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1.
Gut Microbes ; 16(1): 2383353, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-39105259

RESUMO

The role of the gut microbiota in the occurrence and progression of primary biliary cholangitis (PBC) is not fully understood. First, the fecal microbiota of patients with PBC (n = 4) (PBC-FMT) or healthy individuals (n = 3) (HC-FMT) was transplanted into pseudo germ-free mice or 2OA-BSA-induced PBC models. The functions, histology and transcriptome of the liver, and microbiota and metabolome of the feces were analyzed. Second, the liver transcriptomes of PBC patients (n = 7) and normal individuals (n = 7) were analyzed. Third, the liver transcriptomes of patients with other liver diseases were collected from online databases and compared with our human and mouse data. Our results showed that PBC-FMT increased the serum ALP concentration, total bile acid content, liver injury and number of disease-related pathways enriched with upregulated liver genes in pseudo germ-free mice and increased the serum glycylproline dipeptidyl aminopeptidase level and liver damage in a 2OA-BSA-induced PBC model. The gut microbiota and metabolome differed between PBC-FMT and HC-FMT mice and reflected those of their donors. PBC-FMT tended to upregulate hepatic immune and signal transduction pathways but downregulate metabolic pathways, as in some PBC patients. The hematopoietic cell lineage, Toll-like receptor, and PPAR signaling pathway were not affected in patients with alcoholic hepatitis, HBV, HCV, HCV cirrhosis, or NASH, indicating their potential roles in the gut microbiota affecting PBC. In conclusion, the altered gut microbiota of PBC patients plays an important role in the occurrence and progression of PBC. The improvement of the gut microbiota is worthy of in-depth research and promotion as a critical aspect of PBC prevention and treatment.


Assuntos
Modelos Animais de Doenças , Fezes , Microbioma Gastrointestinal , Cirrose Hepática Biliar , Fígado , Animais , Humanos , Camundongos , Cirrose Hepática Biliar/microbiologia , Cirrose Hepática Biliar/patologia , Cirrose Hepática Biliar/metabolismo , Fígado/patologia , Fígado/metabolismo , Fígado/microbiologia , Fezes/microbiologia , Feminino , Bactérias/classificação , Bactérias/isolamento & purificação , Bactérias/genética , Transplante de Microbiota Fecal , Masculino , Ácidos e Sais Biliares/metabolismo , Transcriptoma , Camundongos Endogâmicos C57BL
2.
J Obstet Gynaecol Can ; 46(9): 102613, 2024 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-39004404
3.
Nat Commun ; 15(1): 6311, 2024 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-39060258

RESUMO

Respiratory syncytial virus (RSV) hijacks cholesterol or autophagy pathways to facilitate optimal replication. However, our understanding of the associated molecular mechanisms remains limited. Here, we show that RSV infection blocks cholesterol transport from lysosomes to the endoplasmic reticulum by downregulating the activity of lysosomal acid lipase, activates the SREBP2-LDLR axis, and promotes uptake and accumulation of exogenous cholesterol in lysosomes. High cholesterol levels impair the VAP-A-binding activity of ORP1L and promote the recruitment of dynein-dynactin, PLEKHM1, or HOPS VPS39 to Rab7-RILP, thereby facilitating minus-end transport of autophagosomes and autolysosome formation. Acidification inhibition and dysfunction of cholesterol-rich lysosomes impair autophagy flux by inhibiting autolysosome degradation, which promotes the accumulation of RSV fusion protein. RSV-F storage is nearly abolished after cholesterol depletion or knockdown of LDLR. Most importantly, the knockout of LDLR effectively inhibits RSV infection in vivo. These findings elucidate the molecular mechanism of how RSV co-regulates lysosomal cholesterol reprogramming and autophagy and reveal LDLR as a novel target for anti-RSV drug development.


