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1.
J Colloid Interface Sci ; 677(Pt B): 331-341, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39151226

ABSTRACT

Anchoring Pt onto multi-heteroatom doped carbon materials has been recognized as an effective approach to improve the performance of electrocatalytic methanol oxidation. However, distinct contributions and specific behavior mechanisms of different heteroatoms, notably N and P, the specific behavior mechanisms in synergistically promoting Pt NPs remain elusive. In this work, we construct 1D N and P co-doped carbon nanotube (N, P-CNTs) supports with abundant defect anchors for Pt. The as-prepared Pt/N, P-CNTs exhibit outstanding activity and exceptional stability in methanol oxidation reaction (MOR), achieving high mass activity up to 6481.3 mA mg-1Pt. Moreover, they can retain 90.5 % of their initial current density even after 800 cycles tests. Detailed characterizations and theoretical calculations indicate that the robust strong metal-support interactions (SMSI) effect caused by N doping within the unique N and P co-doped coordination structure controllably regulate the coordination environment of Pt, reduce the d-band center of Pt, thus promoting the adsorption and decomposition of CH3OH. However, P doping weakens the adsorption strength of CO on the Pt active site by sacrificing partial electron transfer, accelerating the oxidative conversion of the CO-like poisoning species (COads). Significantly, the synergistic mechanism of N and P species on the modification of Pt's electronic structure and its subsequent impact on the electrocatalytic methanol oxidation behaviors on the Pt surface was thoroughly elucidated, providing a constructive route for designing robust MOR electrocatalysts with high MOR activity and durability.

2.
J Colloid Interface Sci ; 677(Pt A): 416-424, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39096709

ABSTRACT

Surface strain engineering has proven to be an efficient strategy to enhance catalytic properties of platinum (Pt)-based catalysts for electrooxidation reactions. Herein, the S-doped PtMn concave cubes (CNCs) enclosed with high index facets (HIFs) and regulatable surface strain are successfully fabricated by two steps hydrothermal method. The S element with electrophilic property can modify the near-surface of PtMn nanocrystals, altering the electronic structure of Pt to effectively regulate the adsorption/desorption of intermediates in the ethanol electrooxidation reaction (EOR). The PtMnS1.1 catalyst with optimal surface strain delivered extraordinary catalytic performance on EOR in acidic media, with a specific activity of 2.88 mA/cm2 and mass activity of 1.10 mA/µgPt, which is 4.1 and 2.2 times larger than that of state-of-the-art Pt/C catalyst, respectively. Additionally, the PtMnS1.1 catalyst also achieve excellent catalytic properties in alkaline electrolyte for EOR. The results of kinetic studies indicated that the surface strain and modified electronic structure can degrade the activation energy barrier during the process of EOR, which is beneficial for enhance the reaction rate. This work provides a promising approach to construct highly efficient electrocatalysts with tunable surface strain effects for clean energy electro-chemical reactions.

3.
Small ; : e2406829, 2024 Oct 06.
Article in English | MEDLINE | ID: mdl-39370665

ABSTRACT

The nickel hydroxide-based (Ni(OH)2) methanol-to-formate electrooxidation reaction (MOR) performance is greatly related to the d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital electronic states. Hence, optimizing the d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital electronic states to achieve enhanced MOR activities are highly desired. Here, cobalt (Co) and iron (Fe) doping are used to modify the d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital electronic states. Although both dopants can broaden the d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital; however, Co doping leads to an elevation in the energy level of d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ highest occupied crystal orbital (HOCO), whereas Fe doping results in its reduction. Such a discrepancy in the regulation of d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital electronic states stems from the disparate partial electron transfer mechanisms amongst these transition metal ions, which possess distinct energy level and occupancy of d orbitals. Motivated by this finding, the NiCoFe hydroxide is prepared and exhibited an excellent MOR performance. The results showed that the Co dopants effectively suppress the partial electron transfer from Ni to Fe, combined with the d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital broadening induced by NiO6 octahedra distortion, endowing NiCoFe hydroxide with high d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ HOCO and broad d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital. It is believed that the work gives an in-depth understanding on d x 2 - y 2 ${{d}_{{{x}^2} - {{y}^2}}}$ orbital electronic states regulation in Ni(OH)2, which is beneficial for designing Ni(OH)2-based catalysts with high MOR performance.

