. The PbO2–TiO2 electrode effectively removes chemical oxygen demand (COD) from actual wastewater was 54.93 %,The after-treated Pb2+ concentration (0.037 mg·L−1) was lower than China’s wastewater discharge standard (1 mg·L−1). Finally, the degradation pathway of PAP was determined based on the intermediates detected using gas chromatography–mass spectrometry and the reactive sites of PAP were predicted using the Fukui function.These results suggest that the photoelectrocatalysis degradation of PAP using electrodes is feasible.

Effect of bismuth doping on electrodeposition, physicochemical properties and electrocatalytic activity of lead dioxide electrodes

The bismuth (Bi)-doped PbO2 electrodes were electrodeposited from a nitric plating solution containing Pb (II) and Bi (III) ions by varying the concentrations of Bi (III). Cyclic voltammetry was used to investigate the effect of Bi (III) ions on the kinetics of PbO2 electrodeposition. It is observed that increasing Bi (III) ions in the plating solution reduces the rate of nucleation or formation of PbO2 but does not change the process mechanism. X-ray diffraction confirms that the incorporation of bismuth results in an apparent β (301) texture. Scanning electron microscopic observation reveals that the size of the PbO2-deposit particles gradually decreases by several micrometers as the doping content of Bi (III) increases from 2 to 6 mM. Linear scanning voltammograms show that the oxygen overpotential on Bi-PbO2 is much higher than on undoped PbO2 electrodes. Electrochemical degradation of the target pollutant was performed, and HPLC analysis demonstrated that Bi doping significantly improves the electrocatalytic ability of PbO2 electrodes.

Fabrication and characterization of a novel multilayer heterojunction Si3N4-PbO2 nanocomposite electrode and its application on electrocatalysis degradation of sulfathiazole

To lengthen the lifetime and extend the potential commercial applications of lead dioxide electrode, herein, a novel multilayer heterojunction Ti/ SnO2-Sb2O3/ graphene oxide/ carbon nanotube/ Si3N4-PbO2 electrode (Si3N4-PbO2 electrode) was fabricated by co-electrodeposition process that doping Si3N4 nanoparticles in eletroplating solution. Various spectroscopic and microscopic techniques, including scanning electron microscopy (SEM) equipped with energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), were employed to characterize the surface of the fabricated electrode. The EDS analysis confirmed the successful attachment of 5.49 %wt Si and 2.46 %wt N elements from Si3N4 nanoparticles onto the PbO2 surface, while the XRD results indicated a shift in the preferred orientation of PbO2 grains from β(110) to β(101). The water adsorption energy and ·OH desorption energy in the electrocatalysis process were determined to be 0.71 eV and 0.241 eV through theoretical calculating. Subsequently, the Si3N4-PbO2 electrode was employed as an anode for the electrocatalytic degradation of sulfathiazole-simulated wastewater and real sulfonamides wastewater. Under optimized conditions determined via response surface methodology (RSM), the COD degradation efficiency reached 69.37 % for sulfathiazole and 62.35 % for real sulfonamides wastewater. The final COD concentration of the real sulfonamides wastewater was reduced to 77.05 mg/L, under the national urban sewage discharge standard. Finally, the degradation mechanism and pathway of sulfathiazole has been arranged based on the electron spin resonance (ESR), cyclic voltammetry (CV), while the intermediates were detected by Gas Chromatography-Mass Spectrometer (GC-MS) and the reactive sites of sulfathiazole were predicted by using Fukui function.

Phosphoric Acid Activation of Titanium-Supported Lead Dioxide Electrodes for Bipolar Battery Applications

Titanium foil coated with doped tin dioxide is an attractive option for the positive current collector interface of bipolar lead batteries due its corrosion resistance and mechanical performance. The phosphoric acid and two of its derivatives, one inorganic (calcium hydrogen phosphate) and one organic (poly-vinylphosphonic acid), have been studied as additives with potential for improvement of the capacity retention of such positive electrodes. The results show that the jar-formation process of the electrodes in the sulfuric acid electrolyte containing phosphoric acid successfully overcomes the capacity retention problem at all studied cases. This leads also to considerable improvement of the lead dioxide utilization. The cycling ageing of the electrodes combined with periodic impedance spectroscopy measurements, indicate progressive capacity loss corresponding to the typical processes of degradation of the lead dioxide structure. Rather small changes in the electrode resistance prove the corrosion and the passivation resistance of the current collectors. It is concluded that the combined doping with phosphoric acid species in the electrolyte and in the positive paste offers a potential for further improvements of the electrodes cyclability.