Assuntos
Autofagia , Colesterol , Lisossomos , Receptores de LDL , Infecções por Vírus Respiratório Sincicial , Proteínas de Transporte Vesicular , Replicação Viral , Proteínas rab de Ligação ao GTP , proteínas de unión al GTP Rab7 , Lisossomos/metabolismo , Colesterol/metabolismo , Humanos , Animais , Receptores de LDL/metabolismo , Receptores de LDL/genética , Infecções por Vírus Respiratório Sincicial/metabolismo , Infecções por Vírus Respiratório Sincicial/virologia , Proteínas de Transporte Vesicular/metabolismo , Proteínas de Transporte Vesicular/genética , Proteínas rab de Ligação ao GTP/metabolismo , Proteínas rab de Ligação ao GTP/genética , Camundongos , Complexo Dinactina/metabolismo , Retículo Endoplasmático/metabolismo , Dineínas/metabolismo , Proteínas Adaptadoras de Transdução de Sinal/metabolismo , Proteínas Adaptadoras de Transdução de Sinal/genética , Vírus Sincicial Respiratório Humano/fisiologia , Autofagossomos/metabolismo , Proteínas Virais de Fusão/metabolismo , Proteínas Virais de Fusão/genética , Células HeLa , Células A549
4.
Chemosphere ; 362: 142676, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38936487

RESUMO

A MOF-on-MOF composite derivative material named ZIF-67@Ce-MOF-600 was designed and synthesized. The preparation of ZIF-67@Ce-MOF-600 was optimized from the aspects of the ratio of metal and ligand, heat-treatment temperature. It was demonstrated by XRD, FT-IR, SEM-EDS and TEM. The optimum conditions for the activation of PMS by ZIF-67@Ce-MOF-600 for the degradation of tetracycline (TC) were investigated by adjusting the catalyst dosage, TC, pH, peoxymonosulfate (PMS) concentration, and different kinds of water, co-existing anions and pollution. Under optimal conditions (20 mg catalysts and 50 mg PMS added) in 100 mL of tetracyclines (TC) solvent (20 mg TC/L), the removal rate could reach up to 99.2% and after five cycles was 70.5%. The EPR results indicated the presence of free radicals and non-free radical, among which free radicals intended to play a major role in the degradation process. Its possible degradation pathways and attack sites were analyzed by liquid-phase mass spectrometry and DFT analysis.


Assuntos
Estruturas Metalorgânicas , Peróxidos , Tetraciclina , Poluentes Químicos da Água , Estruturas Metalorgânicas/química , Poluentes Químicos da Água/química , Tetraciclina/química , Peróxidos/química , Purificação da Água/métodos , Catálise , Água/química
5.
Biomaterials ; 308: 122566, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38603824

RESUMO

Achieving sufficient bone regeneration in large segmental defects is challenging, with the structure of bone repair scaffolds and their loaded bioactive substances crucial for modulating the local osteogenic microenvironment. This study utilized digital laser processing (DLP)-based 3D printing technology to successfully fabricate high-precision methacryloylated polycaprolactone (PCLMA) bionic bone scaffold structures. Adipose-derived stem cell-engineered nanovesicles (ADSC-ENs) were uniformly and stably modified onto the bionic scaffold surface using a perfusion device, constructing a conducive microenvironment for tissue regeneration and long bone defect repair through the scaffold's structural design and the vesicles' biological functions. Scanning electron microscopy (SEM) examination of the scaffold surface confirmed the efficient loading of ADSC-ENs. The material group loaded with vesicles (PCLMA-BAS-ENs) demonstrated good cell compatibility and osteogenic potential when analyzed for the adhesion and osteogenesis of primary rabbit bone marrow mesenchymal stem cells (BMSCs) on the material surface. Tested in a 15 mm critical rabbit radial defect model, the PCLMA-BAS-ENs scaffold facilitated near-complete bone defect repair after 12 weeks. Immunofluorescence and proteomic results indicated that the PCLMA-BAS-ENs scaffold significantly improved the osteogenic microenvironment at the defect site in vivo, promoted angiogenesis, and enhanced the polarization of macrophages towards M2 phenotype, and facilitated the recruitment of BMSCs. Thus, the PCLMA-BAS-ENs scaffold was proven to significantly promote the repair of large segmental bone defects. Overall, this strategy of combining engineered vesicles with highly biomimetic scaffolds to promote large-segment bone tissue regeneration holds great potential in orthopedic and other regenerative medicine applications.