4.
Biosensors (Basel) ; 14(9)2024 Sep 19.
Article in English | MEDLINE | ID: mdl-39329823

ABSTRACT

We introduce a novel dual redox mediator synthesized by covalently linking ferrocene dicarboxylic acid (FcDA) and thionine (TH) onto a pre-treated glassy carbon electrode. This unique structure significantly enhances the electro-oxidation of dopamine (DA) and the reduction of hydrogen peroxide (H2O2), offering a sensitive detection method for both analytes. The electrode exhibits exceptional sensitivity, selectivity, and stability, demonstrating potential for practical applications in biosensing. It facilitates rapid electron transfer between the analyte and the electrode surface, detecting H2O2 concentrations ranging from 1.5 to 60 µM with a limit of detection (LoD) of 0.49 µM and DA concentrations from 0.3 to 230 µM with an LoD of 0.07 µM. The electrode's performance was validated through real-sample analyses, yielding satisfactory results.


Subject(s)
Biosensing Techniques , Dopamine , Electrochemical Techniques , Electrodes , Ferrous Compounds , Hydrogen Peroxide , Metallocenes , Oxidation-Reduction , Phenothiazines , Dopamine/analysis , Ferrous Compounds/chemistry , Phenothiazines/chemistry , Metallocenes/chemistry , Limit of Detection
5.
J Environ Manage ; 370: 122638, 2024 Sep 28.
Article in English | MEDLINE | ID: mdl-39342833

ABSTRACT

The oil industry is facing substantial environmental challenges, especially in managing waste streams such as Oilfield Produced Water (OPW), which represents a significant component of the industrial ecological footprint. Conventional treatment methods often fail to effectively remove dissolved oils and grease compounds, leading to operational difficulties and incomplete remediation. Electrochemical oxidation (EO) has emerged as a promising alternative due to its operational simplicity and ability to degrade pollutants directly and indirectly, which has already been applied in treating several effluents containing organic compounds. The application of EO treatment for OPW is still in an initial stage, due to the intricate nature of this matrix and scattered information about it. This study provides a technological overview of EO technology for OPW treatment, from laboratory scale to the development of large-scale prototypes, identifying design and process parameters that can potentially permit high efficiency, applicability, and commercial deployment. Research in this domain has demonstrated notable rates of removal of recalcitrant pollutants (>90%), utilizing active and non-active electrodes. Electro-generated active species, primarily from chloride, play a pivotal role in the oxidation of organic compounds. However, the highly saline conditions in OPW hinder the complete mineralization of these organics, which can be improved by using non-active anodes and lower salinity levels. The performance of electrodes greatly influences the efficiency and effectiveness of OPW treatment. Various factors must be considered when selecting the electrode material, such as its conductivity, stability, surface area, corrosion resistance, and cost. Additionally, the specific contaminants present in the OPW, and their electrochemical reactivity must be considered to ensure optimal treatment outcomes. Balancing these considerations can be challenging, but it is crucial for achieving successful OPW treatment. Active electrode materials exhibit a high affinity for chloride molecules, generating more active species than non-active materials, which exhibit more significant degradation potential due to the production of hydroxyl radicals. Regarding scale-up, key challenges include low current efficiency, the formation of by-products, electrode deactivation, and limitations in mass transfer. To address these issues, enhanced mass transfer rates and appropriate residence times can be achieved using flow-through mesh anodes and moderate current densities, which have proven to be the optimal configuration for this process.

