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1.
Proc Natl Acad Sci U S A ; 120(43): e2311585120, 2023 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-37844255

RESUMO

Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure-performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure-reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.

2.
Nano Lett ; 24(25): 7732-7740, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38869233

RESUMO

Rechargeable lithium-ion batteries are integral to contemporary energy storage, yet current anode material systems struggle to meet the increasing demand for extended range capabilities. This work introduces a novel composite anode material composed of one-dimensional 2H-phase tin disulfide (SnS2) nanoribbons enclosed within cavities of single-walled carbon nanotubes (SnS2@SWCNTs), achieved through precise atomic engineering. Employing aberration-corrected transmission electron microscopy, we precisely elucidated the crystal structure of SnS2 within the confines of the SWCNTs. This deliberate design effectively addresses the inherent limitations of SnS2 as a lithium-ion anode material, including its low electrical conductivity, considerable volume expansion effects, and unstable solid electrolyte interface membrane. Testing confirmed that SnS2 transforms into the Li5Sn2 alloy phase after full lithiation and back to SnS2 after delithiation, showing excellent reversibility. The composite also benefits from edge effects, improving lithium storage through stronger binding and lower migration barriers, which were supported by calculations. This pioneering work advances high-performance anode materials for applications.

3.
Small ; 20(30): e2310196, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38377307

RESUMO

"Perovskite / Carbon" interface has remained a key bottleneck for the hole-conductor-free perovskite solar cells based on carbon-electrode (CPSCs), due to problems like loose physics contact, defects, energy mismatch, poor chemical coupling, etc. A previous study shows that octylammonium iodide (OAI) blending in carbon paste induced a kind of "in-situ healing" effect for "perovskite / carbon" interface, and improved power conversion efficiency from ≈13% to >19%. Here the beneath mechanism is further explored by careful examination of the interaction between OAI molecule and carbon black (CB) nanoparticles. It comes to show that, the famous "CB adsorption" plays a key role during the "healing" processes. Due to CB adsorption behavior, the mass ratio between OAI and CB influences much on the healing effect. By suitably adjusting the mass ratio between OAI and CB, and increasing the light harvest of perovskite, an efficiency of 19.41% is achieved for the hole-conductor-free CPSCs. Device efficiency and the charge-extraction and recombination process are tracked with the storage period, continuous improvement appears for devices assembled by relatively higher CB mass. A kind of "slow-release effect" is revealed during the OAI-induced "in-situ healing" process, which is caused by the famous "CB adsorption" behavior.

4.
Environ Res ; 252(Pt 4): 119076, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38710430

RESUMO

The large yield of anaerobic digestates and the suboptimal efficacy of nutrient slow-release severely limit its practical application. To address these issues, a new biochar based fertilizer (MAP@BRC) was developed using biogas residue biochar (BRC) to recover nitrogen and phosphorus from biogas slurry. The nutrient release patterns of MAP@BRC and mechanisms for enhancing soil fertility were studied, and it demonstrated excellent performance, with 59% total nitrogen and 50% total phosphorus nutrient release rates within 28 days. This was attributed to the coupling of the mechanism involving the dissolution of struvite skeletons and the release of biochar pores. Pot experiments showed that crop yield and water productivity were doubled in the MAP@BRC group compared with unfertilized planting. The application of MAP@BRC also improved soil nutrient levels, reduced soil acidification, increased microbial populations, and decreased soil heavy metal pollution risk. The key factors that contributed to the improvement in soil fertility by MAP@BRC were an increase in available nitrogen and the optimization of pH levels in the soil. Overall, MAP@BRC is a safe, slow-release fertilizer that exhibits biochar-fertilizer interactions and synergistic effects. This slow-release fertilizer was prepared by treating a phosphorus-rich biogas slurry with a nitrogen-rich biogas slurry, and it simultaneously addresses problems associated with livestock waste treatment and provides a promising strategy to promote zero-waste agriculture.


