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Highly active biochar has great application potential in heterogeneous catalysis and adsorptive processes. The complexity of carbonization process makes it difficult to construct target active sites. This work put forward a reactive descriptor based on pyrolysis parameters and intrinsic composition of biomass. Results show that the model showed better predictive performance for C-C/C=C (R2 = 0.85), C=O (R2 = 0.85) and defect (R2 = 0.91) sites. The SHapley Additive exPlanation analysis shows that the pyrolysis parameters and the higher heating values are equally important for the active sites. The predictive performance and guiding role of the descriptor were validated by experiments. The descriptors proposed in this study integrated significant advantages of simplicity and easy accessibility, which would break the bottleneck of accurate construction of active sites and provide a theoretical basis for high-value resource utilization of biomass.
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Carbón Orgánico , Carbón Orgánico/química , Adsorción , Catálisis , Biomasa , PirólisisRESUMEN
With the rapid advancement of photopolymerization-based 3D printing technology, the volume of PCW has experienced a sharp increase. The potential environmental ramifications of PCW disposal demand careful consideration, especially given its current practice of being incineration alongside MSW. In this study, the TG-MS/FTIR system was carried out to probe the thermogravimetric characteristics and volatile byproducts during combustion. Various product compositions resulting from different mixing ratios of PCW incineration with MSW were investigated. It was observed that fluorene (C13H10) and triphenylene (C18H12) produced by PCW combustion 0.52 mg/g and 0.43 mg/g respectively, which are twice as abundant as those generated from normal plastic. When PCW incineration along with MSW, compounds such as naphthalene (C10H8), cyclohexane (C6H12), and heptane (C7H16) were generated in concentrations of 1.25 mg/g, 1.05 mg/g, and 0.95 mg/g respectively, which are at least twice as much as with MSW incineration alone. The incineration of PCW with rubber and textiles resulted in the production of 2.34 mg/g to 3.76 mg/g more PAHs compared to PCW combustion alone. The incineration of PCW with paper resulted in the production of 3.12 mg/g to 5.15 mg/g more heptane, nonane, cyclohexane, pyrene, and anthracene than PCW combustion alone. Incineration of PCW with wood proved to be the cleanest method, with product contents primarily below 0.10 mg/g. When incinerated with food residues or normal plastic, most of the product content remained below 0.05 mg/g. Considering the environmental pollution resulting from PCW combustion, the disposal of PCW warrants careful consideration and management.
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Incineración , Hidrocarburos Policíclicos Aromáticos , Impresión Tridimensional , Incineración/métodos , Hidrocarburos Policíclicos Aromáticos/análisis , Eliminación de Residuos/métodos , Fluorenos/química , Contaminantes Ambientales/análisisRESUMEN
Cleanliness has been paramount for municipal solid waste incineration (MSWI) systems. In recent years, the rapid advancement of intelligent technologies has fostered unprecedented opportunities for enhancing the cleanliness of MSWI systems. This paper offers a review and analysis of cutting-edge intelligent technologies in MSWI, which include process monitoring, intelligent algorithms, combustion control, flue gas treatment, and particulate control. The objective is to summarize current applications of these techniques and to forecast future directions. Regarding process monitoring, intelligent image analysis has facilitated real-time tracking of combustion conditions. For intelligent algorithms, machine learning models have shown advantages in accurately forecasting key process parameters and pollutant concentrations. In terms of combustion control, intelligent systems have achieved consistent prediction and regulation of temperature, oxygen content, and other parameters. Intelligent monitoring and forecasting of carbon monoxide and dioxins for flue gas treatment have exhibited satisfactory performance. Concerning particulate control, multi-objective optimization facilitates the sustainable utilization of fly ash. Despite remarkable progress, challenges remain in improving process stability and monitoring instrumentation of intelligent MSWI technologies. By systematically summarizing current applications, this timely review offers valuable insights into the future upgrade of intelligent MSWI systems.
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Biochar is a promising sorbent for Cd removal from water, while the disposal of the exhausted Cd-enriched biochar remains a challenge. In this study, pyrolysis was employed to treat the exhausted biochar under N2 and CO2 atmospheres at 600-900 °C, and the fate of Cd during pyrolysis and characteristics of high-valued products were determined. The results indicated that higher temperature and CO2 atmosphere favored the volatilization of Cd. Based on the toxicity characteristic leaching procedure (TCLP) results, the pyrolysis treatment under both atmospheres enhanced the stability of Cd, and the leached Cd concentration of regenerated biochar obtained at high temperatures (>800 °C) was lower than 1 mg/L. Compared with the pristine biochar, the regenerated biochar demonstrated higher carbon content and pH, whereas the contents of oxygen and hydrogen declined, and exhibited promising sorption properties (35.79 mg/g). The atmosphere played an important role in modifying biochar properties and syngas composition. The N2 atmosphere facilitated CH4 production, whereas the CO2 atmosphere increased the proportion of CO. These results implied that pyrolysis can be a valuable and environmental-friendly strategy for the treatment and reuse of exhausted biochar sorbent.
