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1.
Article in English | MEDLINE | ID: mdl-38963227

ABSTRACT

The electrochemical reduction of nitrate (NO3-) ions to ammonia (NH3) provides an alternative method to eliminate harmful NO3- pollutants in water as well as to produce highly valuable NH3 chemicals. The NH3 yield rate however is still limited to the µmol h-1 cm-2 range when dealing with dilute NO3- concentrations found in waste streams. Copper (Cu) has attracted much attention because of its unique ability to effectively convert NO3- to NH3. We have reported a simple and scalable electrochemical method to produce a Cu foil having its surface covered with a porous Cu nanostructure enriched with (100) facets, which efficiently catalyzes NO3- to NH3. The Cu(100)-rich electrocatalyst showed a very high NH3 production rate of 1.1 mmol h-1 cm-2 in NO3- concentration as low as 14 mM NO3-, which is 4-5 times higher than the best-reported values. Increasing the NO3- concentration (140 mM) resulted in an NH3 production yield rate of 3.34 mmol h-1 cm-2. The durability test conducted for this catalyst foil in a flow cell system showed greater than 100 h stability with a Faradaic efficiency greater than 98%, demonstrating its potential to be used on an industrially relevant scale. Further, density functional theory (DFT) calculations have been performed to understand the better catalytic activity of Cu(100) compared to Cu(111) facets toward NO3-RR.

2.
Article in English | MEDLINE | ID: mdl-38954330

ABSTRACT

Animal farming wastewater is one of the most important sources of ammonia nitrogen (NH4+-N) emissions. Electro-oxidation can be a viable solution for removing NH4+-N in wastewater. Compared with other treatment methods, electro-oxidation has the advantages of i) high removal efficiency, ii) smaller size of treatment facilities, and iii) complete removal of contaminant. In this study, a previously prepared DSA (W, Ti-doped IrO2) was used for electro-oxidation of synthetic mariculture and livestock wastewater. The DSA was tested for chlorine evolution reaction (CER) activity, and the reaction kinetics was investigated. CER current efficiency reaches 60-80% in mariculture wastewater and less than 20% in livestock wastewater. In the absence of NH4+-N, the generation of active chlorine follows zero-order kinetics and its consumption follows first-order kinetics, with cathodic reduction being its main consumption pathway, rather than escape or conversion to ClO3-. Cyclic voltammetry experiments show that NH4+-N in the form of NH3 can be oxidized directly on the anode surface. In addition, the generated active chlorine combines with NH4+-N at a fast rate near the anode, rather than in the bulk solution. In electrolysis experiments, the NH4+-N removal rate in synthetic mariculture wastewater (30-40 mg/L NH4+-N) and livestock wastewater (~ 450 mg/L NH4+-N) is 112.9 g NH4+-N/(m2·d) and 186.5 g NH4+-N/(m2·d), respectively, which is much more efficient than biological treatment. The specific energy consumption (SEC) in synthetic mariculture wastewater is 31.5 kWh/kg NH4+-N, comparable to other modified electro-catalysts reported in the literature. However, in synthetic livestock wastewater, the SEC is as high as 260 kWh/kg NH4+-N, mainly due to the suppression of active chlorine generation by HCO3- and the generation of NO3- as a by-product. Therefore, we conclude that electro-oxidation is suitable for mariculture wastewater treatment, but is not recommended for livestock wastewater. Electrolysis prior to urea hydrolysis may enhance the treatment efficiency in livestock wastewater.