Assuntos
Biocombustíveis , Carvão Vegetal , Fertilizantes , Nitrogênio , Fósforo , Solo , Fertilizantes/análise , Carvão Vegetal/química , Solo/química , Fósforo/análise , Nitrogênio/análise , Biocombustíveis/análise , Agricultura/métodos
5.
Environ Res ; 252(Pt 1): 118758, 2024 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-38527724

RESUMO

Under the system of full straw returning, the relationship between soil fungal community diversity and soil physiochemical properties, and the combined application of slow-release nitrogen and urea is unclear. To evaluate its effect and provide an effective strategy for sustainable agricultural production, a 2-year field positioning trial was conducted using maize as the research object. The experiment was designed with two factors: straw treatment(S) and nitrogen fertilizer treatment(N),Six experimental treatments were set up,S1N0,S1N1,S1N2,S1N3,S1N4,S0N2,respectively.Analysis of 54 soil samples revealed 15 fungal phyla and 49 fungal classes. The composition of fungal communities in each treatment was basically the same, but there were significant differences in species abundance. Under total straw returning conditions, the combined application of slow-release nitrogen fertilizer and normal nitrogen fertilizer significantly increased the relative abundance of Ascomycota. During the jointing stage, tasseling stage and maturity stage, S1N4, S1N3 and S1N2 increased by 25.76%, 22.97%, 20.74%; 25.11%, 30.02%, 23.64% and 22.47%, 28.14%, 22.71% respectively compared with S0N2.The relative abundance of Basidiomycota was significantly reduced. Alpha diversity analysis showed that the straw returning mode significantly increased the Shannon index and decreased the Simpson index, which was obvious in the jointing stage and tasseling stage. The principal coordinate analysis analysis results showed that the fungal communities formed different clusters in the horizontal and vertical directions at the three growth stages of corn jointing, tasseling and maturity. At the jointing stage and tasseling stage, the communities of the straw return treatment and the straw removal treatment were separated, and the community distribution of each treatment was not significantly different in the mature stage. Total straw returning combined with slow-release fertilizer significantly (P<0.05) increased the soil organic carbon, nitrate nitrogen and ammonia nitrogen content in each growth period, and increased the soil total nitrogen and hydrolyzable nitrogen content (P>0.05).After the straw was returned to the field, the combined application of slow-release nitrogen fertilizer and common urea had a significant impact on soil urease, catalase, and sucrase activities. Among them, the three enzyme activities were the highest in the S1N3 treatment at the jointing stage and maturity stage, and the S1N4 treatment at the tasseling stage had the highest enzyme activity. Fungal community composition is closely related to environmental factors. Soil organic carbon, urease and catalase are positively correlated with Ascomycota and negatively correlated with Basidiomycota.


Assuntos
Fertilizantes , Fungos , Nitrogênio , Microbiologia do Solo , Solo , Ureia , Zea mays , Fertilizantes/análise , Nitrogênio/análise , Solo/química , Ureia/análise , Zea mays/crescimento & desenvolvimento , Agricultura/métodos
6.
J Nanobiotechnology ; 22(1): 453, 2024 Jul 30.
Artigo em Inglês | MEDLINE | ID: mdl-39080653

RESUMO

Bioactive agents have demonstrated regenerative potential for cell-free bone tissue engineering. Nevertheless, certain challenges persist, including ineffective delivery methods and confined therapeutic potency. Here, we demonstrated that the biomimetic calcium phosphate coating system (BioCaP) could effectively uptake and slowly release the incorporated bioactive agents compared to the surface absorption system via osteoclast-mediated degradation of BioCaP coatings. The release kinetics were determined as a function of time. The release rate was stable without remarkable burst release during the first 1 day, followed by a sustained release from day 7 to day 19. Then, we developed the bi-functional BioCaP-coated silk fibroin scaffolds enabling the effective co-delivery of TGF-ß3 and BMP-2 (SFI-T/SFI-B) and the corresponding slow release of TGF-ß3 and BMP-2 exhibited superior potential in promoting chondrogenesis and osteogenesis without impairing cell vitality in vitro. The SFI-T/SFI-B scaffolds could improve cartilage and bone regeneration in 5 × 4 mm rabbit osteochondral (OC) defect. These findings indicate that the biomimetic calcium-phosphate coated silk fibroin scaffolds with slowly co-released TGF-ß3 and BMP-2 effectively promote the repair of OC defects, hence facilitating the future clinical translation of controlled drug delivery in tissue engineering.