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Cadmio , Pirólisis , Dióxido de Carbono , Carbón Orgánico/químicaRESUMEN
Heterogeneity of pyrolytic parameters in municipal solid waste (MSW) significantly hinders its waste-to-energy efficiency. So far, hardly any light has been shed on current pyrolytic heterogeneity conditions or feasible pyrolytic homogeneity enhancement approaches of MSW. Accordingly, pyrolytic properties (Ea and logA) of 130 MSW samples in 6 categories were collected from literature. A kinetic parameters clustering-based sorting strategy for MSW was proposed. A so-called C index was established to compare their sorting performance for Ea and logA against two traditional sorting strategies (substance categorization and density clustering). Results showed that the proposed sorting strategies outperformed the traditional ones in pyrolytic homogeneity enhancement, where the optimal C_Ea and C_logA reached 1578.30 kJ/mol and 93.11 -log min. Among investigated clustering methods, k-means clustering outperformed hierarchical clustering, which could be attributed to its adaptability to the sample structure. Future perspectives involving data set expansion, model framework development, and downstream technologies matching were also discussed. The index C established in this study can be used to evaluate other clustering models.
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Pirólisis , Residuos Sólidos , Análisis por Conglomerados , Cinética , TecnologíaRESUMEN
Excavated waste is a byproduct of microbial decomposition and fermentation following landfill disposal. The effective management and utilization of excavated waste offer broad prospects for environmental and resource protection, as well as economic growth. While current research predominantly focuses on plastics in landfills, the physico-chemical properties of excavated waste over extended landfilling time remain unclear. This study aimed to address this gap by excavating waste from a landfill in Tianjin, China, with a maximum landfilling time of 18 years. The findings revealed that, compared to municipal solid waste (MSW), the excavated waste exhibited increased calorific value, ash content, and fixed carbon content after screening the landfill-mined-soil-like-fine fraction. The average calorific value of the excavated waste could reach 57.8 MJ/kg. Additionally, the oxygen content in the excavated combustible waste exceeded that of MSW, increasing from 25.59 % to 34.22 %. This phenomenon is potentially linked to the oxidation of attached soil impurities and waste. The study identified polyethylene (PE), polypropylene (PP), expanded polystyrene (EPS), polyethylene terephthalate (PET), and wood as the primary combustible components. Notably, the excavated waste exhibited a significant decrease in surface gloss, adopting a rough texture with apparent holes, potentially attributed to the acidification and corrosion of organic matter during fermentation. Nevertheless, the breaking of molecular bonds could also contribute to waste fragmentation. Furthermore, an increase in landfilling time resulted in a more pronounced decrease in mechanical properties. For instance, the failure load of PE decreased from 15.61 N to 6.46 N, and PET reduced from 884.83 N to 186.56 N. The chemical composition of excavated waste has changed, with -OH and CO observed in PE with an 18-year landfilling time. In conclusion, these results provide a theoretical foundation for the recycling of excavated waste and contribute to the advancement of waste management and recycling technologies.
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The interaction of fuel with NOx chemistry is important for the construction of the reaction mechanism and engine application. In this work, the reaction pathways of nC5H12 + NO2 were studied by high-level electronic structure calculations (DLPNO-CCSD(T)-F12/cc-pVTZ-F12//B2PLYPD3/cc-pVTZ). The rate constants were calculated by using the multistructural canonical transition-state theory with the Eckart tunneling method (TST/MS-T/ET). The studied condition is in a wide temperature range of 298-2400 K. The influence of MS-T anharmonicity and tunneling effect will be clarified for these site-specific H-abstraction pathways. The result reflects the large deviation introduced by the treatment of MS-T anharmonicity, especially at a high temperature. For the same type of reactions, the rate constants of H-abstraction both occurring at the secondary carbon are not almost identical. The branching ratios show that abstraction from the secondary site forming cis-HONO (R2c) contributes 36-78% to nC5H12 consumption in the temperature range of 298-2400 K. The current results show that the multistructural torsional anharmonicity has a crucial influence on the accurate estimation of branching ratios.
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Tar problem seriously hinders the development of biomass gasification. The tar formation of biomass is greatly influenced by cellulose. In this work, PY-GC/MS was employed for providing a precise insight into the formation of primary and secondary products, and a tar contribution index was introduced to evaluate the potential of tar formation from different origins. Combined with statistical analysis and corroboration by DFT analysis, key intermediates for tar formation are recognized, and corresponding influence is confirmed. A new framework from cellulose to tar was built. The secondary reaction acts a more important role for tar formation. The aromatic precursors and high-activity small-molecular gases are two key compounds responding to tar formation, and the existence of high-activity small-molecular gases could significantly reduce the energy barrier during tar formation. For furans, the energy barrier can be reduced from 100.2 kcal/mol to 74.2 kcal/mol in the presence of ethylene.