6.
Small ; : e2406782, 2024 Sep 30.
Article in English | MEDLINE | ID: mdl-39344630

ABSTRACT

Transforming glycerol (GLY, biodiesel by-product) into lactic acid (LA, biodegradable polymer monomer) through sustainable electrocatalysis presents an effective strategy to reduce biodiesel production costs and consequently enhance its applications. However, current research faces a trade-off between achieving industrially-relevant current density (>300 mA cm-2) and high LA selectivity (>80%), limiting technological advancement. Herein, a Au3Ag1 alloy electrocatalyst is developed that demonstrates exceptional LA selectivity (85%) under high current density (>400 mA cm-2). The current density can further reach 1022 mA cm-2 at 1.2 V versus RHE, superior to most previous reports for GLY electrooxidation. It is revealed that the Au3Ag1 alloy can enhance GLY adsorption and reactive oxygen species (OH*) generation, thereby significantly boosting activity. As a proof of concept, a homemade flow electrolyzer is constructed, achieving remarkable LA productivity of 68.9 mmol h-1 at the anode, coupled with efficient H2 production of 3.5 L h-1 at the cathode. To further unveil the practical possibilities of this technology, crude GLY extracted from peanut oil into LA is successfully transformed, while simultaneously producing H2 at the cathode. This work showcases a sustainable method for converting biodiesel waste into high-value products and hydrogen fuel, promoting the broader application of biodiesel.

7.
Article in English | MEDLINE | ID: mdl-39348016

ABSTRACT

The present research aimed to explore the durability of MMO electrodes through electro-oxidation (EO) in purifying secondary treated actual sewage wastewater using batch and pilot-scale setups. The main aim is to inactivate bacteria in sewage treatment plants before they are released into the environment, thus contaminating water and soil. Process parameters such as current density (j), NaCl dose (n), and treatment time (t) were optimized using response surface methodology in a lab-scale EO reactor under batch conditions. The results showed that optimization of current density at 5.90 mA/cm2 and NaCl concentration at 1.31 g/L led to 93.90% of bacterial inactivation (Q1) within 8 min of treatment and 0.48 kWh/m3 energy consumption (Q2). Biological analysis was conducted to validate bacterial cell destruction and count coliform bacteria in the EO-treated sewage wastewater. XRD, cyclic voltammetry studies, and FE-SEM/EDS analysis were done to confirm the MMO anode's durability and stability after 100 recycles. The study prioritized bacterial inactivation along with organic matter degradation. Besides that, a small pilot-scale study on the actual sewage wastewater with a volume of 10-50 L was done in batch mode under previously optimized conditions to analyze the efficacy of the MMO anodes in terms of bacterial inactivation.

8.
Heliyon ; 10(16): e35791, 2024 Aug 30.
Article in English | MEDLINE | ID: mdl-39220931

ABSTRACT

Nickel-iron-based spinel oxide was prepared and supported on multi-walled carbon nanotubes to enhance the electrochemical oxidation of ethylene glycol in an alkaline medium. NiFe2O4 was prepared using facile sol-gel techniques. Then the prepared material was characterized using different bulk and surface techniques like powder X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM), and transmitted electron microscope (TEM). Different electrodes of NiFe2O4/CNT ratios were prepared to find out the optimum spinel oxide/CNT ratio. The activity of the metal spinel oxides composite was characterized toward ethylene glycol conversion by different electrochemical techniques like cyclic voltammetry (CV), Chronoamperometry (CA), and electrochemical impedance spectroscopy (EIS). The modified electrode reached an oxidation current of 43 mA cm-2 in a solution of 1.0 M ethylene glycol and 1.0 M NaOH. Furthermore, some kinetics parameters (like diffusion coefficient, and rate constant) were calculated to evaluate the catalytic performance. Additionally, the electrode showed extreme stability for long-term ethylene glycol oxidation.

9.
Small ; : e2406068, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-39223867

ABSTRACT

Electrochemical upcycling of end-of-life polyethylene terephthalate (PET) using renewable electricity offers a route to generate valuable chemicals while processing plastic wastes. However, it remains a huge challenge to design an electrocatalyst with reliable structure-property relationships for PET valorization. Herein, spinel Co3O4 with rich oxygen vacancies for improved activity toward formic acid (FA) production from PET hydrolysate is reported. Experimental investigations combined with theoretical calculations reveal that incorporation of VO into Co3O4 not only promotes the generation of reactive hydroxyl species (OH*) species at adjacent tetrahedral Co2+ (Co2+ Td), but also induces an electronic structure transition from octahedral Co3+ (Co3+ Oh) to octahedral Co2+ (Co2+ Oh), which typically functions as highly-active catalytic sites for ethylene glycol (EG) chemisorption. Moreover, the enlarged Co-O covalency induced by VO facilitates the electron transfer from EG* to OH* via Co2+ Oh-O-Co2+ Td interaction and the following C─C bond cleavage via direct oxidation with a glyoxal intermediate pathway. As a result, the VO-Co3O4 catalyst exhibits a high half-cell activity for EG oxidation, with a Faradaic efficiency (91%) and productivity (1.02 mmol cm-2 h-1) of FA. Lastly, it is demonstrated that hundred gram-scale formate crystals can be produced from the real-world PET bottles via two-electrode electroreforming, with a yield of 82%.