Assuntos
Proteína Morfogenética Óssea 2 , Regeneração Óssea , Fosfatos de Cálcio , Fibroínas , Osteogênese , Engenharia Tecidual , Alicerces Teciduais , Fator de Crescimento Transformador beta3 , Fibroínas/química , Fibroínas/farmacologia , Animais , Proteína Morfogenética Óssea 2/farmacologia , Fator de Crescimento Transformador beta3/farmacologia , Fosfatos de Cálcio/química , Fosfatos de Cálcio/farmacologia , Coelhos , Alicerces Teciduais/química , Regeneração Óssea/efeitos dos fármacos , Engenharia Tecidual/métodos , Osteogênese/efeitos dos fármacos , Condrogênese/efeitos dos fármacos , Materiais Biomiméticos/química , Materiais Biomiméticos/farmacologia , Bombyx , Masculino
7.
Food Microbiol ; 121: 104524, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38637086

RESUMO

Aspergillus flavus colonization on agricultural products during preharvest and postharvest results in tremendous economic losses. Inspired by the synergistic antifungal effects of essential oils, the aims of this study were to explore the mechanism of combined cinnamaldehyde and nonanal (SCAN) against A. flavus and to evaluate the antifungal activity of SCAN loading into diatomite (DM). Shriveled mycelia were observed by scanning electron microscopy, especially in the SCAN treatment group. Calcofluor white staining, transmission electron microscopy, dichloro-dihydro-fluorescein diacetate staining and the inhibition of key enzymes in tricarboxylic acid cycle indicated that the antifungal mechanism of SCAN against A. flavus was related to the cell wall damage, reactive oxygen species accumulation and energy metabolism interruption. RNA sequencing revealed that some genes involved in antioxidation were upregulated, whereas genes responsible for cell wall biosynthesis, oxidative stress, cell cycle and spore development were significantly downregulated, supporting the occurrence of cellular apoptosis. In addition, compared with the control group, conidia production in 1.5 mg/mL DM/cinnamaldehyde, DM/nonanal and DM/SCAN groups were decreased by 27.16%, 48.22% and 76.66%, respectively, and the aflatoxin B1 (AFB1) contents decreased by 2.00%, 73.02% and 84.15%, respectively. These finding suggest that DM/SCAN complex has potential uses in food preservation.


Assuntos
Acroleína/análogos & derivados , Aldeídos , Antifúngicos , Aspergillus flavus , Antifúngicos/farmacologia , Antifúngicos/metabolismo , Aflatoxina B1/metabolismo , Conservação de Alimentos
8.
J Environ Manage ; 357: 120727, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38555844

RESUMO

The urgent concerns of controlling water body eutrophication and the alleviating phosphorus shortage have led to an urgent need for action. The removal of phosphate from polluted waters and its reuse are essential for the prevention of eutrophication and for the sustainable utilization of phosphate resources. In this study, modified attapulgite with different Ca:Mg molar ratios was synthesized to facilitate the recovery of phosphate, with subsequent use of soil fertilizer. Ca-Mg modified attapulgite with the optimal ratio (ACM-5:3) exhibited an exceptional adsorption quality, achieving a maximum adsorption capacity of 63.2 mg/g. The pseudo-second-order model and Langmuir model could well describe the adsorption kinetics and isotherms, respectively. The adsorption mechanism analyses suggested that the interaction between ACM-5:3 and phosphate depended mainly on ion exchange and electrostatic attraction. Moreover, phosphate-laden-ACM-5:3 demonstrated a significant potential as a phosphorus-releasing fertilizer. It could promote corn growth by ensuring a continuous supply of phosphorus and minimizing phosphorus runoff losses. The above results suggested that ACM-5:3 was a potential adsorbent for efficient phosphate removal and recovery.