Assuntos
Regeneração Óssea , Células-Tronco Mesenquimais , Osteogênese , Impressão Tridimensional , Engenharia Tecidual , Alicerces Teciduais , Animais , Coelhos , Alicerces Teciduais/química , Regeneração Óssea/efeitos dos fármacos , Osteogênese/efeitos dos fármacos , Células-Tronco Mesenquimais/citologia , Engenharia Tecidual/métodos , Biônica , Poliésteres/química , Tecido Adiposo/citologia
6.
Microbiol Resour Announc ; 13(5): e0002024, 2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38591919

RESUMO

In this article, we present a comprehensive analysis of the genome sequence of Escherichia coli isolate ACESH02881hy, which has a 5,071,463-bp genome size. The strain was isolated from patient who visited the Pediatrics People's Hospital of Pingguo, China, 2021.

7.
Toxics ; 12(3)2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38535914

RESUMO

Ruthenium is required to separate from high-level liquid waste (HLLW) because Ru is a valuable resource and is negatively influential on the vitrification process of HLLW. However, the separation of Ru is very challenging due to its complicated complexation properties. In this study, the adsorption and desorption characteristics of ruthenium on a synthesized SiPyR-N3 (weak-base anion exchange resin with pyridine functional groups) composite were investigated in nitric acid and nitrite-nitric acid systems, respectively, and the adsorption mechanism was explored. The experimental results showed that SiPyR-N3 has a significantly better adsorption effect on Ru in the nitrite-nitric acid system than in the nitric acid system, with an increase in the adsorption capacity of approximately three times. The maximum adsorption capacity of Ru is 45.6 mg/g in the nitrite-nitric acid system. The SiPyR-N3 possesses good adsorption selectivity (SFRu/other metal ions is around 100) in 0.1 M NO2--0.1 M HNO3 solution. The adsorption processes of Ru in the two different systems are fitted with the pseudo-second-order kinetic model and Langmuir model for uptake kinetics and adsorption isotherms, respectively. The results obtained from the FT-IR, XPS, and UV absorption spectrometry indicate that NO2- was involved in the adsorption process either as a complexing species with the metal ions or as free NO2- from the solution. A 0.1 M HNO3 + 1 M thiourea mixed solution shows effective desorption performance, and the desorption efficiency can reach 92% at 328 K.

8.
Adv Sci (Weinh) ; 11(21): e2308381, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38447173

RESUMO

3D bioprinting techniques have enabled the fabrication of irregular large-sized tissue engineering scaffolds. However, complicated customized designs increase the medical burden. Meanwhile, the integrated printing process hinders the cellular uniform distribution and local angiogenesis. A novel approach is introduced to the construction of sizable tissue engineering grafts by employing hydrogel 3D printing for modular bioadhesion assembly, and a poly (ethylene glycol) diacrylate (PEGDA)-gelatin-dopamine (PGD) hydrogel, photosensitive and adhesive, enabling fine microcage module fabrication via DLP 3D printing is developed. The PGD hydrogel printed micocages are flexible, allowing various shapes and cell/tissue fillings for repairing diverse irregular tissue defects. In vivo experiments demonstrate robust vascularization and superior graft survival in nude mice. This assembly strategy based on scalable 3D printed hydrogel microcage module could simplify the construction of tissue with large volume and complex components, offering promise for diverse large tissue defect repairs.