10.
Natl Sci Rev ; 11(10): nwae271, 2024 Oct.
Article in English | MEDLINE | ID: mdl-39301081

ABSTRACT

Using the electrochemical polyol oxidation reaction (POR) to produce formic acid over nickel-based oxides/hydroxides (NiO x H y ) is an attractive strategy for the electrochemical upgrading of biomass-derived polyols. The key step in the POR, i.e. the cleavage of the C-C bond, depends on an oxygen-vacancy-induced mechanism. However, a high-energy oxygen vacancy is usually ineffective for Schottky-type oxygen-vacancy-rich ß-Ni(OH)2 (VSO-ß-Ni(OH)2). As a result, both ß-Ni(OH)2 and VSO-ß-Ni(OH)2 cannot continuously catalyze oxygen-vacancy-induced C-C bond cleavage during PORs. Here, we report a strategy of oxygen-vacancy-filling with sulfur to synthesize a ß-Ni(OH)2 (S-VO-ß-Ni(OH)2) catalyst, whose oxygen vacancies are protected by filling with sulfur atoms. During PORs over S-VO-ß-Ni(OH)2, the pre-electrooxidation-induced loss of sulfur and structural self-reconstruction cause the in-situ generation of stable Frenkel-type oxygen vacancies for activating vacancy-induced C-C bond cleavage, thus leading to excellent POR performances. This work provides an intelligent approach for guaranteeing the sustaining action of the oxygen-vacancy-induced catalytic mechanism in electrooxidation reactions.

11.
Angew Chem Int Ed Engl ; : e202414481, 2024 Sep 03.
Article in English | MEDLINE | ID: mdl-39227999

ABSTRACT

Electro-oxidation (EO) technology demonstrates significant potential in wastewater treatment. However, the high energy consumption has become a pivotal constraint hindering its large-scale implementation. Herein, we design an EO and 4-electron oxygen reduction reaction coupled system (EO-4eORR) to replace the traditional EO and hydrogen evolution reaction (HER) coupled system (EO-HER). The theoretical cathodic potential of the electrolytic reactor is tuned from 0 V (vs. RHE) in HER to 1.23 V (vs. RHE) in 4eORR, which greatly decreases the required operation voltage of the reactor. Moreover, we demonstrate that convection can improve the mass transfer of oxygen and organic pollutants in the reaction system, leading to low cathodic polarization and high pollutant removal rate. Compared with traditional EO-HER system, the energy consumption of the EO-4eORR system under air aeration for 95% total organic carbon (TOC) removal is greatly decreased to 2.61 kWh/kgTOC (only consider the electrolyzer energy consumption), which is superior to previously reported EO-based water treatment systems. The reported results in this study offer a new technical mode for development of highly efficient and sustainable EO-based treatment systems to remove organic pollutants in waste water.

