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1.
Cell ; 179(5): 1084-1097.e21, 2019 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-31730851

RESUMEN

The ocean is home to myriad small planktonic organisms that underpin the functioning of marine ecosystems. However, their spatial patterns of diversity and the underlying drivers remain poorly known, precluding projections of their responses to global changes. Here we investigate the latitudinal gradients and global predictors of plankton diversity across archaea, bacteria, eukaryotes, and major virus clades using both molecular and imaging data from Tara Oceans. We show a decline of diversity for most planktonic groups toward the poles, mainly driven by decreasing ocean temperatures. Projections into the future suggest that severe warming of the surface ocean by the end of the 21st century could lead to tropicalization of the diversity of most planktonic groups in temperate and polar regions. These changes may have multiple consequences for marine ecosystem functioning and services and are expected to be particularly significant in key areas for carbon sequestration, fisheries, and marine conservation. VIDEO ABSTRACT.


Asunto(s)
Biodiversidad , Plancton/fisiología , Agua de Mar/microbiología , Geografía , Modelos Teóricos , Océanos y Mares , Filogenia
2.
Small ; 20(5): e2305136, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37759415

RESUMEN

This work addresses the challenges in developing carbon fiber paper-based supercapacitors (SCs) with high energy density by focusing on the limited capacity of carbon fiber. To overcome this limitation, a sponge-like porous carbon fiber paper enriched with oxygen functional groups (OFGs) is prepared, and Cu(OH)2 nanorods are grown on its surface to construct the SC anode. This design results in a multi-layered carbon fiber paper-based electrode with a specific structure and enhanced capacitance. The Cu(OH)2 @PCFP anode exhibits an areal capacitance of 547.83 mF cm-2 at a current density of 1 mA cm-2 and demonstrates excellent capacitance retention of 99.8% after 10 000 cycles. Theoretical calculations further confirm that the Cu(OH)2 /OFGs-graphite heterostructure exhibits higher conductivity, facilitating faster charge transfer. A solid-state SC is successfully assembled using Ketjen Black@PCFP as the cathode and KOH/PVA as the gel electrolyte. The resulting device exhibits an energy density of 0.21 Wh cm-2 at 1.50 mW cm-2 , surpassing the performance of reported Cu(OH)2 SCs. This approach, combining materials design with an understanding of underlying mechanisms, not only expands the range of electrode materials but also provides valuable insights for the development of high-capacity energy storage devices.

3.
Small ; : e2309756, 2024 Apr 11.
Artículo en Inglés | MEDLINE | ID: mdl-38602191

RESUMEN

Control over particle size and shape heterogeneity is highly relevant to the design of photonic coatings and supracolloidal assemblies. Most developments in the area have relied on mineral and petroleum-derived polymers that achieve well-defined chemical and dimensional characteristics. Unfortunately, it is challenging to attain such control when considering renewable nanoparticles. Herein, a pathway toward selectable biobased particle size and physicochemical profiles is proposed. Specifically, lignin is fractionated, a widely available heterogeneous polymer that can be dissolved in aqueous solution, to obtain a variety of monodispersed particle fractions. A two-stage cascade and density gradient centrifugation that relieves the need for solvent pre-extraction or other pretreatments but achieves particle bins of uniform size (~60 to 860 nm and polydispersity, PDI<0.06, dynamic light scattering) along with characteristic surface chemical features is introduced. It is found that the properties and associated colloidal behavior of the particles are suitably classified in distinctive size populations, namely, i) nanoscale (50-100 nm), ii) photonic (100-300 nm) and iii) near-micron (300-1000 nm). The strong correlation that exists between size and physicochemical characteristics (molar mass, surface charge, bonding and functional groups, among others) is introduced as a powerful pathway to identify nanotechnological uses that benefit from the functionality and cost-effectiveness of biogenic particles.