Assuntos
Hidrogéis , Camundongos Nus , Impressão Tridimensional , Engenharia Tecidual , Alicerces Teciduais , Animais , Camundongos , Engenharia Tecidual/métodos , Hidrogéis/química , Alicerces Teciduais/química , Gelatina/química , Bioimpressão/métodos , Polietilenoglicóis/química , Neovascularização Fisiológica/fisiologia , Dopamina/metabolismo , Regeneração/fisiologia , Humanos
9.
Adv Rheumatol ; 64(1): 19, 2024 03 06.
Artigo em Inglês | MEDLINE | ID: mdl-38449057

RESUMO

OBJECTIVES: Rheumatoid arthritis (RA) is a chronic inflammatory joint disease, which might trigger cartilage, bone damage, and disability. Recent studies have suggested that Tetramethylpyrazine (TMP), an alkaloid monomer isolated from the rhizome of the traditional herbal medicine Ligusticum wallichii Franch, exerts a broad spectrum of pharmacological properties, containing anti-inflammatory. This study aimed to analyze the role and underlying mechanism of TMP in RA. METHODS: Under Hypoxia condition, RA-Fibroblast-like synoviocyte (FLS) were treated with TMP at different doses. Cell viability, proliferation, cell cycle progression, and migration were detected using Cell Counting Kit-8 (CCK-8) assay, 5-ethynyl-2'-deoxyuridine (EdU) assay, flow cytometry assay, wound healing assay, and transwell assay. Cyclin D1, Proliferating cell nuclear antigen (PCNA), Matrix metalloproteinase-2 (MMP2), MMP9, and hypoxia-inducible factor-1α (HIF-1α) protein levels were measured using western blot assay. Interleukin-6 (IL-6) and IL-8 were evaluated using ELISA. Circular RNA (circRNA) hsa_circ_0005178 (circCDC42BPB), CDC42BPB, and HIF-1α expression were determined using real-time quantitative polymerase chain reaction (RT-qPCR). Binding between HIF-1α and CDC42BPB promoter was predicted by JASPAR and verified using dual-luciferase reporter and Chromatin immunoprecipitation (ChIP) assays. RESULTS: TMP might hinder FLS proliferation, cycle progression, migration, and inflammatory response under hypoxic conditions. CircCDC42BPB expression was increased in RA patients and RA-FLSs treated with hypoxia, while its level was obviously reduced in RA-FLSs treated with hypoxia and TMP. TMP might abolish hypoxia-induced circCDC42BPB expression. Upregulation of circCDC42BPB might partially overturn the repression of TMP on hypoxia-caused RA-FLS damage. TMP might regulate circCDC42BPB level via HIF-1α in RA-FLSs under hypoxic conditions. CONCLUSION: TMP might block RA-FLS injury partly via regulating the HIF-1α- circCDC42BPB pathway, providing a promising therapeutic target for RA.


HIGHLIGHTS: • TMP suppressed hypoxia-induced RA-FLS growth and inflammatory response.• TMP might repress circCDC42BPB expression in RA-FLSs under hypoxic conditions.• TMP might inhibit HIF-1α-induced circCDC42BPB transcription under hypoxic conditions.


Assuntos
Artrite Reumatoide , Sinoviócitos , Humanos , Metaloproteinase 2 da Matriz , Pirazinas , Artrite Reumatoide/tratamento farmacológico , Proliferação de Células
10.
Adv Mater ; 36(26): e2401271, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38549262

RESUMO

The advancement of aqueous micro-supercapacitors offers an enticing prospect for a broad spectrum of applications, spanning from wearable electronics to micro-robotics and sensors. Unfortunately, conventional micro-supercapacitors are characterized by low capacity and slopy voltage profiles, limiting their energy density capabilities. To enhance the performance of these devices, the use of 2D MXene-based compounds has recently been proposed. Apart from their capacitive contributions, these structures can be loaded with redox-active nanowires which increase their energy density and stabilize their operation voltage. However, introducing rigid nanowires into MXene films typically leads to a significant decline in their mechanical properties, particularly in terms of flexibility. To overcome this issue, super stretchable micro-pseudocapacitor electrodes composed of MXene nanosheets and in situ reconstructed Ag nanoparticles (Ag-NP-MXene) are herein demonstrated, delivering high energy density, stable operation voltage of ≈1 V, and fast charging capabilities. Careful experimental analysis and theoretical simulations of the charging mechanism of the Ag-NP-MXene electrodes reveal a dual nature charge storage mechanism involving ad(de)sorption of ions and conversion reaction of Ag nanoparticles. The superior mechanical properties of synthesized films obtained through in situ construction of Ag-NP-MXene structure show an ultra stretchability, allowing the devices to provide stable voltage and energy output even at 100% elongation.