12.
Water Res ; 266: 122317, 2024 Aug 29.
Article in English | MEDLINE | ID: mdl-39260192

ABSTRACT

The advanced oxidation process is an efficient technology for the degradation and detoxification of refractory organics to ensure water safety. However, most researches focus on improving pollutant degradation but overlook carbon emission and resource utilization. In this study, a flow-through electrochemical integrated system was constructed to simultaneously realize bisphenol A (BPA) oxidation into small non-toxic organics and CO2, and generated CO2 coupled with nitrate-containing wastewater conversion to urea and ammonia on a porous cathode (Zr-Fe/CN). The synergistic effect between anodic BPA oxidation with cathodic CO2 and NO3-reduction improves the electron utilization efficiency and thus increasing the BPA degradation, urea yield rate (UYR) and NH3 yield rate (NYR) by 13.4 % 18.4 % and 8.3 %, respectively. Furthermore, the flow-through operation mode significantly increased the mass transfer efficiency and quickly carried generated CO2 from the anode into the cathode to improve CO2 utilization efficiency. Compared to the parallel plate electrode reactor, the BPA degradation efficiency, UYR and NYR in the flow-through reactor increased from 59.46 % to 84.49 % (the initial concentration of BPA was 40 mg/L), 9.94 mmol h-1g-1 to 19.55 mmol h-1g-1, and 80.31 mmol h-1g-1 to 106.06 mmol h-1g-1 within 60 min, respectively. Moreover, the total carbon conversion efficiency (from BPA to urea) increased from 20.2 % to 42.4 % and the total Faraday efficiency (FE) increased from 78.6 % to 96.3 %. This work provides a multi-win strategy of harmless, resource-based and carbon emission reduction for wastewater treatment.

13.
J Colloid Interface Sci ; 678(Pt B): 153-161, 2024 Sep 03.
Article in English | MEDLINE | ID: mdl-39241446

ABSTRACT

Efficient CC bond cleavage and the complete oxidation of alcohols are key to improving the efficiency of renewable energy utilization. Herein, we successfully prepare porous Fe-doped hexagonal close-packed (hcp)-PtBi/face-centered cubic (fcc)-Pt heterostructured nanoplates with abundant grain/phase interfaces (h-PtBi/f-Pt@Fe1.7 PNPs) via a simple solvothermal method. The open porous structure, abundant grain/phase interface and stacking fault defects, and the synergistic effect between intermetallic hcp-PtBi and fcc-Pt make h-PtBi/f-Pt@Fe1.7 PNPs an effective electrocatalyst for the glycerol oxidation reaction (GOR) in direct glycerol fuel cells (DGFCs). Notably, the h-PtBi/f-Pt@Fe1.7 PNPs exhibit an excellent mass activity of 7.6 A mgPt-1 for GOR, 4.75-fold higher than that of commercial Pt black in an alkaline medium. Moreover, the h-PtBi/f-Pt@Fe1.7 PNPs achieve higher power density (125.8 mW cm-2) than commercial Pt/C (81.8 mW cm-2) in a single DGFC. The h-PtBi/f-Pt@Fe1.7 PNPs can also effectively catalyze the electrochemical oxidation of 1-propanol (17.1 A mgPt-1), 1,2-propanediol (7.2 A mgPt-1), and 1,3-propanediol (5.2 A mgPt-1). The in-situ Fourier-transform infrared spectra further reveal that the CC bond of glycerol, 1-propanol, 1,2-propanediol, and 1,3-propanediol was dissociated for the complete oxidation by the h-PtBi/f-Pt@Fe1.7 PNPs. This study provides a new class of porous Pt-based heterostructure nanoplates and insight into the intrinsic activity of different C3 alcohols.

14.
Angew Chem Int Ed Engl ; : e202408736, 2024 Aug 06.
Article in English | MEDLINE | ID: mdl-39107260

ABSTRACT

The electrooxidation of catalyst surfaces is across various electrocatalytic reactions, directly impacting their activity, stability and selectivity. Precisely characterizing the electrooxidation on well-defined surfaces is essential to understanding electrocatalytic reactions comprehensively. Herein, we employed in situ Raman spectroscopy to monitor the electrooxidation process of palladium single crystal. Our findings reveal that the Pd surface's initial electrooxidation process involves forming *OH intermediate and ClO4 - ions facilitate the deprotonation process, leading to the formation of PdOx. Subsequently, under deep electrooxidation potential range, the oxygen atoms within PdOx contribute to creating surface-bound peroxide species, ultimately resulting in oxygen generation. The adsorption strength of *OH and the coverage of ClO4 - can be adjusted by the controllable electronic effect, resulting in different oxidation rates. This study offers valuable insights into elucidating the electrooxidation mechanisms underlying a range of electrocatalytic reactions, thereby contributing to the rational design of catalysts.