Electrocatalytic Degradation of Acyclovir by Three-Dimensional Porous Lead Dioxide Anodes: Condition Optimization, Kinetic Analysis and Degradation Mechanisms

A three-dimensional porous lead dioxide electrode (3D-PbO2) was developed by the template electrodeposition approach. Polystyrene microspheres were prepared by microemulsion polymerization, and then the polystyrene template was loaded on the PbO2 electrode by electrodeposition. Finally, a porous structure was formed by removing the template. Under these optimized conditions, the degradation of acyclovir could achieve complete removal, while the removal of COD was 29.59%. The electrochemical degradation process of acyclovir was consistent with the proposed primary reaction kinetics. The 3D-PbO2 electrode was comprehensively characterized using SEM, XRD, and XPS techniques. The SEM analysis revealed the presence of well-defined porous structures on the electrode surface, while the XRD results indicated a reduction in electrode crystal sizes. Additionally, the XPS analysis demonstrated a higher proportion of reactive oxygen species on the 3D-PbO2 electrode. The electrochemical properties of the electrode were investigated using CV and EIS. The experimental findings demonstrate that the 3D-PbO2 electrode exhibits a higher oxygen evolution potential and lower charge transfer resistance than the conventional PbO2 electrode. This study presents a viable approach to enhance the electrochemical oxidation performance of lead dioxide.

Stable acidic water oxidation by tunable electronic states in β-PbO2 anode electrocatalyst aided by incorporation of various anions and cations

Developing stable and cost-effective electrodes is one of the main challenges of clean hydrogen fuel production. However, the investigation of non-precious materials for this application, from both experimental and theoretical aspects, has been limited in scope. In the present research, the lead dioxide (β-PbO2) electrode was prepared by an anodic electrodeposition method on Ti substrate to use as the anode in electrochemical water splitting cells, where the oxygen evolution half-reaction occurs. The substitution of F– anion and Fe3+ and Co2+ cations into the structure of lead dioxide, to improve the properties and performance of these anodes, was investigated through a combination of experimental studies and quantum mechanical (QM) calculations. The β-PbO2, β-PbO2-F, β-PbO2-Fe, and β-PbO2-Co electrodes were characterized by the XRD, SEM, EDS, and electrochemical analyses, including CV, LSV, CP, and EIS. Furthermore, the electrode structures were investigated in theoretical studies by the density functional theory (DFT) method. The Gibbs energy change of intermediates formation and electronic properties, including band structure, the density of states, and charge density difference, were calculated and studied. The results showed that the substitutional elements improved the PbO2 activity toward oxygen evolution reaction (OER) by reducing the intermediates' adsorption resistance from 84.2 in pure PbO2 to 11.7 Ω.cm2 in PbO2-Fe. Fe3+ substitution had the most effect on durability and increased the efficient lifetime of the anode about 4 times relative to pure PbO2. The electrochemically active surface area (ECSA) was also increased intensively by doping Fe3+. It is concluded from the DFT calculations that the reaction energy barriers are reduced by ion incorporation. The OER overpotential decreases significantly from 920 mV on pure PbO2 surface to 350 mV by Co2+ substitution. The enhancement of the intrinsic activity of cation-substituted anodes was evidenced by the remarkable reduction of band gap energy at the Fermi level.

Efficient recovery and treatment of actual electroplating wastewater using stable electrocatalyst-coupled super-stable mineralizer

Electroplating plays an indispensable and pivotal role in various aspects of industrial production, but its wastewater contains a large number of heavy metal ions, resulting in huge discharge pressure. The recovery of metals in wastewater, while meeting discharge standards, has become an urgent issue that requires a simple and efficient solution. In this work, a stable electrocatalyst-coupled with super-stable mineralizer structure has been developed for the recycling and treatment of wastewater. Using actual high-concentration copper electroplating wastewater (5330 mg/L) as a model, we successfully recovered 91.1 % copper by electrolysis process using a low-cost and stable lead dioxide electrode. Following the addition of a super-stable mineralization treatment utilizing layered double hydroxides (LDHs), the resultant pollution water successfully attained the prescribed threshold, specifically below 0.5 mg/L for Cu2+, with reduction of about 90 % of hazardous waste sludge. This new method of recycling heavy metals from wastewater is expected to be both environmentally friendly and sustainable, while also being cost-effective and efficient.