11.
Biotechnol J ; 19(2): e2300648, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38403408

RESUMO

L-Cysteine production through fermentation stands as a promising technology. However, excessive accumulation of L-cysteine poses a challenge due to the potential to inflict damage on cellular DNA. In this study, we employed a synergistic approach encompassing atmospheric and room temperature plasma mutagenesis (ARTP) and adaptive laboratory evolution (ALE) to improve L-cysteine tolerance in Escherichia coli. ARTP-treated populations obtained substantial enhancement in L-cysteine tolerance by ALE. Whole-genome sequencing, transcription analysis, and reverse engineering, revealed the pivotal role of an effective export mechanism mediated by gene eamB in augmenting L-cysteine resistance. The isolated tolerant strain, 60AP03/pTrc-cysEf , achieved a 2.2-fold increase in L-cysteine titer by overexpressing the critical gene cysEf during batch fermentation, underscoring its enormous potential for L-cysteine production. The production evaluations, supplemented with L-serine, further demonstrated the stability and superiority of tolerant strains in L-cysteine production. Overall, our work highlighted the substantial impact of the combined ARTP and ALE strategy in increasing the tolerance of E. coli to L-cysteine, providing valuable insights into improving L-cysteine overproduction, and further emphasized the potential of biotechnology in industrial production.


Assuntos
Cisteína , Escherichia coli , Escherichia coli/genética , Escherichia coli/metabolismo , Cisteína/metabolismo , Temperatura , Mutagênese , Fermentação
12.
J Hazard Mater ; 467: 133741, 2024 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-38341887

RESUMO

Radioactive strontium (90Sr) is considered as one of the most dangerous radionuclides due to its high biochemical toxicity. For the efficient and selective separation of Sr from acidic environments, a novel functional adsorbent CEPA@SBA-15-APTES was prepared in this work through the phosphorylation of amino-modified mesoporous silica with organic content of approximately 20 wt%. CEPA@SBA-15-APTES was characterized by TEM, SEM, EDS, TG-DSC, BET, FTIR, and XPS techniques, revealing its characteristics of an ordered hexagonal lattice-like structure and rich functional groups. The experimental results demonstrated that the adsorbent exhibited good adsorption capacity for Sr over a wide acidity range (i.e., from 10-10 M to 4 M HNO3). The adsorption equilibriums of Sr by CEPA@SBA-15-APTES in 10-6 M and 3 M HNO3 solutions were reached within 30 and 5 min, respectively, and the adsorption capacities at 318 K were 112.6 and 71.8 mg/g, respectively. Furthermore, by combining the experimental and characterization results, we found that the adsorption mechanism consisted of ion exchange between Sr(II) and H+ (in P-OH) in the 10-6 M HNO3 solution and coordination between the Sr(II) and oxygen-containing (CO and P = O) functional groups in the 3 M HNO3 solution.