4.
Small ; : e2312122, 2024 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-38709229

RESUMEN

Management of functional groups in hole transporting materials (HTMs) is a feasible strategy to improve perovskite solar cells (PSCs) efficiency. Therefore, starting from the carbazole-diphenylamine-based JY7 molecule, JY8 and JY9 molecules are incorporated into the different electron-withdrawing groups of fluorine and cyano groups on the side chains. The theoretical results reveal that the introduction of electron-withdrawing groups of JY8 and JY9 can improve these highest occupied molecular orbital (HOMO) energy levels, intermolecular stacking arrangements, and stronger interface adsorption on the perovskite. Especially, the results of molecular dynamics (MD) indicate that the fluorinated JY8 molecule can yield a preferred surface orientation, which exhibits stronger interface adsorption on the perovskite. To validate the computational model, the JY7-JY9 are synthesized and assembled into PSC devices. Experimental results confirm that the HTMs of JY8 exhibit outstanding performance, such as high hole mobility, low defect density, and efficient hole extraction. Consequently, the PSC devices based on JY8 achieve a higher PCE than those of JY7 and JY9. This work highlights the management of the electron-withdrawing groups in HTMs to realize the goal of designing HTMs for the improvement of PSC efficiency.

5.
Small ; : e2309580, 2024 May 05.
Artículo en Inglés | MEDLINE | ID: mdl-38705865

RESUMEN

Li-ion batteries with superior interior thermal management are crucial to prevent thermal runaway and ensure safe, long-lasting operation at high temperatures or during rapid discharging and charging. Typically, such thermal management is achieved by focusing on the separator and electrolyte. Here, the study introduces a Se-terminated MXene free-standing electrode with exceptional electrical conductivity and low infrared emissivity, synergistically combining high-rate capacity with reduced heat radiation for safe, large, and fast Li+ storage. This is achieved through a one-step organic Lewis acid-assisted gas-phase reaction and vacuum filtration. The Se-terminated Nb2Se2C outperformed conventional disordered O/OH/F-terminated materials, enhancing Li+-storage capacity by ≈1.5 times in the fifth cycle (221 mAh·g-1 at 1 A·g-1) and improving mid-infrared adsorption with low thermal radiation. These benefits result from its superior electrical conductivity, excellent structural stability, and high permittivity in the infrared region. Calculations further reveal that increased permittivity and conductivity along the z-direction can reduce heat radiation from electrodes. This work highlights the potential of surface groups-terminated layered material-based free-standing flexible electrodes with self-thermal management ability for safe, fast energy storage.

6.
Chemistry ; 30(29): e202304065, 2024 May 23.
Artículo en Inglés | MEDLINE | ID: mdl-38487973

RESUMEN

Recent years have witnessed great research interests in developing high-performance electrocatalysts for the two-electron (2e-) oxygen reduction reaction (ORR) that enables the sustainable and flexible synthesis of H2O2. Carbon-based electrocatalysts exhibit attractive catalytic performance for the 2e- ORR, where oxygen-containing functional groups (OFGs) play a decisive role. However, current understanding is far from adequate, and the contribution of OFGs to the catalytic performance remains controversial. Therefore, a critical overview on OFGs in carbon-based electrocatalysts toward the 2e- ORR is highly desirable. Herein, we go over the methods for constructing OFGs in carbon including chemical oxidation, electrochemical oxidation, and precursor inheritance. Then we review the roles of OFGs in activating carbon toward the 2e- ORR, focusing on the intrinsic activity of different OFGs and the interplay between OFGs and metal species or defects. At last, we discuss the reasons for inconsistencies among different studies, and personal perspectives on the future development in this field are provided. The results provide insights into the origin of high catalytic activity and selectivity of carbon-based electrocatalysts toward the 2e- ORR and would provide theoretical foundations for the future development in this field.

7.
Chemistry ; 30(22): e202400074, 2024 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-38366948

RESUMEN

Conductive additives are of great importance for the adequate utilization of active materials in all-solid-state lithium batteries by establishing conductive networks in the composite cathode. However, it usually causes severe interfacial side reactions with solid electrolytes, especially sulfide electrolytes, leading to sluggish ion transportation and accelerated performance degradation. Herein, a simple hydrogen thermal reduction process is proposed on a commonly used conductive additive Super P, which effectively removes the surface oxygen functional groups and weakens the interfacial side reactions with sulfide. With a small amount of 1 wt % reduced Super P, ASSLBs demonstrates a competitive capacity of 180.2 mAh g-1, which is much higher than the 130.8 mAh g-1 of untreated Super P. Impressively, reduced Super P based ASSLBs also exhibit a higher capacity retention of 81.8 % than 64.6 % of untreated Super P. The cathode interfacial chemical evolutions reveal that reduced Super P could effectively alleviate the side reactions of sulfide. Reduced Super P shows better reversible capacity compared to reduced carbon nanofiber with almost no loss of capacity retention, due to its more complete conductive network. Our results highlight the importance of oxygen-containing functional groups for conductive additives, lightening the prospect of low-cost 0D conductive additives for practical ASSLBs.