CMS and Nd Co-Modified PbO2 Electrodes with Enhanced Lifetime and Electrochemical Activity for the Degradation of Bisphenol S

In this study, a lead dioxide electrode co-modified with carbon microspheres and neodymium (CMS-Nd-PbO2) was prepared. The structural morphology and electrochemical properties of the four electrodes, PbO2, CMS-PbO2, Nd-PbO2, and CMS-Nd-PbO2, were compared by field emission scanning electron microscopy, X-ray diffractometer, X-ray photoelectron spectroscopy, cyclic voltammetry, and electrochemical impedance, respectively. The results showed that the prepared CMS-Nd-PbO2 electrode had higher surface denseness and higher electrode activity. Based on the accelerated lifetime experiment, the actual working life of four electrodes was studied, and the CMS-Nd-PbO2 electrode had a relatively long lifetime, increased 24.60% compared with the PbO2 electrode. The influencing parameters of electrochemical degradation of bisphenol S (BPS) by CMS-Nd-PbO2 electrode, the ability of different electrodes to generate hydroxyl radicals, reaction mechanism, and the possible BPS degradation pathways were also discussed. Further, the safety of the prepared electrode was evaluated. Under the optimal parameters, the removal rate of BPS and chemical oxygen demand (COD) were 96.49% and 51.84%, respectively. The dissolved lead ion concentration in the solution after electrochemical oxidation was lower than the WHO standard. The CMS-Nd-PbO2 electrode showed promising applications in the degradation of emerging contaminants wastewater.

Влияние ультразвука на кинетику электроосаждения диоксида свинца на стальную основу и свойства покрытия

The influence of the ultrasonic field on lead dioxide electrodeposition from nitrate electrolyte was studied. The adsorption of electroactive particles and the amount of nucleation on the electrode surface were found to have increased as well as the formation of OH-radicals accelerated under the influence of the ultrasonic field. Fine-crystalline deposits of lead dioxide were formed, which contributed to obtaining high current yield of lead dioxide, coefficient increasing of the electrode active mass and increasing of the discharge capacity of the emergency current generator cell layout. It was shown that the application of ultrasound in producing a lead dioxide electrode made it possible to reduce the time of the technological procedure.

Crystal facet controlled stable PbO2 electrode for efficient degradation of tetracycline

• The robust PbO 2 electrodes had high onset potential. • The crystal plane strategy was adopted to modify the PbO 2 surface structure. • The modified electrode improved electrode life and reduced lead dissolution. • The modified electrode achieved efficient degradation of tetracycline wastewater. Achieving the robust PbO 2 electrode with the high onset potential is of considerable importance for applying electrochemical pollutants degradation. Herein, the crystal plane strategy was adopted to modify the PbO 2 surface structure through the surfactant induction during synthesis in the electrodeposition process. PbO 2 (β(3 0 1)) and PbO 2 (α(2 0 0), β(3 0 1)) electrodes were obtained by the controlling conditions of surfactants sodium dodecyl sulfate (SDS) and hexadecyl trimethyl ammonium bromide (CTAB). Compared with conventional PbO 2 , the PbO 2 (CTAB) electrode exhibits outstanding performance in electrochemical stability and higher onset potential versus the PbO 2 (SDS). Accelerated life of the PbO 2 (CTAB) electrode is 147 h longer than that of the pure PbO 2 under a high current density of 1A·cm −2 , and the amount of lead ion dissolution is only 45% of that observed in pure PbO 2 . In this work, tetracycline (TC) was taken as an example to evaluate the degradation effect of electrodes. Due to its unique crystal texture, the PbO 2 (CTAB) electrode exhibits higher COD removal rate and TOC removal rate, 35% and 20% respectively beyond that of the conventional lead dioxide electrode. Therefore, it is of great value for its industrial electrode degradation of pollutants.

Electrocatalytic Degradation of Crystal Violet by a Lead Dioxide Electrode: Operation Parameters and Degradation Mechanism

Electrocatalytic Degradation of Crystal Violet by a Lead Dioxide Electrode: Operation Parameters and Degradation Mechanism

Recent developments of lead dioxide electrodes electrodeposited from methanesulfonate electrolytes

Lead dioxide (PbO[Formula: see text] electrodes have been actively studied since their large-scale application in energy storage industries in the late 20th century. In modern industry, PbO2 electrodes are anodically electrodeposited from the oxidizing and toxic chloride and nitrate systems. In recent studies, the PbO2 electrodeposition from methanesulfonate medium is widely proposed owing to the large ion solubility and environmental friendliness. The further developments in PbO2 electrodeposited from methanesulfonate electrolytic system is now becoming increasingly important and its future scale-up applications could be envisaged. In this regard, this review illustrates the recent developments of lead dioxide electrodes prepared from methanesulfonate electrolytes.