13.
Environ Res ; 249: 118428, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38325788

RESUMO

Polyethelene terephthalate (PET) is a well-known thermoplastic, and recycling PET waste is important for the natural environment and human health. This study provides a comprehensive overview of the recycling and reuse of PET waste through energy recovery and physical, chemical, and biological recycling. This article summarizes the recycling methods and the high-value products derived from PET waste, specifically detailing the research progress on regenerated PET prepared by the mechanical recycling of fiber/yarn, fabric, and composite materials, and introduces the application of PET nanofibers recycled by physical dissolution and electrospinning in fields such as filtration, adsorption, electronics, and antibacterial materials. This article explains the energy recovery of PET through thermal decomposition and comprehensively discusses various chemical recycling methods, including the reaction mechanisms, catalysts, conversion efficiencies, and reaction products, with a brief introduction to PET biodegradation using hydrolytic enzymes provided. The analysis and comparison of various recycling methods indicated that the mechanical recycling method yielded PET products with a wide range of applications in composite materials. Electrospinning is a highly promising recycling strategy for fabricating recycled PET nanofibers. Compared to other methods, physical recycling has advantages such as low cost, low energy consumption, high value, simple processing, and environmental friendliness, making it the preferred choice for the recycling and high-value utilization of waste PET.


Assuntos
Polietilenotereftalatos , Reciclagem , Polietilenotereftalatos/química , Reciclagem/métodos , Biodegradação Ambiental
14.
J Environ Manage ; 353: 120283, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38330842

RESUMO

The recovery of rare earth elements (REEs) including neodymium (Nd) and dysprosium (Dy) from NdFeB permanent magnets has become one of the main ways to solve the increased demand for rare earth. Herein, n-dodecyl phosphate (DPPA) was used for the first time as the adsorption functional group donor, sodium alginate as the substrate, and calcium chloride solution as the reactive solvent, a hybrid hydrogel adsorbent DPPA/CaALG was synthesized by sol-gel method for application in the adsorption and separation of Nd and Dy from the Co-Nd-Dy ternary system. SEM-EDS, and N2 adsorption-desorption analysis showed the successful preparation of DDPA/CaALG with mesoporous structure. Batch experiments showed the superiority of the hybrid hydrogel for the good selective adsorption of Nd and Dy, such as large adsorption capacity (Nd: 162.5 mg/g, Dy: 183.5 mg/g), and no adsorption for Co. FT-IR, XPS showed that PO and P-O groups are involved in the adsorption process of Nd and Dy as electron acceptors, where the ion exchange of P-OH is dominant. Furthermore, the chemical properties of ligands and complexes were analyzed by Density Functional Theory (DFT) calculations and revealed their adsorption behaviors as well as the competition between different metal ions.


Assuntos
Metais Terras Raras , Neodímio , Disprósio , Hidrogéis , Adsorção , Alginatos , Espectroscopia de Infravermelho com Transformada de Fourier , Fosfatos
15.
Retina ; 44(6): 1100-1106, 2024 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-38232294

RESUMO

PURPOSE: To evaluate the surgical, anatomical, and functional results of "viscoelastic agent pool" technique-assisted stability of inverted internal limiting membrane flap in macular hole retinal detachment. METHODS: The innovative surgical technique was performed on 10 patients with macular hole retinal detachment. The primary outcomes included best-corrected visual acuity after surgery, rate of closure of macular hole, retinal reattachment, and occurrence of complications. RESULTS: The mean age of the individuals was 67.70 ± 8.75 (range, 55-84) years; mean axial length, 29.34 ± 1.53 (range, 27.10-30.93) mm; mean corrected MH diameter, 685.30± 345.65 (range, 172-1,325) µ m; and average follow-up period, 6.01 ± 1.71 (range, 3.10-8.4) months. In 6 eyes (60%), the postoperative best-corrected visual acuity showed improvement. All patients had macular hole closure, and the retinal reattachment rate was 100%. No postoperative complications were noted. CONCLUSION: The "viscoelastic agent pool" technique, an innovative surgical approach designed to enhance the stability of the internal limiting membrane flap, serves as an effective adjunctive procedure for the inverted internal limiting membrane flap technique. It presents a viable option for patients with macular hole retinal detachment.