8.
Ecol Appl ; 34(2): e2931, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-37950629

RESUMEN

Wetlands in arid or semiarid zones are vital for maintaining biodiversity but face growing threats. Flooding regime variability is a key driver of ecological dynamism in these systems, dictating primary productivity on a large spatial scale. The functional composition or diversity of wetland-dependent bird species has been found to be sensitive to fluctuations in hydrological regimes and can thus be indicative of cascading ecosystem responses associated with climate change. In this paper, we investigate whether large-scale changes in inundation and fire-a significant additional biodiversity determinant in (semi-)arid landscapes-are reliable predictors of functional group responses of wetland-dependent birds along a perennial channel of the Okavango Delta, Botswana. We fit generalized additive models (GAMs) to 6 years of bird survey data collected along ~190-km-long annual transects and use remotely sensed landscape-level inundation estimates, as well as spatiotemporal distance to fire, to predict the responsiveness of seven trait-based functional group abundances. During the surveys, a total of 89 different wetland-dependent bird species were recorded, including 76 residents, across all years, with below-surface feeding waders consistently the most abundant functional group. Including estimated spatiotemporal variability in flooding and fire, as well as their interactions, improved model fit for all seven functional groups, explaining between 46.8% and 68.3% of variability in functional group abundances. Covariates representing longer-term variability in inundation generally performed better than shorter-term ones. For example, variability in inundation over the 5 months preceding a survey best predicted the responses of all functional groups, which also all exhibited responsiveness to the interaction between flooding and fire. We were able to interpret the responses of individual functional groups, based on the resource exploitation assumption. Overall, our results suggest that perennial waters in dryland wetlands offer functional refugia to wetland-dependent birds and highlight the indicative power of large-scale trait-based bird monitoring. Our findings demonstrate the potential utility of such a monitoring regime for dryland wetland ecosystems vulnerable to industrial-scale anthropogenic pressure and associated climate change.


Asunto(s)
Ecosistema , Humedales , Animales , Biodiversidad , Aves , Inundaciones
9.
Microb Ecol ; 87(1): 58, 2024 Apr 11.
Artículo en Inglés | MEDLINE | ID: mdl-38602532

RESUMEN

Fungi play vital regulatory roles in terrestrial ecosystems. Local community assembly mechanisms, including deterministic and stochastic processes, as well as the size of regional species pools (gamma diversity), typically influence overall soil microbial community beta diversity patterns. However, there is limited evidence supporting their direct and indirect effects on beta diversity of different soil fungal functional groups in forest ecosystems. To address this gap, we collected 1606 soil samples from a 25-ha subtropical forest plot in southern China. Our goal was to determine the direct effects and indirect effects of regional species pools on the beta diversity of soil fungi, specifically arbuscular mycorrhizal (AM), ectomycorrhizal (EcM), plant-pathogenic, and saprotrophic fungi. We quantified the effects of soil properties, mycorrhizal tree abundances, and topographical factors on soil fungal diversity. The beta diversity of plant-pathogenic fungi was predominantly influenced by the size of the species pool. In contrast, the beta diversity of EcM fungi was primarily driven indirectly through community assembly processes. Neither of them had significant effects on the beta diversity of AM and saprotrophic fungi. Our results highlight that the direct and indirect effects of species pools on the beta diversity of soil functional groups of fungi can significantly differ even within a relatively small area. They also demonstrate the independent and combined effects of various factors in regulating the diversities of soil functional groups of fungi. Consequently, it is crucial to study the fungal community not only as a whole but also by considering different functional groups within the community.


Asunto(s)
Microbiota , Micorrizas , China , Bosques , Rayos gamma , Suelo
10.
Environ Sci Technol ; 58(22): 9896-9907, 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38669322

RESUMEN

Efficient use of humic acid (HA) for eco-friendly farming and environmental remediation requires further understanding of how targeted modification of HA affects the chemical structure of HA and thereby its effectiveness in enhancing soil quality. We developed novel selective modifiers (SMs) for extracting HA by codoping sodium and copper elements into the birnessite lattice. The structure of SMs was thoroughly examined, and the HAs extracted using SMs, referred to as SMHs, were subjected to a detailed evaluation of their functional groups, molecular weight, carbon composition, flocculation limits, and effectiveness in saline soil remediation. The results showed that replacing manganese with sodium and copper in SMs alters the valence state and reactive oxygen species. In contrast, SMHs exhibited increased acidic functional groups, a lower molecular weight, and transformed aliphatic carbon. Furthermore, the saline soil was improved through increased salt leaching and an optimized soil aggregate structure by SMHs. This research highlights the importance of targeted modification of HA and demonstrates the potential of these modifiers in improving soil quality for eco-friendly farming and environmental remediation.