3.
J Colloid Interface Sci ; 675: 24-35, 2024 Jul 02.
Article in English | MEDLINE | ID: mdl-38964122

ABSTRACT

To improve the efficiency of the methanol oxidation reaction (MOR) in direct methanol fuel cells (DMFCs), it is essential to develop catalysts with high catalytic activity. However, constructing polyatomic doped carbon nanomaterials and understanding the interaction mechanisms between dopant elements remain significant challenges. In this study, we propose nitrogen-doped carbon nanobox (CNB) derived from Zeolitic Imidazolate Framework-67 (ZIF-67) crystals as precursors to serve as carriers for highly efficient platinum nanoparticles (Pt NPs). We synthesized platinum/poly(3,4-propylenedioxythiophene)/carbon nanobox (Pt/PProDOT/CNB) composites by wrapping CNB around PProDOT films via in situ oxidative polymerization. This unique structural design provides several advantages to the catalyst, including a large active surface area, numerous accessible electrocatalytic active centers, an optimized electronic structure, and good electronic conductivity. The Pt/PProDOT/CNB composites demonstrated excellent methanol oxidation performance, with a remarkable mass activity (MA) of 1639.9 mA mg-1Pt and a high electrochemical active surface area (ECSA) of 160.8 m2/g. Furthermore, the catalyst exhibited good CO resistance and outstanding durability.

4.
Small ; : e2403557, 2024 Jul 05.
Article in English | MEDLINE | ID: mdl-38966886

ABSTRACT

It is a grand challenge to deep understanding of and precise control over functional sites for the rational design of highly efficient catalysts for methanol electrooxidation. Here, an L12-Pt2RhFe intermetallic catalyst with integrated functional components is demonstrated, which exhibits exceptional CO tolerance. The Pt2RhFe/C achieves a superior mass activity of 6.43 A mgPt -1, which is 2.23-fold and 3.53-fold higher than those of PtRu/C and Pt/C. Impressively, the Pt2RhFe/C exhibits a significant enhancement in durability owing to its high CO-tolerance and stability. Density functional theory calculations reveal that high performance of Pt2RhFe intermetallic catalyst arises from the synergistic effect: the strong OH binding energy (OHBE) at Fe sites induce stably adsorbed OH species and thus facilitate the dehydrogenation step of methanol via rapid hydrogen transfer, while moderate OHBE at Rh sites promote the formation of the transition state (Pt-CO···OH-Rh) with a low activation barrier for CO removal. This work provides new insights into the role of OH binding strength in the removal of CO species, which is beneficial for the rational design of highly efficient catalysts.

5.
Small ; : e2401998, 2024 Jul 08.
Article in English | MEDLINE | ID: mdl-38973636

ABSTRACT

The study presents the first example of an adsorbed carbon monoxide (CO) enabled self-terminated Au-grafting on triphenylphosphine (PPh3) stabilized Pt6 nanoclusters (NCs) (Pt6 (PPh3)4Cl5 NCs or Pt6 NCs). Adsorbed PPh3 ligands weaken the Pt-CO bond enabling the self-terminated Au-grafting on Pt6 NCs. The Au-grafted Pt6 NCs exhibit enhanced methanol electrooxidation (MOR) in acidic solutions. The surface is composed of a PtAu ensemble exhibiting enhanced MOR and CO tolerance due to the synergistic interaction of Pt with Au and PPh3. The hydrogen underpotential deposition (H-UPD) signal from a CO-covered surface reveals the existence of free-Pt sites on the PtAu ensemble causing higher MOR reactivity. The Au and PPh3 ensure electrocatalytic activity of the NCs, depriving of them at anodic potentials results in "a death-valley" trend.

