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1.
Nano Lett ; 24(29): 8902-8910, 2024 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-39008627

RESUMO

Ion transportation at the interface significantly influences the electrochemical performance of the lithium ion battery, especially at high rates and low temperatures. Here, we develop a controlled self-assembly strategy for constructing a mesoporous carbon nanolayer with a uniform pore size and varied thicknesses on the two-dimensional monolayer MXene substrate. On the basis of the excellent electron conductivity of MXene, the mesoporous carbon layer is found with a voltage-driven ion accumulation effect, acting as an "ionic pump". The thicker mesoporous layer (∼2.28 nm) has the ability to accommodate a substantial quantity of ions, demonstrating enhanced ionic conductivity, remarkable cycling stability (192.8 mAh/g after 9400 cycles at 5.0 A/g), and outstanding rate capability at ambient and sub-zero temperatures (∼601 mAh/g at 0 °C and 0.05 A/g). This work provides valuable insights and guidance for the further development of high-performance electrode materials at high rates or low temperatures.

2.
Small ; 20(11): e2306910, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37926698

RESUMO

Heterogeneous membranes play a crucial role in osmotic energy conversion by effectively reducing concentration polarization. However, most heterogeneous membranes mitigate concentration polarization through an asymmetric charge distribution, resulting in compromised ion selectivity. Herein, hetero-nanochannels with asymmetric wettability composed of 2D mesoporous carbon and graphene oxide are constructed. The asymmetric wettability of the membrane endows it with the ability to suppress the concentration polarization without degrading the ion selectivity, as well as achieving a diode-like ion transport feature. As a result, enhanced osmotic energy harvesting is achieved with a power density of 6.41 W m-2 . This represents a substantial enhancement of 102.80-137.85% when compared to homogeneous 2D membranes, surpassing the performance of the majority of reported 2D membranes. Importantly, the membrane can be further used for high-performance ionic power harvesting by regulating ion transport, exceeding previously reported data by 89.1%.

3.
Small ; 20(1): e2304558, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37649197

RESUMO

Near-neutral zinc-air batteries (ZABs) have garnered significant research interest due to their high energy density, exceptional electrochemical reversibility, and adaptability to ambient air. However, these batteries suffer from substantial electrochemical polarization, low energy efficiency, and poor rate performance. In this study, a mesoporous carbon (meso-C) with a high specific surface area (1081 m2 g-1 ) and abundant porous structure for the cathode of near-neutral ZABs using a scalable synthesis method is prepared. The meso-C-based cathode is endowed with stable hydrophobicity and abundant electrochemical active sites, which considerably improve the energy efficiency, rate performance, and cycle life of the battery compare to commercial carbon black-based cathode when applied to near-neutral ZABs with 1 mol kg-1 (1 m) zinc acetate and 1 m zinc trifluoromethanesulfonate electrolytes. Additionally, the mesopores of meso-C facilitate the construction of better three-phase reaction interfaces and contribute to better electrochemical reversibility. The work presents a general and scalable approach for carbon materials in the cathode of near-neutral ZABs.

4.
Mikrochim Acta ; 191(7): 428, 2024 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-38940957

RESUMO

A novel nitrogen-doped ordered mesoporous carbon (OMC) pore-embedded growth Pt-Ru-Fe nanoparticles (Pt1-Ru7.5-Fex@N-OMCs) composite was designed and synthesized for the first time. SBA-15 was used as a template, and dopamine was used as a carbon and nitrogen source and metal linking reagent. The oxidative self-polymerization reaction of dopamine was utilized to polymerize dopamine into two-dimensional ordered SBA-15 template pores. Iron porphyrin was introduced as an iron source at the same time as polymerization of dopamine, which was introduced inside and outside the pores using dopamine-metal linkage. Carbonization of polydopamine, nitrogen doping and iron nanoparticle formation were achieved by one-step calcination. Then the templates were etched to form Fex@N-OMCs, and finally the Pt1-Ru7.5-Fex@N-OMCs composites were stabilized by the successful introduction of platinum-ruthenium nanoparticles through the substitution reaction. The composite uniformly embeds the transition metal nanoparticles inside the OMC pores with high specific surface area, which limits the size of the metal nanoparticles inside the pores. At the same time, the metal nanoparticles are also loaded onto the surface of the OMCs, realizing the uniform loading of metal nanoparticles both inside and outside the pores. This enhances the active sites of the composite, promotes the mass transfer process inside and outside the pores, and greatly enhances the electrocatalytic performance of the catalyst. The material shows high electrocatalytic performance for adrenaline, which is characterized by a wide linear range, high sensitivity and low detection limit, and can realize the detection of actual samples.