Electrocatalysis degradation of coal tar wastewater using a novel hydrophobic benzalacetone modified lead dioxide electrode

Coal tar wastewater is hard to degrade by traditional methods because of its toxic pollutant constituents and high concentration of aromatic hydrocarbons, especially phenolic substances. A new type of hydrophobic benzacetone modified PbO2 anode (BA-PbO2 electrodes) was used for the electrocatalytic treatment of coal tar wastewater in a continuous cycle reactor. The surface morphology, structure, valences of elements, hydrophobicity, hydroxyl radical (·OH) produced capacity, electrochemical properties and stability of BA-PbO2 electrodes were characterized by SEM (scanning electron microscopy), XRD (X-ray diffraction), XPS (X-ray photoelectron spectroscopy), contact angle, a fluorescence probe test, an electrochemical workstation and accelerated life test, respectively. The BA-PbO2 electrodes exhibited a compact structure and finely dispersed crystallize size of 4.6 nm. The optimum degradation conditions of coal tar wastewater were as follows: current density of 90 mA cm−2, electrode gap of 1 cm and temperature at 25 °C with flow velocity of 80 L h−1. The chemical oxygen demand (COD) removal efficiency reached 92.39% after 240 min of degradation under the optimized conditions and the after-treatment COD value was 379.51 mg L−1 which was lower than the centralized emission standard (less than 400 mg L−1). These findings demonstrated the feasibility and efficiency of electrocatalytically degrading coal tar wastewater by BA-PbO2 electrodes. The possible mechanism and pathway for phenol a specific pollutant in coal tar wastewater were investigated by quantum chemistry calculations (Multiwfn) and gas chromatography-mass spectrometry (GC-MS). The toxicity of each intermediate was predicted by the ECOSAR program.

Controllable Preparation of a Three-Dimensional Porous Lead Dioxide Electrode with an Oxygen Bubble Template and Its Electrocatalytic Performance

Controllable Preparation of a Three-Dimensional Porous Lead Dioxide Electrode with an Oxygen Bubble Template and Its Electrocatalytic Performance

Fabrication of a multi-layer CNT-PbO2 anode for the degradation of isoniazid: Kinetics and mechanism

In this study, the CNTs were successfully compounded in PbO2 electrode through composite electrodeposition technology to obtain multi-layer CNT-PbO2 electrode. Scanning electron microscope, X-ray diffraction and X-ray Photoelectron Spectroscopy were comprehensively used to characterize the lead dioxide electrode and the electrochemical performance were also tested by cyclic voltammetry, and electrochemical impedance spectroscopy. Results showed that CNT-PbO2 significantly improved the electrochemical performance, which was attributed to that the compound of CNTs in PbO2 improved the active sites on the surface, with higher oxidation peaks, smaller particle size, larger specific surface area, and lower charge transfer resistance. In the degradation experiment, the chemical oxygen demand removal efficiency of isoniazid by CNT-PbO2 electrode were 1.37 times of that by pure PbO2 electrode. The main influence factors on the degradation of ISN, such as initial ISN concentration, Na2SO4 concentration, current density and initial pH value was analyzed in detail. Considered comprehensively the effects of ISN removal efficiency, COD and average current efficiency, the degradation of ISN and COD reached 99.4% and 86.8%, respectively, after the electrode was degraded by electrochemical oxidation for 120 min under the best conditions. In addition, the degradation mechanism of ISN in electrochemical oxidation was studied. According to the intermediate products detected by GC-MS, the possible degradation pathway of ISN in electrochemical oxidation system were proposed.