Asunto(s)
Sustancias Húmicas , Suelo , Suelo/química , Restauración y Remediación Ambiental/métodos , Contaminantes del Suelo
11.
Environ Sci Technol ; 58(26): 11542-11553, 2024 Jul 02.
Artículo en Inglés | MEDLINE | ID: mdl-38871676

RESUMEN

Nanoplastics (NPs) are emerging pollutants and have been reported to cause the disintegration of anaerobic granular sludge (AnGS). However, the mechanism involved in AnGS disintegration was not clear. In this study, polyvinyl chloride nanoplastics (PVC-NPs) were chosen as target NPs and their long-term impact on AnGS structure was investigated. Results showed that increasing PVC-NPs concentration resulted in the inhibition of acetoclastic methanogens, syntrophic propionate, and butyrate degradation, as well as AnGS disintegration. At the presence of 50 µg·L-1 PVC-NPs, the hydrophobic interaction was weakened with a higher energy barrier due to the relatively higher hydrophilic functional groups in extracellular polymeric substances (EPS). PVC-NPs-induced ROS inhibited quorum sensing, significantly downregulated hydrophobic amino acid synthesis, whereas it highly upregulated the genes related to the synthesis of four hydrophilic amino acids (Cys, Glu, Gly, and Lys), resulting in a higher hydrophily degree of protein secondary structure in EPS. The differential expression of genes involved in EPS biosynthesis and the resulting protein secondary structure contributed to the greater hydrophilic interaction, reducing microbial aggregation ability. The findings provided new insight into the long-term impact of PVC-NPs on AnGS when treating wastewater containing NPs and filled the knowledge gap on the mechanism involved in AnGS disintegration by PVC-NPs.


Asunto(s)
Matriz Extracelular de Sustancias Poliméricas , Cloruro de Polivinilo , Aguas del Alcantarillado , Aguas del Alcantarillado/microbiología , Cloruro de Polivinilo/química , Matriz Extracelular de Sustancias Poliméricas/metabolismo , Anaerobiosis , Interacciones Microbianas
12.
Environ Sci Technol ; 58(24): 10752-10763, 2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38848107

RESUMEN

Groundwater contamination by 1,2,3-trichloropropane (TCP) poses a unique challenge due to its human toxicity and recalcitrance to degradation. Previous work suggests that nitrogenous functional groups of pyrogenic carbonaceous matter (PCM), such as biochar, are important in accelerating contaminant dechlorination by sulfide. However, the reaction mechanism is unclear due, in part, to PCM's structural complexity. Herein, PCM-like polymers (PLPs) with controlled placement of nitrogenous functional groups [i.e., quaternary ammonium (QA), pyridine, and pyridinium cations (py+)] were employed as model systems to investigate PCM-enhanced TCP degradation by sulfide. Our results suggest that both PLP-QA and PLP-py+ were highly effective in facilitating TCP dechlorination by sulfide with half-lives of 16.91 ± 1.17 and 0.98 ± 0.15 days, respectively, and the reactivity increased with surface nitrogenous group density. A two-step process was proposed for TCP dechlorination, which is initiated by reductive ß-elimination, followed by nucleophilic substitution by surface-bound sulfur nucleophiles. The TCP degradation kinetics were not significantly affected by cocontaminants (i.e., 1,1,1-trichloroethane or trichloroethylene), but were slowed by natural organic matter. Our results show that PLPs containing certain nitrogen functional groups can facilitate the rapid and complete degradation of TCP by sulfide, suggesting that similarly functionalized PCM might form the basis for a novel process for the remediation of TCP-contaminated groundwater.