5.
Mikrochim Acta ; 191(4): 228, 2024 04 01.
Artigo em Inglês | MEDLINE | ID: mdl-38558104

RESUMO

A cutting-edge electrochemical method is presented for precise quantification of amitraz (AMZ), a commonly used acaricide in veterinary medicine and agriculture. Leveraging a lab-made screen-printed carbon electrode modified with a synergistic blend of perylene tetracarboxylic acid (PTCA), mesoporous carbon (MC), and Nafion, the sensor's sensitivity was significantly improved. Fine-tuning of PTCA, MC, and Nafion ratios, alongside optimization of the pH of the supporting electrolyte and accumulation time, resulted in remarkable sensitivity enhancements. The sensor exhibited a linear response within the concentration range 0.01 to 0.70 µg mL-1, boasting an exceptionally low limit of detection of 0.002 µg mL-1 and a limit of quantification of 0.10 µg mL-1, surpassing maximum residue levels permitted in honey, tomato, and longan samples. Validation with real samples demonstrated high recoveries ranging from 80.8 to 104.8%, with a relative standard deviation below 10%, affirming the method's robustness and precision. The modified PTCA/MC/Nafion@SPCE-based electrochemical sensor not only offers superior sensitivity but also simplicity and cost-effectiveness, making it a pivotal tool for accurate AMZ detection in food samples. Furthermore, beyond the scope of this study, the sensor presents promising prospects for wider application across various electrochemical analytical fields, thereby significantly contributing to food safety and advancing agricultural practices.


Assuntos
Carbono , Polímeros de Fluorcarboneto , Perileno , Toluidinas , Carbono/química , Perileno/química , Eletrodos
6.
Molecules ; 29(7)2024 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-38611716

RESUMO

Selective oxidation, which is crucial in diverse chemical industries, transforms harmful chemicals into valuable compounds. Heterogeneous sonocatalysis, an emerging sustainable approach, urges in-depth exploration. In this work, we investigated N-doped or non-doped carbonaceous materials as alternatives to scarce, economically sensitive metal-based catalysts. Having synthesized diverse carbons using a hard-template technique, we subjected them to sonication at frequencies of 22, 100, 500, and 800 kHz with a 50% amplitude. Sonochemical reaction catalytic tests considerably increased the catalytic activity of C-meso (non-doped mesoporous carbon material). The scavenger test showed a radical formation when this catalyst was used. N-doped carbons did not show adequate and consistent sonoactivity for the selective oxidation of 4-Hydroxy-3,5 dimethoxybenzyl alcohol in comparison with control conditions without sonication, which might be associated with an acid-base interaction between the catalysts and the substrate and sonoactivity prohibition by piridinic nitrogen in N-doped catalysts.

7.
Molecules ; 29(3)2024 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-38338360

RESUMO

Currently, the obvious side effects of anti-tumor drugs, premature drug release, and low tumor penetration of nanoparticles have largely reduced the therapeutic effects of chemotherapy. A drug delivery vehicle (MCN-SS-GQDs) was designed innovatively. For this, the mesoporous carbon nanoparticles (MCN) with the capabilities of superior photothermal conversion efficiency and high loading efficiency were used as the skeleton structure, and graphene quantum dots (GQDs) were gated on the mesopores via disulfide bonds. The doxorubicin (DOX) was used to evaluate the pH-, GSH-, and NIR-responsive release performances of DOX/MCN-SS-GQDs. The disulfide bonds of MCN-SS-GQDs can be ruptured under high glutathione concentration in the tumor microenvironment, inducing the responsive release of DOX and the detachment of GQDs. The local temperature of a tumor increases significantly through the photothermal conversion of double carbon materials (MCN and GQDs) under near-infrared light irradiation. Local hyperthermia can promote tumor cell apoptosis, accelerate the release of drugs, and increase the sensitivity of tumor cells to chemotherapy, thus increasing treatment effect. At the same time, the detached GQDs can take advantage of their extremely small size (5-10 nm) to penetrate deeply into tumor tissues, solving the problem of low permeability of traditional nanoparticles. By utilizing the photothermal properties of GQDs, synergistic photothermal conversion between GQDs and MCN was realized for the purpose of synergistic photothermal treatment of superficial and deep tumor tissues.