15.
Angew Chem Int Ed Engl ; : e202411542, 2024 Aug 12.
Article in English | MEDLINE | ID: mdl-39132837

ABSTRACT

Electrooxidation of biomass-derived glycerol which is regarded as a main byproduct of industrial biodiesel production, is an innovative strategy to produce value-added chemicals, but currently showcases slow kinetics, limited Faraday efficiency, and unclear catalytic mechanism. Herein, we report high-efficiency electrooxidation of glycerol into formate via a Cu doped NiCo alloy catalyst supported on nickel foam (Cu-NiCo/NF) in a coupled system paired with nitrate reduction. The designed Cu-NiCo/NF delivers only 1.23 V vs. RHE at 10 mA cm-2, and a record Faraday efficiency of formate of 93.8 %. The superior performance is ascribed to the rapid generation of NiIII-OOH and CoIII-OOH species and favorable coupling of surface *O with reactive intermediates. Using Cu-NiCo/NF as a bifunctional catalyst, the coupled system synchronously produces NH3 and formate, showing 290 mV lower than the coupling of hydrogen evolution reaction, together with excellent long-term stability for up to 144 h. This work lays out new guidelines and reliable strategies from catalyst design to system coupling for biomass-derived electrochemical refinery.

16.
Small ; : e2405160, 2024 Aug 07.
Article in English | MEDLINE | ID: mdl-39109948

ABSTRACT

The formation of NiOOH on the catalyst surface is widely considered to be the active species in electrochemical urea oxidation reactions (UOR). Though in situ-formed NiOOH species are reported to be more active than the synthesized ones, the mechanistic study of the actual active species remains a daunting task due to the possibility of different phases and instability of surface-formed NiOOH. Herein, mechanistic UOR aspects of electrochemically activated metallic Ni60Nb40 Nanoglass showing stability toward the γ-NiOOH phase are reported, probed via in situ Raman spectroscopy, supported by electron microscopy analysis and X-ray photoelectron spectroscopy in contrast with the ß-NiOOH formation favored on Ni foil. Detailed mechanistic study further reveals that γ-NiOOH predominantly follows a direct UOR mechanism while ß-NiOOH favors indirect UOR from time-dependent Raman study, and electrochemical impedance spectroscopy (EIS) analysis. The Nanoglass has shown outstanding UOR performance with a low Tafel slope of 16 mV dec-1 and stability for prolonged electrolysis (≈38 mA cm-2 for 70 h) that can be attributed to the nanostructured glassy interfaces facilitating more γ-NiOOH species formation and stabilization on the surface. The present study opens up a new direction for the development of inexpensive Ni-based UOR catalysts and sheds light on the UOR mechanism.

17.
ChemSusChem ; : e202401446, 2024 Aug 20.
Article in English | MEDLINE | ID: mdl-39161988

ABSTRACT

The sluggish anodic oxygen evolution reaction (OER) seriously restricts the overall efficiency of water splitting. Here, we present an environmentally friendly and efficient aniline oxidation (BOR) to replace the sluggish OER, accomplishing the co-production of H2 and high value-added benzonitrile (BN) at low voltages. Cobalt oxalates grown on cobalt foam (CoC2O4·2H2O/CF) are adopted as the pre-catalysts, which further evolve into working electrocatalysts active for BOR and HER after appropriate electrochemical activation. Thereinto, cyclic voltammetry activation at positive potentials is performed to reconstruct cobalt oxalate via extensive oxidation, resulting in enriched Co(III) species and nanoporous structures beneficial for BOR, while chronoamperometry at negative potentials is introduced for the cathodic activation toward efficient HER with obvious improvement. The two activated electrodes can be combined into a two-electrode system, which achieves a high current density of 75 mA cm-2 at the voltage of 1.95 V, with the high Faraday efficiencies of both BOR (90.0%) and HER (90.0%) and the satisfactory yield of BN (76.8%).