Asunto(s)
Polímeros , Sulfuros , Sulfuros/química , Polímeros/química , Agua Subterránea/química , Contaminantes Químicos del Agua/química , Carbono/química , Propano/análogos & derivados
13.
Biometals ; 2024 May 25.
Artículo en Inglés | MEDLINE | ID: mdl-38789822

RESUMEN

The bioactive compounds contained within many plants account for their pharmacological values. Aloe vera has a wide range of organic and inorganic components, including carbohydrate polymers, glucomannans, and a variety of other natural and synthetic materials. The study aims to take a look into the characteristics of some metal complexes produced from Aloe vera extracts. The extracts from Aloe vera were derived by means of acetone, distilled water and ethanol. The solubility of the metal complexes with the ligand at varying temperatures was established. FT-IR was used to carry out the infra-red examination of the ligand. The results revealed that alcoholic extract of Aloe vera leaf was not soluble in Cu, Fe, or Zn but only soluble in Fe, the extract by distilled water was soluble in Cu, Fe and Zn. However, the Aloe vera in acetone as well as in the Zn (II) and Cu (II) composites displayed a bending that was found at 1430.97 cm-1, 1500.01 cm-1 and 1615.90 cm-1.every functional groups are assigned to be coordinating sites as a result of increase or decrease in the wave number, and absorption band. Findings from the investigation reveal that the complexion of the metal salts with diverse donor sites in the extract is indicated by an increase in the absorption peak of the functional groups in the metal composites of the extracts.

14.
Part Fibre Toxicol ; 21(1): 21, 2024 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-38658944

RESUMEN

BACKGROUND: Increasing attention is being paid to the environmental and health impacts of nanoplastics (NPs) pollution. Exposure to nanoplastics (NPs) with different charges and functional groups may have different adverse effects after ingestion by organisms, yet the potential ramifications on mammalian blood glucose levels, and the risk of diabetes remain unexplored. RESULTS: Mice were exposed to PS-NPs/COOH/NH2 at a dose of 5 mg/kg/day for nine weeks, either alone or in a T2DM model. The findings demonstrated that exposure to PS-NPs modified by different functional groups caused a notable rise in fasting blood glucose (FBG) levels, glucose intolerance, and insulin resistance in a mouse model of T2DM. Exposure to PS-NPs-NH2 alone can also lead the above effects to a certain degree. PS-NPs exposure could induce glycogen accumulation and hepatocellular edema, as well as injury to the pancreas. Comparing the effect of different functional groups or charges on T2DM, the PS-NPs-NH2 group exhibited the most significant FBG elevation, glycogen accumulation, and insulin resistance. The phosphorylation of AKT and FoxO1 was found to be inhibited by PS-NPs exposure. Treatment with SC79, the selective AKT activator was shown to effectively rescue this process and attenuate T2DM like lesions. CONCLUSIONS: Exposure to PS-NPs with different functional groups (charges) induced T2DM-like lesions. Amino-modified PS-NPs cause more serious T2DM-like lesions than pristine PS-NPs or carboxyl functionalized PS-NPs. The underlying mechanisms involved the inhibition of P-AKT/P-FoxO1. This study highlights the potential risk of NPs pollution on T2DM, and provides a new perspective for evaluating the impact of plastics aging.


Asunto(s)
Glucemia , Diabetes Mellitus Tipo 2 , Resistencia a la Insulina , Nanopartículas , Poliestirenos , Proteínas Proto-Oncogénicas c-akt , Animales , Diabetes Mellitus Tipo 2/inducido químicamente , Glucemia/efectos de los fármacos , Glucemia/metabolismo , Masculino , Poliestirenos/toxicidad , Poliestirenos/química , Nanopartículas/toxicidad , Proteínas Proto-Oncogénicas c-akt/metabolismo , Diabetes Mellitus Experimental/inducido químicamente , Ratones , Proteína Forkhead Box O1/metabolismo , Microplásticos/toxicidad , Fosforilación , Ratones Endogámicos C57BL , Hígado/efectos de los fármacos , Hígado/metabolismo , Hígado/patología
15.
Proc Natl Acad Sci U S A ; 118(35)2021 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-34429362

RESUMEN

The popularly reported energy storage mechanisms of potassium-ion batteries (PIBs) are based on alloy-, de-intercalation-, and conversion-type processes, which inevitably lead to structural damage of the electrodes caused by intercalation/de-intercalation of K+ with a relatively large radius, which is accompanied by poor cycle stabilities. Here, we report the exploration of robust high-temperature PIBs enabled by a carboxyl functional group energy storage mechanism, which is based on an example of p-phthalic acid (PTA) with two carboxyl functional groups as the redox centers. In such a case, the intercalation/de-intercalation of K+ can be performed via surface reactions with relieved volume change, thus favoring excellent cycle stability for PIBs against high temperatures. As proof of concept, at the fixed working temperature of 62.5 °C, the initial discharge and charge specific capacities of the PTA electrode are ∼660 and 165 mA⋅h⋅g-1, respectively, at a current density of 100 mA⋅g-1, with 86% specific capacity retention after 160 cycles. Meanwhile, it delivers 81.5% specific capacity retention after 390 cycles under a high current density of 500 mA⋅g-1 The cycle stabilities achieved under both low and high current densities are the best among those of high-temperature PIBs reported previously.