6.
Sci Bull (Beijing) ; 2024 Jun 14.
Article in English | MEDLINE | ID: mdl-38942696

ABSTRACT

Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), a sustainable strategy to produce bio-based plastic monomer, is always conducted in a high-concentration alkaline solution (1.0 mol L-1 KOH) for high activity. However, such high concentration of alkali poses challenges including HMF degradation and high operation costs associated with product separation. Herein, we report a single-atom-ruthenium supported on Co3O4 (Ru1-Co3O4) as a catalyst that works efficiently in a low-concentration alkaline electrolyte (0.1 mol L-1 KOH), exhibiting a low potential of 1.191 V versus a reversible hydrogen electrode to achieve 10 mA cm-2 in 0.1 mol L-1 KOH, which outperforms previous catalysts. Electrochemical studies demonstrate that single-atom-Ru significantly enhances hydroxyl (OH-) adsorption with insufficient OH- supply, thus improving HMF oxidation. To showcase the potential of Ru1-Co3O4 catalyst, we demonstrate its high efficiency in a flow reactor under industrially relevant conditions. Eventually, techno-economic analysis shows that substitution of the conventional 1.0 mol L-1 KOH with 0.1 mol L-1 KOH electrolyte may significantly reduce the minimum selling price of FDCA by 21.0%. This work demonstrates an efficient catalyst design for electrooxidation of biomass working without using strong alkaline electrolyte that may contribute to more economic biomass electro-valorization.

7.
Environ Sci Pollut Res Int ; 31(30): 42593-42613, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38900403

ABSTRACT

The prevalence of polyfluoroalkyls and perfluoroalkyls (PFAS) represents a significant challenge, and various treatment techniques have been employed with considerable success to eliminate PFAS from water, with the ultimate goal of ensuring safe disposal of wastewater. This paper first describes the most promising electrochemical oxidation (EO) technology and then analyses its basic principles. In addition, this paper reviews and discusses the current state of research and development in the field of electrode materials and electrochemical reactors. Furthermore, the influence of electrode materials and electrolyte types on the deterioration process is also investigated. The importance of electrode materials in ethylene oxide has been widely recognised, and therefore, the focus of current research is mainly on the development of innovative electrode materials, the design of superior electrode structures, and the improvement of efficient electrode preparation methods. In order to improve the degradation efficiency of PFOS in electrochemical systems, it is essential to study the oxidation mechanism of PFOS in the presence of ethylene oxide. Furthermore, the factors influencing the efficacy of PFAS treatment, including current density, energy consumption, initial concentration, and other parameters, are clearly delineated. In conclusion, this study offers a comprehensive overview of the potential for integrating EO technology with other water treatment technologies. The continuous development of electrode materials and the integration of other water treatment processes present a promising future for the widespread application of ethylene oxide technology.


Subject(s)
Electrodes , Oxidation-Reduction , Water Pollutants, Chemical/chemistry , Fluorocarbons/chemistry , Electrochemical Techniques , Water Purification/methods , Wastewater/chemistry
8.
ACS Appl Mater Interfaces ; 16(27): 35074-35083, 2024 Jul 10.
Article in English | MEDLINE | ID: mdl-38919051

ABSTRACT

The electrocatalytic conversion of formate in alkaline solutions is of paramount significance in the realm of fuel cell applications. Nonetheless, the adsorptive affinity of adsorbed hydrogen (Had) on the catalyst surface has traditionally impeded the catalytic efficiency of formate in such alkaline environments. To circumvent this challenge, our approach introduces an interfacial push-pull effect on the catalyst surface. This mechanism involves two primary actions: First, the anchoring of palladium (Pd) nanoparticles on a phosphorus-doped TiO2 substrate (Pd/TiO2-P) promotes the formation of electron-rich Pd with a downshifted d band center, thereby "pushing" the desorption of Had from the Pd active sites. Second, the TiO2-P support diminishes the energy barrier for Had transfer from the Pd sites to the support itself, "pulling" Had to effectively relocate from the Pd active sites to the support. The resultant Pd/TiO2-P catalyst showcases a remarkable mass activity of 4.38 A mgPd-1 and outperforms the Pd/TiO2 catalyst (2.39 A mgPd-1) by a factor of 1.83. This advancement not only surmounts a critical barrier in catalysis but also delineates a scalable pathway to bolster the efficacy of Pd-based catalysts in alkaline media.