Assuntos
Antineoplásicos , Grafite , Hipertermia Induzida , Nanopartículas , Neoplasias , Pontos Quânticos , Humanos , Pontos Quânticos/química , Grafite/química , Antineoplásicos/farmacologia , Antineoplásicos/química , Doxorrubicina , Nanopartículas/química , Fototerapia , Carbono/química , Neoplasias/tratamento farmacológico , Neoplasias/patologia , Dissulfetos , Microambiente Tumoral
8.
J Food Sci Technol ; 61(3): 573-584, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38327853

RESUMO

In this study, determination of aromatic compounds in cheese samples was performed by headspace solid-phase microextraction (HS-SPME) using a new adsorbent as a novel coated fiber in combination with a gas chromatography/mass spectrometry or flame ionization detector to evaluate the changes during ripening. Brine and ultrafiltrated (UF) cheese were sampled via HS-SPME and analyzed by gas chromatography/mass spectrometry. Polysulfone and mesoporous carbon nitride were used as two types of fibers for coating. The results showed that the pH had significant decreased during the 120 days for brine cheese (p < 0.001), and during the 90 days (p < 0.001) for UF cheese. Acidity was relatively stable during the ripening period for both cheeses (p > 0.05). Protein content decreased during the ripening period for both cheeses (p < 0.001). Moisture content also significantly decreased during the ripening period for both cheeses (p < 0.001). 74 compounds were identified in brine cheese and 27 major components in UF cheese. Fatty acids were the predominant components, followed by aldehydes (n: 17, 22.9%), alcohol (n; 12, 16.2%), ester (n: 11, 14.8%), alkane (n: 7, 9.4%), and ketone (n: 6, 8.1%) for white brine cheese, while for UF cheese fatty acid (n: 12, 44.4%) and aldehyde (n: 5, 18.5%), alcohol (n: 3, 11.1%), ketone (n: 3, 11.1%), ester (n: 2, 7.4%) and alkane (n: 1, 3.7%).

9.
Small ; 19(15): e2207348, 2023 04.
Artigo em Inglês | MEDLINE | ID: mdl-36617518

RESUMO

Contamination of water resources by toxic metals and opportunistic pathogens remains a serious challenge. The development of nano-adsorbents with desired features to tackle this problem is a continuously evolving field. Here, magnetic mesoporous carbon nanospheres grafted by antimicrobial polyhexamethylene biguanidine (PHMB) are reported. Detailed mechanistic investigations reveal that the electrostatic stabilizer modified magnetic nanocore interfaced mesoporous shell can be programmatically regulated to tune the size and related morphological properties. The core-shell nano-adsorbent shows tailorable shell thickness (≈20-55 nm), high surface area (363.47 m2 g-1 ), pore volume (0.426 cm3 g-1 ), radially gradient pores (11.26 nm), and abundant biguanidine functionality. Importantly, the nano-adsorbent has high adsorption capacity for toxic thallium (Tl(I) ions (≈559 mg g-1 ), excellent disinfection against Staphylococcus aureus and Escherichia coli (>99.99% at 2 and 2.5 µg mL-1 ), ultrafast disinfection kinetics rate (>99.99% within ≈4 min), and remarkable regeneration capability when exposed to polluted water matrices. The Tl(I) removal is attributed to surface complexation and physical adsorption owing to open ended mesopores, while disinfection relies on contact of terminal biguanidines with phospholipid head groups of membrane. The significance of this work lies in bringing up effective synchronic water purification technology to combat pathogenic microorganisms and toxic metal.


Assuntos
Poluentes Químicos da Água , Água , Desinfecção , Carbono , Adsorção , Fenômenos Magnéticos , Cinética , Concentração de Íons de Hidrogênio
10.
Small ; 19(12): e2205725, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36585360

RESUMO

1D carbon nanotubes have been widely applied in many fields, such as catalysis, sensing and energy storage. However, the long tunnel-like pores and relatively low specific surface area of carbon nanotubes often restrict their performance in certain applications. Herein, a dual-silica template-mediated method to prepare nitrogen-doped mesoporous carbon nanotubes (NMCTs) through co-depositing polydopamine (both carbon and nitrogen precursors) and silica nanoparticles (the porogen for mesopore formation) on a silica nanowire template is proposed. The obtained NMCTs have a hierarchical pore structure of large open mesopores and tubular macropores, a high specific surface area (1037 m2 g-1 ), and homogeneous nitrogen doping. The NMCT-45 (prepared at an interval time of 45 min) shows excellent performance in supercapacitor applications with a high capacitance (373.6 F g-1 at 1.0 A g-1 ), excellent rate capability, high energy density (11.6 W h kg-1 at a power density of 313 W kg-1 ), and outstanding cycling stability (98.2% capacity retention after 10 000 cycles at 10 A g-1 ). Owing to the unique tubular morphology, hierarchical porosity and homogeneous N-doping, the NMCT also has tremendous potential in electrochemical catalysis and sensing applications.