16.
Artículo en Inglés | MEDLINE | ID: mdl-38806110

RESUMEN

From review of the very few topical studies to date, we conclude that while effects are variable, microplastics can induce direct ionoregulatory disturbances in freshwater fish and invertebrates. However, the intensity depends on microplastic type, size, concentration, and exposure regime. More numerous are studies where indirect inferences about possible ionoregulatory effects can be drawn; these indicate increased mucus production, altered breathing, histopathological effects on gill structure, oxidative stress, and alterations in molecular pathways. All of these could have negative effects on ionoregulatory homeostasis. However, previous research has suffered from a lack of standardized reporting of microplastic characteristics and exposure conditions. Often overlooked is the fact that microplastics are dynamic contaminants, changing over time through degradation and fragmentation and subsequently exhibiting altered surface chemistry, notably an increased presence and diversity of functional groups. The same functional groups characterized on microplastics are also present in dissolved organic matter, often termed dissolved organic carbon (DOC), a class of substances for which we have a far greater understanding of their ionoregulatory actions. We highlight instances in which the effects of microplastic exposure resemble those of DOC exposure. We propose that in future microplastic investigations, in vivo techniques that have proven useful in understanding the ionoregulatory effects of DOC should be used including measurements of transepithelial potential, net and unidirectional radio-isotopic ion flux rates, and concentration kinetic analyses of uptake transport. More sophisticated in vitro approaches using cultured gill epithelia, Ussing chamber experiments on gill surrogate membranes, and scanning ion selective electrode techniques (SIET) may also prove useful. Finally, in future studies we advocate for minimum reporting requirements of microplastic properties and experimental conditions to help advance this important emerging field.


Asunto(s)
Peces , Agua Dulce , Branquias , Invertebrados , Microplásticos , Contaminantes Químicos del Agua , Animales , Branquias/efectos de los fármacos , Branquias/metabolismo , Microplásticos/toxicidad , Peces/fisiología , Peces/metabolismo , Contaminantes Químicos del Agua/toxicidad , Invertebrados/efectos de los fármacos , Invertebrados/fisiología
17.
Ecotoxicol Environ Saf ; 270: 115916, 2024 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-38171108

RESUMEN

Mercury (Hg) contamination is acknowledged as a global issue and has generated concerns globally due to its toxicity and persistence. Tunable surface-active sites (SASs) are one of the key features of efficient BCs for Hg remediation, and detailed documentation of their interactions with metal ions in soil medium is essential to support the applications of functionalized BC for Hg remediation. Although a specific active site exhibits identical behavior during the adsorption process, a systematic documentation of their syntheses and interactions with various metal ions in soil medium is crucial to promote the applications of functionalized biochars in Hg remediation. Hence, we summarized the BC's impact on Hg mobility in soils and discussed the potential mechanisms and role of various SASs of BC for Hg remediation, including oxygen-, nitrogen-, sulfur-, and X (chlorine, bromine, iodine)- functional groups (FGs), surface area, pores and pH. The review also categorized synthesis routes to introduce oxygen, nitrogen, and sulfur to BC surfaces to enhance their Hg adsorptive properties. Last but not the least, the direct mechanisms (e.g., Hg- BC binding) and indirect mechanisms (i.e., BC has a significant impact on the cycling of sulfur and thus the Hg-soil binding) that can be used to explain the adverse effects of BC on plants and microorganisms, as well as other related consequences and risk reduction strategies were highlighted. The future perspective will focus on functional BC for multiple heavy metal remediation and other potential applications; hence, future work should focus on designing intelligent/artificial BC for multiple purposes.