18.
J Environ Manage ; 367: 122067, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39111011

ABSTRACT

Adhesive production industry wastewater can be characterized by high chemical oxygen demand (COD) sourced from high refractory organic contaminants and high total suspended solids (TSS) concentration. Biodegradability of the wastewater is low and wastewater quality is unstable. Various treatment processes have limited applicability in such characterized wastewater. In this study, the treatment performance of electrochemical processes was investigated. Because it is not possible to meet the discharge standards by application of only one process for high refractory organic content, sequential electrochemical processes were studied in this work. In the first step of the sequential process, electrocoagulation (EC) using Al electrodes by which better performance was achieved was applied. In the second step, electrooxidation (EO) and peroxi-coagulation (PC) processes were applied to the EC effluent. In EO, Ti/MMO was selected as the most effective anode whereas in PC, Fe was used as the anode, and graphite was used as the cathode. Box-Behnken Design was applied to optimize the operating conditions of EO and PC processes and to obtain mathematical model equations. In the EC process, 77% COD, 78.5% TSS, and 85% UV254 removal efficiency were obtained under the optimum conditions (pH 7.2, reaction time 35 min, and current density 0.5 mA/cm2). With the EO and PC processes applied to the effluent of EC, 68.5% COD, 77% TSS, and 83% UV254 removal and 77.5% COD, 87% TSS, and 86.5% UV254 removal were obtained, respectively. The specific energy consumption of EC-EO and EC-PC processes was 16.08 kWh/kg COD and 15.06 kWh/kg COD, respectively. Considering the treatment targets and process operating costs, it was concluded that both sequential electrochemical systems could be promising alternative systems for the treatment of adhesive production industry wastewater.


Subject(s)
Electrocoagulation , Oxidation-Reduction , Waste Disposal, Fluid , Wastewater , Wastewater/chemistry , Waste Disposal, Fluid/methods , Electrocoagulation/methods , Biological Oxygen Demand Analysis , Adhesives , Water Pollutants, Chemical/chemistry , Electrodes
19.
Small ; : e2405225, 2024 Aug 19.
Article in English | MEDLINE | ID: mdl-39161189

ABSTRACT

To meet the industrial demand for overall water splitting, oxygen evolution reaction (OER) electrocatalysts with low-cost, highly effective, and durable properties are urgently required. Herein, a facile confined strategy is utilized to construct 2D NiFe2O4/Ni(OH)2 heterostructures-based self-supporting electrode with surface-interfacial coengineering, in which abundant and ultrastable interfaces are developed. Under the high molar ratio of Ni/Fe, both spinel oxide and hydroxides phases are formed simultaneously to obtain 2D NiFe2O4/Ni(OH)2 heterostructure. The in-depth analysis indicates that the NiFe2O4/Ni(OH)2 interface displays strong electronic interactions and triggers the formation of crystalline-amorphous coexisting catalytic active NiOOH. Meanwhile, the stable catalyst-collector interface favors the electron transfer and oxygen molecules transport. The resultant 2D NiFe2O4/Ni(OH)2@CP electrode exhibits superior OER performance, including a low overpotential of 389 mV and a long operating time of 12 h at 1 A cm-2. This work paves a novel method for fabricating efficient and low-cost electrocatalysts for electrochemical conversation devices.

20.
Article in English | MEDLINE | ID: mdl-39210224

ABSTRACT

The application of hybrid advanced oxidation processes (AOPs) is an efficacious way to remediate emerging contaminants from wastewater. In the present research work, a hybrid electrochemical oxidation and ultraviolet light-based persulfate activation processes (EO-UV/PS) were used to efficiently degrade sodium dodecyl sulfate (SDS) surfactant from synthetic and municipal wastewater. By operating the EO-UV/PS at optimum operating conditions at pH of 7.0, NaCl of 0.02 M, current density of 6.4 mA/cm2, persulfate dose of 2.5 mM, and operating period of 180 min, about 94.5 ± 2.8% of SDS (20 mg/L) removal was achieved from synthetic wastewater. The abetment of SDS in both EO and UV/PS obeyed pseudo-first-order kinetics with a rate constant of 0.012 and 0.019 min-1, respectively. Moreover, the economic analysis revealed 0.23 $ m-3 order-1 as the operating cost for degrading SDS in EO-UV/PS. The degradation pathway experimentation suggested the generation of lauric acid by-product during SDS abatement. Besides, nearly 89.3 ± 2.9% of SDS and 58.7 ± 2.4% of total organic carbon reduction was also achieved from real municipal wastewater. Phytotoxicity test on Vigna radiata affirms the non-toxic nature of the EO-UV/PS effluent.

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