9.
J Colloid Interface Sci ; 673: 616-627, 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38897063

ABSTRACT

Oxygen evolution reaction (OER) is the efficiency limiting half-reaction in water electrolysis for green hydrogen production due to the 4-electron multistep process with sluggish kinetics. The electrooxidation of thermodynamically more favorable organics accompanied by CC coupling is a promising way to synthesize value-added chemicals instead of OER. Efficient catalyst is of paramount importance to fulfill such a goal. Herein, a molybdenum iron carbide-copper hybrid (Mo2C-FeCu) was designed as anodic catalyst, which demonstrated decent OER catalytic capability with low overpotential of 238 mV at response current density of 10 mA cm-2 and fine stability. More importantly, the Mo2C-FeCu enabled electrooxidation assisted aldol condensation of phenylcarbinol with α-H containing alcohol/ketone in weak alkali electrolyte to selective synthesize cinnamaldehyde/benzalacetone at reduced potential. The hydroxyl and superoxide intermediate radicals generated at high potential are deemed to be responsible for the electrooxidation of phenylcarbinol and aldol condensation reactions to afford cinnamaldehyde/benzalacetone. The current work showcases an electrochemical-chemical combined CC coupling reaction to prepare organic chemicals, we believe more widespread organics can be synthesized by tailored electrochemical reactions.

10.
Angew Chem Int Ed Engl ; : e202408765, 2024 May 26.
Article in English | MEDLINE | ID: mdl-38797705

ABSTRACT

Despite the great research interest in two-dimensional metal nanowire networks (2D MNWNs) due to their large specific surface area and abundance of unsaturated coordination atoms, their controllable synthesis still remains a significant challenge. Herein, a microfluidics laminar flow-based approach is developed, enabling the facile preparation of large-scale 2D structures with diverse alloy compositions, such as PtBi, AuBi, PdBi, PtPdBi, and PtAuCu alloys. Remarkably, these 2D MNWNs can reach sizes up to submillimeter scale (~220 µm), which is significantly larger than the evolution from the 1D or 3D counterparts that typically measure only tens of nanometers. The PdBi 2D MNWNs affords the highest specific activity for formic acid (2669.1 mA mg-1) among current unsupported catalysts, which is 103.5 times higher than Pt-black, respectively. Furthermore, in situ Fourier transform infrared (FTIR) experiments provide comprehensive evidence that PdBi 2D MNWNs catalysts can effectively prevent CO* poisoning, resulting in exceptional activity and stability for the oxidation of formic acid.

11.
J Colloid Interface Sci ; 670: 96-102, 2024 Sep 15.
Article in English | MEDLINE | ID: mdl-38759272

ABSTRACT

Replacing the anodic oxygen evolution reaction (OER) in water splitting with 5-hydroxymethylfurfural oxidation reaction (HMFOR) can not only reduce the energy required for hydrogen production but also yield the valuable chemical 2,5-furandicarboxylic acid (FDCA). Co-based catalysts are known to be efficient for HMFOR, with high-valent Co being recognized as the main active component. However, efficiently promoting the oxidation of Co2+ to produce high-valent reactive species remains a challenge. In this study, Ni-doped CoTe (CoNiTe) nanorods were prepared as efficient catalysts for HMFOR, achieving a high HMFOR current density of 65.3 mA cm-2 at 1.50 V. Even after undergoing five successive electrolysis processes, the Faradaic efficiency (FE) remained at approximately 90.7 %, showing robust electrochemical durability. Mechanistic studies indicated that Ni doping changes the electronic configuration of Co, enhancing its charge transfer rate and facilitating the oxidation of Co2+ to high-valent CoO2 species. This work reveals the effect of Ni doping on the reconfiguration of the active phase during HMFOR.