Facile fabricate of F-doped lead dioxide electrode coating onto porous 3D titanium plate for advanced lead-carbon hybrid capacitor

Lead-carbon hybrid capacitor has been widely used in hybrid electrical vehicle, uninterruptible power supply, smart grid and other fields, with low prices, stable performance at high-low temperature and good security. However, it is difficult for lead-carbon hybrid capacitors to meet the requirements of high-performance electrochemical energy storage devices because the effective availability of the positive active materials is relatively low and the cycle life of this hybrid capacitor is also unsatisfactory. In this study, a 3D-Ti/SnO2-Sb2O5/F-PbO2 electrode was prepared in the co-electrodeposition method. The F doping in the corner of the PbO2 crystal is beneficial for the morphological transformation from enormous columnar to planar special structure, which can enhance the cycling stability and energy density. The lead-carbon hybrid capacitor with optimized F-PbO2 electrode electrodeposited at 1.50 V has high energy density (133 mAh g−1 at 1 mA cm−2) and excellent cycling stability (98.8% of original capacitance after 1000 cycles).

Electrochemical degradation of vanillin using lead dioxide electrode: influencing factors and reaction pathways

ABSTRACT In this study, a novel PbO2-CeO2 composite electrode was applied it to the electrocatalytic degradation of vanillin. The operating parameters such as applied current density, initial vanillin concentration, supporting electrolyte concentration and pH value were investigated and optimised. After 120 min, in a 0.10 mol L−1 Na2SO4 solution with a current density of 50 mA cm−2 and a pH value of 5.0 containing 30 mg L−1 vanillin, the vanillin removal efficiency can reach 98.03%, the COD removal efficiency is up to 73.28%. The results indicate that electrochemical degradation has a high ability to remove vanillin in aqueous solution. The reaction follows a pseudo-first-order reaction kinetics model with rate constants of 0.03036 min−1. In the process of electrochemical degradation, up to eight hydroxylated or polyhydroxylated oxidation by-products were identified through hydroxylation, dealkylation and substitution reactions. Furthermore, the degradation pathways were proposed, which eventually mineralised into inorganic water and carbon dioxide.

Fabrication and characterization of titanium-based lead dioxide electrode by electrochemical deposition with Ti4 O7 particles.

A novelly modified Ti/PbO2 electrode was synthesized with Ti4 O7 particles through electrochemical deposition method (marked as PbO2 -Ti4 O7 ). The properties of the as-prepared electrodes were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), linear sweep voltammetry (LSV), electrochemical impedance spectroscopy (EIS), hydroxyl radical concentration, accelerated life test, etc. Azophloxine was chosen as the model pollutant for electro-catalytic oxidation to evaluate electrochemical activity of the electrode. The experimental results indicated that Ti4 O7 modification could prominently improve the properties of the electrodes, especially, improve the surface morphology, enhance the current response, and reduce the impedance. However, the predominant phases of PbO2 electrodes were unchanged, which were completely pure β-PbO2 . During the electrochemical oxidation process, the PbO2 -Ti4 O7 (1.0) electrode showed the best performance on degradation of AR1 (i.e., the highest removal efficiency and the lowest energy consumption), which could be attributed to its high oxygen evolution potential (OEP) and strong capability of HO· generation. Moreover, the accelerated service lifetime of PbO2 -Ti4 O7 (1.0) electrode was 175hr, 1.65 times longer than that of PbO2 electrode (105.5hr). PRACTITIONER POINTS: PbO2 /Ti4 O7 composite anode was fabricated through electrochemical co-deposition. Four concentration gradients of Ti4 O7 particle were tested. PbO2 -Ti4 O7 (1.0) showed optimal electrocatalytic ability due to its high OEP and HO· productivity.

Study of simultaneously electrodepositing α/β-PbO2 coating materials in methanesulfonic acid and its application in novel flow battery

Abstract In the present work, a novel Pb-0.6%Sb/α-PbO2/β-PbO2 composite electrode with quantitatively phases of α or β-PbO2 was obtained by electrodeposition in methanesulfonic acid (MSA) and further investigated in novel flow battery. The physicochemical properties of lead dioxide were analyzed by anodic polarization curves, X-ray powder diffraction (XRD), scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS) and Tafel curves. Results showed that the selection of temperature ranges was found to cause a quantitative difference in the formation of α/β-PbO2 phases, as it made interval effects on the overpotential that was the primary control condition to affect transfer proces.The precise conditions of obtaining α or β-PbO2 phases by varying temperatures were confirmed and samples were prepared to be tested in long-period galvanostatic electrolysis. By comparing, the electrode (deposition time-α&β: 2 h&2 h) showed the best physicochemical properties, which could effectively improve the energy storage and extend the lifetime (63.6 h) compared with the traditional lead dioxide electrodes (24.5 h) in novel flow battery.