11.
Small ; 19(28): e2301203, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37010007

RESUMO

Hard carbons (HCs) with high sloping capacity are considered as the leading candidate anode for sodium-ion batteries (SIBs); nevertheless, achieving basically complete slope-dominated behavior with high rate capability is still a big challenge. Herein, the synthesis of mesoporous carbon nanospheres with highly disordered graphitic domains and MoC nanodots modification via a surface stretching strategy is reported. The MoOx surface coordination layer inhibits the graphitization process at high temperature, thus creating short and wide graphite domains. Meanwhile, the in situ formed MoC nanodots can greatly promote the conductivity of highly disordered carbon. Consequently, MoC@MCNs exhibit an outstanding rate capacity (125 mAh g-1 at 50 A g-1 ). The "adsorption-filling" mechanism combined with excellent kinetics is also studied based on the short-range graphitic domains to reveal the enhanced slope-dominated capacity. The insight in this work encourages the design of HC anodes with dominated slope capacity toward high-performance SIBs.

12.
Small ; 19(32): e2301038, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37069771

RESUMO

Photo-regulated nanofluidic devices have attracted great attention in recent years due to their adjustable ion transport in real time. However, most of the photo-responsive nanofluidic devices can only adjust the ionic current unidirectionally, and cannot simultaneously increase or decrease the current signal intelligently by one device. Herein, a mesoporous carbon-titania/ anodized aluminum hetero-channels (MCT/AAO) is constructed by super-assembly strategy, which exhibits dual-function of cation selectivity and photo response. The polymer and TiO2 nanocrystals jointly build the MCT framework. Polymer framework with abundant negatively charged sites endows MCT/AAO with excellent cation selectivity, and TiO2 nanocrystals are responsible for the photo-regulated ion transport. High photo current densities of 1.8 mA m-2 (increase) and 1.2 mA m-2 (decrease) are realized by MCT/AAO benefiting from the ordered hetero-channels. Significantly, MCT/AAO can also achieve the bidirectionally adjustable osmotic energy by alternating the configurations of concentration gradient. Theoretical and experimental results reveal that the superior photo-generated potential is responsible for the bidirectionally adjustable ion transport. Consequently, MCT/AAO performs the function of harvesting ionic energy from the equilibrium electrolyte solution, which greatly expands its practical application field. This work provides a new strategy in constructing dual-functional hetero-channels toward bidirectionally photo-regulated ionic transport and energy harvesting.

13.
Small ; 19(36): e2302334, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37127856

RESUMO

The surging demand for environmental-friendly and safe electrochemical energy storage systems has driven the development of aqueous zinc (Zn)-ion batteries (ZIBs). However, metallic Zn anodes suffer from severe dendrite growth and large volume change, resulting in a limited lifetime for aqueous ZIB applications. Here, it is shown that 3D mesoporous carbon (MC) with controlled carbon and defect configurations can function as a highly reversible and dendrite-free Zn host, enabling the stable operation of aqueous ZIBs. The MC host has a structure-controlled architecture that contains optimal sp2 -carbon and defect sites, which results in an improved initial nucleation energy barrier and promotes uniform Zn deposition. As a consequence, the MC host shows outstanding Zn plating/stripping performance over 1000 cycles at 2 mA cm-2 and over 250 cycles at 6 mA cm-2 in asymmetric cells. Density functional theory calculations further reveal the role of the defective sp2 -carbon surface in Zn adsorption energy. Moreover, a full cell based on Zn@MC900 anode and V2 O5 cathode exhibits remarkable rate performance and cycling stability over 3500 cycles. These results establish a structure-mechanism-performance relationship of the carbon host as a highly reversible Zn anode for the reliable operation of ZIBs.