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Celulosa , Gases , BiomasaRESUMEN
Emerging contaminants can be removed effectively in heterogeneous Fenton-like systems. Currently, catalyst activity and contaminant removal mechanisms have been studied extensively in Fenton-like systems. However, a systematic summary was lacking. This review summarized: 1) The effects of various heterogeneous catalysts on emerging contaminants degradation by activating H2O2; 2) The role of active sites in different catalysts during the activation of H2O2 and their contribution to the generation of active species; 3) The modulation of degradation pathways of emerging contaminants. This paper will help scholars to advance the controlled construction of active sites in heterogeneous Fenton-like systems. Suitable heterogeneous Fenton catalysts can be selected in practical water treatment processes.
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Dissolved organic matters (DOM) are widely present in different water sources, causing significant effects on water treatment processes. Herein, the molecular transformation behavior of DOM during peroxymonosulfate (PMS) activation by biochar for organic degradation in a secondary effluent were comprehensively analyzed. Evolution of DOM was identified and inhibition mechanisms to organic degradation were elucidated. DOM underwent oxidative decarbonization (e.g., -C2H2O, -C2H6, -CH2 and -CO2), dehydrogenation (-2H) and dehydration reactions by ·OH and SO4·-. N and S containing compounds witnessed deheteroatomisation (e.g., -NH, -NO2+H, -SO2, -SO3, -SH2), hydration (+H2O) and N/S oxidation reactions. Among DOM, CHO-, CHON-, CHOS-, CHOP- and CHONP-containing molecules showed moderate inhibition while condensed aromatic compounds and aminosugars exhibited strong and moderate inhibition effects on contaminant degradation. The fundamental information could provide references for the rational regulation of ROS composition and DOM conversion process in a PMS system. This in turn offered theoretical guidance to minimize the interference of DOM conversion intermediates on PMS activation and degradation of target pollutants.
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Materia Orgánica Disuelta , Contaminantes Ambientales , Peróxidos , Compuestos OrgánicosRESUMEN
Due to the wide applications of polyurethane (PU), production is constantly increasing, accounting for 8% of produced plastics. PU has been regarded as the 6th most used polymer in the world. Improper disposal of waste PU will result in serious environmental consequences. The pyrolysis of polymers is one of the most commonly used disposal methods, but PU pyrolysis easily produces toxic and harmful nitrogen-containing substances due to its high nitrogen content. This paper reviews the decomposition pathways, kinetic characteristics, and migration of N-element by product distribution during PU pyrolysis. PU ester bonds break to produce isocyanates and alcohols or decarboxylate to produce primary amines, which are then further decomposed to MDI, MAI, and MDA. The nitrogenous products, including NH3, HCN, and benzene derivatives, are released by the breakage of C-C and C-N bonds. The N-element migration mechanism is concluded. Meanwhile, this paper reviews the removal of gaseous pollution from PU pyrolysis and discusses the removal mechanism in depth. Among the catalysts for pollutant removal, CaO has the most superior catalytic performance and can convert fuel-N to N2 by adsorption and dehydrogenation reactions. At the end of the review, new challenges for the utilization and high-quality recycling of PU are presented.
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Pyrolysis of oily sludge (OS) is a feasible technology to match the principle of reduction and recycling; however, it is difficult to confirm the feasible environmental destination and meet the corresponding requirements. Therefore, an integrated strategy of biochar-assisted catalytic pyrolysis (BCP) of OS and residue utilization for soil reclamation is investigated in this study. During the catalytic pyrolysis process, biochar as a catalyst intensifies the removal of recalcitrant petroleum hydrocarbons at the expense of liquid product yield. Concurrently, biochar as an adsorbent can inhibit the release of micromolecular gaseous pollutants (e.g. HCN, H2S, and HCl) and stabilize heavy metals. Due to the assistance of biochar, pyrolysis reactions of OS are more likely to occur and require a lower temperature to achieve the same situation. During the soil reclamation process, the obtained residue as a soil amendment can not only provide a carbon source and mineral nutrients but can also improve the abundance and diversity of microbial communities. Thus, it facilitates the plant germination and the secondary removal of petroleum hydrocarbons. The integrated strategy of BCP of OS and residue utilization for soil reclamation is a promising management strategy, which is expected to realize the coordinated and benign disposal of more than one waste.