12.
Adv Mater ; : e2403792, 2024 May 14.
Article in English | MEDLINE | ID: mdl-38742953

ABSTRACT

Seawater electrolysis is a potentially cost-effective approach to green hydrogen production, but it currently faces substantial challenges for its high energy consumption and the interference of chlorine evolution reaction (ClER). Replacing the energy-demanding oxygen evolution reaction with methanol oxidation reaction (MOR) represents a promising alternative, as MOR occurs at a significantly low anodic potential, which cannot only reduce the voltage needed for electrolysis but also completely circumvents ClER. To this end, developing high-performance MOR catalysts is a key. Herein, a novel quaternary Pt1.8Pd0.2CuGa/C intermetallic nanoparticle (i-NP) catalyst is reported, which shows a high mass activity (11.13 A mgPGM -1), a large specific activity (18.13 mA cmPGM -2), and outstanding stability toward alkaline MOR. Advanced characterization and density functional theory calculations reveal that the introduction of atomically distributed Pd in Pt2CuGa intermetallic markedly promotes the oxidation of key reaction intermediates by enriching electron concentration around Pt sites, resulting in weak adsorption of carbon-containing intermediates and favorable adsorption of synergistic OH- groups near Pd sites. MOR-assisted seawater electrolysis is demonstrated, which continuously operates under 1.23 V for 240 h in simulated seawater and 120 h in natural seawater without notable degradation.

13.
Small Methods ; : e2400368, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38745535

ABSTRACT

The development of highly efficient electrocatalysts for the ethanol oxidation reaction (EOR) is essential for the commercialization of direct ethanol fuel cells, yet challenges remain. In this study, a one-pot solution-phase method to synthesize Pd nanowire networks (NNWs) with very high surface-to-volume ratio having numerous twin and grain boundaries is developed. Using the same method, the Pd lattice is further engineered by introducing Ag and Cu atoms to produce AgPd, and CuPd alloy structure which significantly shifts the Pd d-band center upward and downward, respectively due to strain and ligand effects. Theoretical analysis employing density functional theory (DFT) demonstrates that such modification of the d-band center significantly influences the adsorption energies of reactants on the catalytic surface. Owing to their notably high surface-to-volume ratio and the presence of multiple twin and grain boundaries, Pd NNWs demonstrate significantly enhanced electrocatalytic activity toward EOR, ≈7.2 times greater than that of commercial Pd/C. Remarkably, compared to Pd NNWs, AgPd, and CuPd NNWs display enlarged and reduced electrocatalytic activity toward EOR, respectively. Specifically, Ag4Pd7 NNWs achieve a remarkable mass activity of 9.00 A mgpd -1 for EOR, which is 13.6 times higher than commercial Pd/C.

14.
Front Chem ; 12: 1393860, 2024.
Article in English | MEDLINE | ID: mdl-38752198

ABSTRACT

Long-term electrolyses of glucose in a potassium carbonate (K2CO3) aqueous electrolyte have been performed on graphite felt electrodes with TEMPO as a homogeneous catalyst. The influences of the operating conditions (initial concentrations of glucose, TEMPO, and K2CO3 along with applied anode potential) on the conversion, selectivity toward gluconate/glucarate, and faradaic efficiency were assessed first. Then, optimizations of the conversion, selectivity, and faradaic efficiency were performed using design of experiments based on the L9 (34) Taguchi table, which resulted in 84% selectivity toward gluconate with 71% faradaic efficiency for up to 79% glucose conversion. Side products such as glucaric acid were also obtained when the applied potential exceeded 1.5 V vs. reversible hydrogen electrode.

15.
Anal Bioanal Chem ; 416(15): 3619-3630, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38702446

ABSTRACT

Glycerol is a widely used signaling bioanalyte in biotechnology. Glycerol can serve as a substrate or product of many metabolic processes in cells. Therefore, quantification of glycerol in fermentation samples with inexpensive, reliable, and rapid sensing systems is of great importance. In this work, an amperometric assay based on one-step designed electroplated functional Pd layers with controlled design was proposed for a rapid and selective measurement of glycerol in yeast fermentation medium. A novel assay utilizing electroplated Pd-sensing layers allows the quantification of glycerol in yeast fermentation medium in the presence of interfering species with RSD below 3% and recoveries ranged from 99 to 103%. The assay requires minimal sample preparation, viz. adjusting of sample pH to 12. The time taken to complete the electrochemical analysis was 3 min. Remarkably, during investigations, it was revealed that sensitivity and selectivity of glycerol determination on Pd sensors were significantly affected by its adsorption and did not depend on the surface structure of sensing layers. This study is expected to contribute to both fundamental and practical research fields related to a preliminary choice of functional sensing layers for specific biotechnology and life science applications in the future.