Asunto(s)
Restauración y Remediación Ambiental , Mercurio , Contaminantes del Suelo , Mercurio/análisis , Dominio Catalítico , Contaminantes del Suelo/análisis , Carbón Orgánico/química , Suelo/química , Azufre , Iones , Nitrógeno , Oxígeno
18.
Sci Technol Adv Mater ; 25(1): 2327274, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38529018

RESUMEN

Vanadium redox flow batteries (VRFBs) have received significant attention for use in large-scale energy storage systems (ESSs) because of their long cycle life, flexible capacity, power design, and safety. However, the poor electrochemical activity of the conventionally used carbon felt electrode results in low energy efficiency of the VRFBs and consequently impedes their commercialization. In this study, a carbon felt (CF) electrode with numerous nanopores and robust oxygen-containing functional groups at its edge sites is designed to improve the electrochemical activity of a carbon felt electrode. To achieve this, Ni metal nanoparticles were initially precipitated on the surface of the CF electrode, followed by etching of the precipitated Ni nanoparticles on the CF electrode using sulfuric acid. The resulting CF electrode had a specific surface area eight times larger than that of the pristine CF electrode. In addition, the oxygen-containing functional groups anchored at the graphite edge sites of the nanopores can act as robust electrocatalysts for VO2+/VO2+ and V2+/V3+ redox reactions. Consequently, the VRFB cell with the resulting carbon felt electrode can deliver a high energy efficiency of 86.2% at the current density of 60 mA cm-2, which is 20% higher than that of the VRFB cell with the conventionally heat-treated CF electrode. Furthermore, the VRFB cell with the resultant carbon felt electrodes showed stable cycling performance with no considerable energy efficiency loss over 200 charge-discharge cycles. In addition, even at a high current density of 160 mA cm-2 , the developed carbon felt electrode can achieve an energy efficiency of 70.1%.


This work reveals the importance of the robust graphite edge-site oxygen functional group and the holey structure of the ET-CF electrode, emphasizing that high VRFB efficiency can be achieved by engineering both the structure and surface properties of the carbon felt electrode.

19.
Nano Lett ; 23(4): 1401-1408, 2023 Feb 22.
Artículo en Inglés | MEDLINE | ID: mdl-36715492

RESUMEN

Engineered MXene surfaces with more -O functional groups are feasible for realizing higher energy density due to their higher theoretical capacitance. However, there have been only a few explorations of this regulation mechanism. Investigating the formation source and mechanism is conducive to expanding the adjustment method from the top-down perspective. Herein, for the first time, the formation dynamics of -O functional groups on Mo2CTx are discovered as a two-step dehydrogenation of adsorbed water through in situ near-ambient-pressure X-ray photoelectron spectroscopy, further confirmed by ab initio molecular dynamics simulations. From this, the controllable substitution of -F functional groups with -O functional groups is achieved on Mo2CTx during electrochemical cycling in an aqueous electrolyte. The obtained Mo2CTx with rich -O groups exhibits a high capacitance of 163.2 F g -1 at 50 mV s -1, together with excellent stability. These results offer new insights toward engineering surface functional groups of MXenes for many specific applications.

20.
Int J Mol Sci ; 25(4)2024 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-38396972

RESUMEN

Due to growing concerns about environmental pollution from plastic waste, plastic recycling research is gaining momentum. Traditional methods, such as incorporating inorganic particles, increasing cross-linking density with peroxides, and blending with silicone monomers, often improve mechanical properties but reduce flexibility for specific performance requirements. This study focuses on synthesizing silica nanoparticles with vinyl functional groups and evaluating their mechanical performance when used in recycled plastics. Silica precursors, namely sodium silicate and vinyltrimethoxysilane (VTMS), combined with a surfactant, were employed to create pores, increasing silica's surface area. The early-stage introduction of vinyl functional groups prevented the typical post-synthesis reduction in surface area. Porous silica was produced in varying quantities of VTMS, and the synthesized porous silica nanomaterials were incorporated into recycled polyethylene to induce cross-linking. Despite a decrease in surface area with increasing VTMS content, a significant surface area of 883 m2/g was achieved. In conclusion, porous silica with the right amount of vinyl content exhibited improved mechanical performance, including increased tensile strength, compared to conventional porous silica. This study shows that synthesized porous silica with integrated vinyl functional groups effectively enhances the performance of recycled plastics.


Asunto(s)
Nanopartículas , Nanoestructuras , Silanos , Compuestos de Vinilo , Dióxido de Silicio , Reciclaje , Contaminación Ambiental
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