Assuntos
Fosfatos , Compostos de Silício , Poluentes Químicos da Água , Fertilizantes , Compostos de Magnésio , Fósforo , Adsorção , Cinética , Poluentes Químicos da Água/análise
9.
J Environ Manage ; 352: 119928, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38219662

RESUMO

This review investigates the potential of nanocellulose in agriculture, encompassing its structure, synthesis, modification, and applications. Our investigation of the characteristics of nanocellulose includes a comprehensive classification of its structure. Various mechanical, chemical and enzymatic synthesis techniques are evaluated, each offering distinct possibilities. The central role of surface functionalization is thoroughly examined. In particular, we are evaluating the conventional production of nanocellulose, thus contributing to the novelty. This review is a pioneering effort to comprehensively explore the use of nanocellulose in slow and controlled release fertilizers, revolutionizing nutrient management and improving crop productivity with reduced environmental impact. Additionally, our work uniquely integrates diverse applications of nanocellulose in agriculture, ranging from slow-release fertilizers, superabsorbent cellulose hydrogels for drought stress mitigation, and long-lasting crop protection via nanocellulose-based seed coatings. The study ends by identifying challenges and unexplored opportunities in the use of nanocellulose in agriculture. This review makes an innovative contribution by being the first comprehensive study to examine the multiple applications of nanocellulose in agriculture, including slow-release and controlled-release fertilizers.


Assuntos
Proteção de Cultivos , Fertilizantes , Preparações de Ação Retardada/química , Agricultura/métodos , Hidrogéis/química
10.
Molecules ; 29(9)2024 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-38731519

RESUMO

Urban tailwater typically has a low carbon-to-nitrogen ratio and adding external carbon sources can effectively improve the denitrification performance of wastewater. However, it is difficult to determine the dosage of additional carbon sources, leading to insufficient or excessive addition. Therefore, it is necessary to prepare solid slow-release carbon source (SRC) materials to solve the difficulty in determining the dosage of carbon sources. This study selected two SRCs of slow-release carbon source 1 (SRC1) and slow-release carbon source 2 (SRC2), with good slow-release performance after static carbon release and batch experiments. The composition of SRC1 was: hydroxypropyl methylcellulose/disodium fumarate/polyhydroxy alkanoate (HPMC/DF/PHA) at a ratio of 3:2:4, with an Fe3O4 mass fraction of 3%. The composition of SRC2 was: HPMC/DF/PHA with a ratio of 1:1:1 and an Fe3O4 mass fraction of 3%. The fitted equations of carbon release curves of SRC1 and SRC2 were y = 61.91 + 7190.24e-0.37t and y = 47.92 + 8770.42e-0.43t, respectively. The surfaces of SRC1 and SRC2 had a loose and porous morphological structure, which could increase the specific surface area of materials and be more conducive to the adhesion and metabolism of microorganisms. The experimental nitrogen removal by denitrification with SRCs showed that when the initial total nitrogen concentration was 40.00 mg/L, the nitrate nitrogen (NO3--N) concentrations of the SRC1 and SRC2 groups on the 10th day were 2.57 and 2.66 mg/L, respectively. On the 20th day, the NO3--N concentrations of the SRC1 and SRC2 groups were 1.67 and 2.16 mg/L, respectively, corresponding to removal efficiencies of 95.83% and 94.60%, respectively. The experimental results indicated that SRCs had a good nitrogen removal effect. Developing these kinds of materials can provide a feasible way to overcome the difficulty in determining the dosage of carbon sources in the process of heterotrophic denitrification.

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