Subject(s)
Fermentation , Glycerol , Saccharomyces cerevisiae , Glycerol/metabolism , Glycerol/chemistry , Saccharomyces cerevisiae/metabolism , Electrochemical Techniques/methods , Electrochemical Techniques/instrumentation , Culture Media , Biosensing Techniques/methods
16.
Article in English | MEDLINE | ID: mdl-38666423

ABSTRACT

Although significant efforts have been made in the past few decades, the development of affordable, durable, and effective electrocatalysts for direct methanol fuel cells (DMFCs) remains a formidable challenge. Herein, we present a facile and efficient phosphorization approach for synthesizing PtP2 intermetallic nanocrystals and utilize them as electrocatalysts in the methanol oxidation reaction (MOR). Impressively, the synthesized PtP2 nanocatalysts exhibit a mass activity of 2.14 mA µg-1 and a specific activity of 6.28 mA cm-2, which are 5.1 and 9.5 times higher than those achieved by the current state-of-the-art commercial Pt/C catalyst, respectively. Moreover, the PtP2 nanocatalysts demonstrate improved stability toward acidic MOR by retaining 92.1% of its initial mass activity after undergoing 5000 potential cycles, far surpassing that of the commercial Pt/C (38%). Further DMFC tests present a 2.7 times higher power density than that of the commercial Pt/C, underscoring their potential for application in methanol fuel cells. Density functional theory calculations suggest that the accelerated MOR kinetics and improved CO tolerance on PtP2 can be attributed to the attenuated binding strength of CO intermediates and the enhanced stability due to strong Pt-P interaction. To our knowledge, this is the first report identifying the MOR performance on PtP2 intermetallic nanocrystals, highlighting their potential as highly active and stable nanocatalysts for DMFCs.

17.
Sensors (Basel) ; 24(8)2024 Apr 17.
Article in English | MEDLINE | ID: mdl-38676181

ABSTRACT

Active medical devices rely on a source of energy that is applied to the human body for specific purposes such as electrosurgery, ultrasounds for breaking up kidney stones (lithotripsy), laser irradiation, and other medical techniques and procedures that are extensively used. These systems must provide adequate working power with a commitment not to produce side effects on patients. Therefore, the materials used in these devices must effectively transmit energy, allow for security control, sense real-time variations in case of any issues, and ensure the implementation of closed-loop systems for control. This work extends to the experimental data adjustment of some different coating techniques based on plasma electro-oxidation (PEO) and thermal spray (TS) using fractional-order models. According to the physical structure of the coating in different coating techniques, Cole family models were selected. The experimental data were obtained by means of a vector network analyzer (VNA) in the frequency spectrum from 0.3 MHz to 5 MHz. The results show that some models from the Cole family (the single-dispersion model and inductive model) offered a goodness of fit to the experimental impedance in terms of RMSE error and a squared error R2 close to unity. The use of this type of fractional-order electrical model allows an adjustment with a very small number of elements compared to integer-order models, facilitating its use and a consequent reduction in instrumentation cost and the development of control devices that are more robust and easily miniaturized for embedded applications. Additionally, fractional-order models allow for more accurate assessment in industrial and medical applications.