14.
Small ; 19(32): e2303214, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37170674

RESUMO

It remains a challenge to develop efficient noble metal-free electrocatalysts for the oxygen reduction reaction (ORR) in various renewable energy systems. Single atom catalysts have recently drawn great attention as promising candidates both due to their high activity and their utmost atom utilization for electrocatalytic ORR. Herein, the synthesis of an efficient ORR electrocatalyst that is composed of N-doped mesoporous carbon and a high density (4.05 wt%) of single Fe atoms via pyrolysis Fe-conjugated polymer is reported. Benefiting from the abundant atomic Fe-N4 sites on its conductive, mesoporous carbon structures, this material exhibits an excellent electrocatalytic activity for ORR, with positive onset potentials of 0.93 and 0.98 V in acidic and alkaline media, respectively. Its electrocatalytic performance for ORR is also comparable to that of Pt/C (20 wt%) in both media. Furthermore, it electrocatalyzes the reaction almost fully to H2 O (or barely to H2 O2 ). Additionally, it is durable and tolerates the methanol crossover reaction well. Furthermore, a proton exchange membrane fuel cell and a zinc-air battery assembled using it on their cathode deliver high maximum power densities (320 and 91 mW cm-2 , respectively). Density functional theory calculation reveals that the material's decent electrocatalytic performance for ORR is due to its atomically dispersed Fe-N4 sites.

15.
Small ; 19(3): e2205693, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36408773

RESUMO

Two-dimensional (2D) mesoporous polymers, combining the advantages of organic polymers, porous materials, and 2D materials, have received great attention in adsorption, catalysis, and energy storage. However, the synthesis of 2D mesoporous polymers is not only challenged by the complex 2D structure construction, but also by the low yield and difficulty in controlling the dynamics of the assembly during the generation of mesopores. Herein, a facile multi-dimensional molecular self-assembly strategy is reported for the preparation of 2D mesoporous polydiaminopyridines (MPDAPs), which features tunable pore sizes (17-35 nm) and abundant N content up to 18.0 at%. Benefitting from the abundant N sites, 2D nanostructure, and uniform-large mesopores, the 2D MPDAPs exhibit excellent catalytic performance for the Knoevenagel condensation reaction. After calcination under N2 atmosphere, the obtained 2D N-doped mesoporous carbon (NMCs) with large and uniform pore sizes, high surface areas, abundant N content (up to 23.1%), and a high ratio of basic N species (57.0% pyridinic N and 35.9% pyrrolic N) can show an excellent CO2 uptake density (11.7 µmol m-2 at 273 K), higher than previously reported porous materials.

16.
Small ; 19(49): e2305353, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37606896

RESUMO

The combination of 2D magnetic nanosheets and mesoporous carbon with unique interfaces shows considerable prospects for microwave absorption (MA). However, traditional assembly procedures make it impossible to accurately manage the assembly of magnetic nanosheets in carbon matrices. Herein, a reverse strategy for preparing complex magnetic nanosheet cores inside carbon-based yolk-shell structures is developed. This innovative approach focuses on controlling the initial crystallite formation sites in a hydrothermal reaction as well as the inflow and in situ growth behavior of 2D NiCo-layered double hydroxide precursors based on the capillary force induced by hollow mesoporous carbon nanospheres. Accordingly, the as-prepared YS-CNC-2 absorber exhibits remarkable MA performances, with an optimal reflection loss as low as -60.30 dB at 2.5 mm and an effective absorption bandwidth of 5.20 GHz at 2.0 mm. The loss of electromagnetic waves (EMW) depends on natural resonance loss, dipole polarization relaxation, and multiple scattering behavior. On top of that, the functionalized super-hydrophobic MA coating is produced in spraying and curing processes utilizing YS-CNC-2 nanoparticles and fumed silica additives in the polydimethylsiloxane matrix. The excellent thermal insulation, self-cleaning capability, and durability in diverse solutions of the coating promise potential applications for military equipment in moist situations.

17.
Chemistry ; 29(69): e202302723, 2023 Dec 11.
Artigo em Inglês | MEDLINE | ID: mdl-37673789

RESUMO

Designing unique nanomaterials for the selective sensing of biomolecules is of significant interest in the field of nanobiotechnology. In this work, we demonstrated the synthesis of ordered Cu nanoparticle-functionalised mesoporous C3 N5 that has unique peroxidase-like nanozymatic activity for the ultrasensitive and selective detection of glucose and glutathione. A nano hard-templating technique together with the in-situ polymerisation and self-assembly of Cu and high N-containing CN precursor was adopted to introduce mesoporosity as well as high N and Cu content in mesoporous C3 N5 . Due to the ordered structure and highly dispersed Cu in the mesoporous C3 N5 , a large enhancement of the peroxidase mimetic activity in the oxidation of a redox dye in the presence of hydrogen peroxide could be obtained. Additionally, the optimised Cu-functionalised mesoporous C3 N5 exhibited excellent sensitivity to glutathione with a low detection limit of 2.0 ppm. The strong peroxidase activity of the Cu-functionalised mesoporous C3 N5 was also effectively used for the sensing of glucose with a detection limit of 0.4 mM through glucose oxidation with glucose oxidase. This unique Cu-functionalised mesoporous C3 N5 has the potential for detecting various molecules in the environment as well as for next-generation glucose and glutathione diagnostic devices.