Assuntos
Membrana Basal , Tamponamento Interno , Descolamento Retiniano , Perfurações Retinianas , Retalhos Cirúrgicos , Tomografia de Coerência Óptica , Acuidade Visual , Vitrectomia , Humanos , Perfurações Retinianas/cirurgia , Perfurações Retinianas/fisiopatologia , Pessoa de Meia-Idade , Idoso , Feminino , Masculino , Descolamento Retiniano/cirurgia , Descolamento Retiniano/fisiopatologia , Acuidade Visual/fisiologia , Vitrectomia/métodos , Idoso de 80 Anos ou mais , Membrana Basal/cirurgia , Tamponamento Interno/métodos , Estudos Retrospectivos , Seguimentos
16.
Dalton Trans ; 53(4): 1586-1598, 2024 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-38165017

RESUMO

Accurate separation and efficient recovery of platinum group metals (PGMs, mainly Ru, Rh and Pd) from high level liquid waste (HLLW) is a good choice for clean production and sustainable development of nuclear energy. Herein a novel SDB polymer modified silica-based amine-functionalized composite (dNbpy/SiO2-P) was synthesized for the separation and recovery of PGMs. Laser particle size analysis and BET results clarified the regular spherical and highly interconnected mesoporous structure of dNbpy/SiO2-P which is critical for the separation of PGMs. The removal percent of PGMs were over 99% on the optimized conditions. In addition, dNbpy/SiO2-P showed excellent selectivity (SFPd/M > 3805, SFRu/M > 1705, SFRh/M > 336) and repeatability (≥5). Interestingly, based on the different adsorption and desorption kinetics of PGMs, a double-column strategy is designed to solve the challenge of separating and recovering PGMs from HLLW. The enrichment factors of Pd(II), Ru(III) and Rh(III) reached 36.7, 8.2, and 1.2. The adsorption of PGMs was coordination mechanism and required the involvement of NO3- to maintain charge balance. The specific distribution of elements within the adsorbents and the changes in valence state were analyzed using depth-profiling XPS. Both depth-profiling XPS results and slope analysis revealed that the complex of dNbpy and PGMs is a 1 : 1 coordination structure. Overall, this work fills the gap that PGMs cannot be effectively separated and enriched from HLLW.

17.
Chemosphere ; 350: 141184, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38215834

RESUMO

Efficient recognition, separation and recovery of palladium from high-level liquid waste (HLLW) not only helps the safe, green and environmentally friendly disposal of nuclear waste, but also is an essential important supplement to overcome the growing shortage of natural palladium resources. Herein, a novel silica-based functional adsorbent named 2AT-SiAaC was prepared by a two-step method, i.e., grafting of 2-aminothiazole (2AT) via the amidated reaction after in-situ polymerization of acrylic monomers on porous silica. SEM, EDS, TG-DSC, BET and PXRD all proved the successful preparation of 2AT-SiAaC, and it exhibited ultrahigh adsorption selectivity for Pd(II) (Kd (distribution coefficient) ≥ 10,344.2 mL/g, SFPd/M (separation factor) ≥ 613.7), fast adsorption kinetics with short equilibrium time (t ≤ 1 h) and good adsorption capacity (Q ≥ 62.1 mg Pd/g). The dynamic column experiments shows that 2AT-SiAaC achieved efficiently separation of Pd(II) from simulated HLLW, and the enrichment coefficients (C/C0) of Pd(II) was as high as about 14 with the recovery rate nearly 99.9% and basically kept the same performance in three adsorption-desorption column cycle experiments. The adsorption mechanism was analyzed by FT-IR, XPS and DFT calculations, and the ultrahigh selectivity of 2AT-SiAaC was attributed to the preferred affinity of the soft N-donor atoms in 2AT for Pd(II). NO3- ions participated in the adsorption reaction to keep charge balance, and the frontier orbital electron density distribution diagram shows the charge transfer in the process of material preparation and adsorption. To sum up, 2AT-SiAaC adsorbent provided a new insight for precise recognition and efficient separation of Pd(II) from HLLW.


Assuntos
Paládio , Tiazóis , Poluentes Químicos da Água , Paládio/análise , Dióxido de Silício , Espectroscopia de Infravermelho com Transformada de Fourier , Adsorção , Cinética
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