18.
Adv Mater ; 36(27): e2403664, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38625813

ABSTRACT

Direct formate fuel cells (DFFCs) receive increasing attention as promising technologies for the future energy mix and environmental sustainability, as formate can be made from carbon dioxide utilization and is carbon neutral. Herein, heterostructured platinum-palladium alloy and oxides nanowires (PtPd-ox NWs) with abundant defect sites are synthesized through a facile self-template method and demonstrated high activity toward formate electrooxidation reaction (FOR). The electronic tuning arising from the heterojunction between alloy and oxides influence the work function of PtPd-ox NWs. The sample with optimal work function reveals the favorable adsorption behavior for intermediates and strong interaction in the d-p orbital hybridization between Pt site and oxygen in formate, favoring the FOR direct pathway with a low energy barrier. Besides the thermodynamic regulation, the heterostructure can also provide sufficient hydroxyl species to facilitate the formation of carbon dioxide due to the ability of combining absorbed hydrogen and carbon monoxide at adjacent active sites, which contributes to the improvement of FOR kinetics on PtPd-ox NWs. Thus, heterostructured PtPd-ox NWs achieve dual regulation of FOR thermodynamics and kinetics, exhibiting remarkable performance and demonstrating potential in practical systems.

19.
ACS Nano ; 18(15): 10341-10373, 2024 Apr 16.
Article in English | MEDLINE | ID: mdl-38572836

ABSTRACT

Noble-metal nanocrystals have emerged as essential electrode materials for catalytic oxidation of organic small molecule fuels in direct liquid fuel cells (DLFCs). However, for large-scale commercialization of DLFCs, adopting cost-effective techniques and optimizing their structures using advanced matrices are crucial. Notably, noble metal-decorated porous carbon nanoarchitectures exhibit exceptional electrocatalytic performances owing to their three-dimensional cross-linked porous networks, large accessible surface areas, homogeneous dispersion (of noble metals), reliable structural stability, and outstanding electrical conductivity. Consequently, they can be utilized to develop next-generation anode catalysts for DLFCs. Considering the recent expeditious advancements in this field, this comprehensive review provides an overview of the current progress in noble metal-decorated porous carbon nanoarchitectures. This paper meticulously outlines the associated synthetic strategies, precise microstructure regulation techniques, and their application in electrooxidation of small organic molecules. Furthermore, the review highlights the research challenges and future opportunities in this prospective research field, offering valuable insights for both researchers and industry experts.

20.
J Environ Sci (China) ; 143: 85-98, 2024 Sep.
Article in English | MEDLINE | ID: mdl-38644026

ABSTRACT

Ciprofloxacin (CIP) is a commonly used antibiotic in the fluoroquinolone group and is widely used in medical and veterinary medicine disciplines to treat bacterial infections. When CIP is discharged into the sewage system, it cannot be removed by a conventional wastewater treatment plant because of its recalcitrant characteristics. In this study, boron-doped diamond anode and persulfate were used to degrade CIP in an aquatic solution by creating an electrochemically activated persulfate (EAP) process. Iron was added to the system as a coactivator and the process was called EAP+Fe. The effects of independent variables, including pH, Fe2+, persulfate concentration, and electrolysis time on the system were optimized using the response surface methodology. The results showed that the EAP+Fe process removed 94% of CIP under the following optimum conditions: A pH of 3, persulfate/Fe2+ concentration of 0.4 mmol/L, initial CIP concentration 30 mg/L, and electrolysis time of 12.64 min. CIP removal efficiency was increased from 65.10% to 94.35% by adding Fe2+ as a transition metal. CIP degradation products, 7 pathways, and 78 intermediates of CIP were studied, and three of those intermediates (m/z 298, 498, and 505) were reported. The toxicological analysis based on toxicity estimation software results indicated that some degradation products of CIP were toxic to targeted animals, including fathead minnow, Daphnia magna, Tetrahymena pyriformis, and rats. The optimum operation costs were similar in EAP and EAP+Fe processes, approximately 0.54 €/m3.


Subject(s)
Anti-Bacterial Agents , Ciprofloxacin , Water Pollutants, Chemical , Water Pollutants, Chemical/toxicity , Water Pollutants, Chemical/chemistry , Anti-Bacterial Agents/chemistry , Anti-Bacterial Agents/toxicity , Ciprofloxacin/toxicity , Animals , Waste Disposal, Fluid/methods , Wastewater/chemistry , Electrochemical Techniques , Sulfates/chemistry
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