Assuntos
Cobre , Nanopartículas , Cobre/química , Glucose/química , Nanopartículas/química , Peróxido de Hidrogênio/química , Peroxidases , Glutationa , Colorimetria
18.
Environ Res ; 236(Pt 1): 116742, 2023 11 01.
Artigo em Inglês | MEDLINE | ID: mdl-37507043

RESUMO

This study investigates the impact of microporous (SP-C) and micro-mesoporous carbon (DP-C) supports on the dispersion and phase transformation of iron oxides and their arsenic (V) removal efficiency. The research demonstrates that carbon-supported iron oxide sorbents exhibit superior As(V) uptake capacity compared to unsupported Fe2O3, attributed to reduced iron oxide crystallite sizes and As(V) adsorption on carbon supports. Maximum As(V) uptake capacities of 23.8 mg/g and 18.9 mg/g were achieved for Fe/SP-C and Fe/DP-C at 30 wt% and 50 wt% iron loading, respectively. The study reveals a nonlinear relationship between As(V) sorption capacity and iron oxide crystallite size after excluding As(V) adsorption capacity on carbon supports, suggesting the iron oxide phase (Fe3O4) plays a role in determining adsorption capacity. Iron oxide-loaded DP-C sorbents exhibit faster adsorption rates at low As(V) concentrations (5 mg/L) than SP-C sorbents due to their bimodal pore structure. Adsorption behavior varies at higher As(V) concentrations (45 mg/L), with Fe/DP-C reaching maximum capacity more slowly due to limited available adsorptive sites. All adsorbents maintained near-complete As(V) removal efficiency over five cycles. The findings provide insights for designing more efficient adsorbents for As(V) removal from contaminated water sources.


Assuntos
Arsênio , Poluentes Químicos da Água , Purificação da Água , Carbono , Poluentes Químicos da Água/análise , Cinética , Arsênio/análise , Ferro/química , Adsorção , Água
19.
Nano Lett ; 22(23): 9551-9558, 2022 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-36378846

RESUMO

Two-electron oxygen reduction toward hydrogen peroxide (H2O2) offers a promising alternative for H2O2 production, but its commercial utilization is still hindered by the difficulty of transferring lab-observed catalyst performance to the practical reactor. Here we report the investigation of the porosity engineering effect on catalytic performance inconsistency through a material platform consisting of a series of hollow mesoporous carbon sphere (HMCS) samples. The performance comparison of HMCS samples in rotating ring-disk electrode and Zn-air battery together with the simulation of diffusion behavior reveals that, in low current density conditions, large surface area is preferred, but the mass transport governs the performance in high current density regions. On account of the favorable porous structure, HMCS-8 nm delivers the most excellent practical performance (166 mW cm-2) and performs well in the bifunctional Zn-air battery for the wastewater purification (70% RhB degraded after 2 min and 99% after 32 min).

20.
Angew Chem Int Ed Engl ; 62(46): e202306791, 2023 Nov 13.
Artigo em Inglês | MEDLINE | ID: mdl-37779352

RESUMO

The electrocatalytic sulfur reduction reaction (SRR) would allow the production of renewable high-capacity rechargeable lithium-sulfur (Li-S) batteries using sustainable and nontoxic elemental sulfur as a cathode material, but its slow reaction rate causes a serious shuttle effect and dramatically reduces the capacity. We found that a catalyst composed of Pd nanoparticles supported by ordered mesoporous carbon (Pd/OMC) had a high reaction rate in the SRR, and a Li-S battery assembled with this catalyst had a low shuttle constant of 0.031 h-1 and a high-rate performance with a specific capacity of 1527 mAh g-1 at 0.1 C which is close to the theoretical value. The high activity of Pd/OMC with a d-orbital vacancy of 0.87 e was predicted from a volcano relationship between the d charge for the metal and the adsorption activation entropy and reaction rate for the SRR by examining Pd, Au, Pt, Rh, and Ru transition-metal nanocatalysts. The strategy of using a single electronic structure descriptor to design high-efficiency SRR catalysts has suggested a way to produce practical Li-S batteries.

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