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Petróleo , Suelo , Suelo/química , Aguas del Alcantarillado/química , Pirólisis , Carbón Orgánico , Aceites , HidrocarburosRESUMEN
Potassium (K) is one of the essential macronutrients for plant growth, while most agricultural soils are suffering from K deficiency worldwide. Therefore, it is a promising strategy to prepare K-enriched biochar from biomass waste. In this study, various K-enriched biochars were prepared from Canna indica at 300-700 °C by pyrolysis, co-pyrolysis with bentonite, and pelletizing-co-pyrolysis. The chemical speciation and release behaviors of K were investigated. The derived biochars showed high yields, pH values, and mineral contents, which were affected by the pyrolysis temperatures and techniques. The derived biochars contained a significant amount of K (161.3-235.7 mg/g), which was much higher than the biochars derived from agricultural residues and wood. Water-soluble K was the dominant K species in biochars with a proportion of 92.7-96.0%, and co-pyrolysis and pelletizing promoted the transformation of K to the exchangeable K and K silicates. In comparison with the C. indica derived biochars (83.3-98.0%), the bentonite-modified biochar showed a lower cumulative release proportion of K (72.5% and 72.6%) in a 28-day release test, meeting the Chinese National Standard for slow-release fertilizers. In addition, the pseudo-first order, pseudo-second order, and Elovich models well described the K release data of the powdery biochars, and the pseudo-second order model was the best fit for the biochar pellets. The modeling results indicated that the K release rate decreased after the addition of bentonite and pelletizing. These results indicated that the biochars derived from C. indica could be used as potential slow-release K fertilizers for agricultural application.
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Potasio , Zingiberales , Fertilizantes , Bentonita , Carbón Orgánico/química , Suelo/químicaRESUMEN
Rapid pyrolysis is a promising technique to convert biomass into fuel oil, where NOX emission remains a substantial environmental risk. NH3 and HCN are top precursors for NOX emission. In order to clarify their migration path and provide appropriate strategies for their controlling, six up-to-date machine learning (ML) models were established to predict the NH3 and HCN yield during rapid pyrolysis of 26 biomass feedstocks. Cross-validation and grid search methods were used to determine the optimal hyperparameters for these ML models. The support vector regression (SVR) model achieved optimal accuracy among them. The optimal root means square error (%), mean absolute error (%), and R2 of test set for NH3/HCN yield were 1.2901/1.1531, 1.0501/0.84712, and 0.98253/0.96152, respectively. In addition, based on the results of Pearson correlation analysis, the input variables with a weak linear correlation with the target product were eliminated, which was found capable of improving the prediction accuracy of almost all ML models except SVR. While after input variables elimination, the SVR model still showed the optimal NH3 and HCN yield prediction accuracy. It reflects SVR's great significance and potential for predicting the yield of NOX precursors during rapid biomass pyrolysis.
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Aprendizaje Automático , Pirólisis , BiomasaRESUMEN
Semipermeable membrane-covered composting is one of the most commonly used composting technologies in northeast China, but its humification process is not yet well understood. This study employed a semipermeable membrane-covered composting system to detect the organic matter humification and bacterial community evolution patterns over the course of agricultural waste composting. Variations in physicochemical properties, humus composition, and bacterial communities were studied. The results suggested that membrane covering improved humic acid (HA) content and degree of polymerization (DP) by 9.28% and 21.57%, respectively. Bacterial analysis indicated that membrane covering reduced bacterial richness and increased bacterial diversity. Membrane covering mainly affected the bacterial community structure during thermophilic period of composting. RDA analysis revealed that membrane covering may affect the bacterial community by altering the physicochemical properties such as moisture content. Correlation analysis showed that membrane covering activated the dominant genera Saccharomonospora and Planktosalinus to participate in the formation of HS and HA in composting, thus promoting HS formation and its structural complexity. Membrane covering significantly reduced microbial metabolism during the cooling phase of composting.
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Compostaje , Bovinos , Animales , Estiércol , Triticum , Suelo , Sustancias Húmicas/análisis , BacteriasRESUMEN
Agricultural application contributes major consumption of antibiotics worldwide. As veterinary antibiotics are poorly metabolized by animals, most of them end up in agricultural waste, which is increasingly subject to thermal treatment, such as torrefaction, pyrolysis, etc. However, there is a lack of research on their thermal decomposition mechanisms and products elucidation. Therefore, this study investigated the thermal decomposition of four major veterinary antibiotics groups (ß-lactams, tetracyclines, fluoroquinolones, sulfonamides) with emphasis on their thermal stability, structural transformation and antibacterial activity. Results show that thermal treatment can remove the parent antibiotics with their antibacterial activity except for gatifloxacin (GAT). Although the parent form of GAT was fully removed at 200 °C, its products showed significant antibacterial activity against E. coli. We present novel evidence that the PhO-CH3 chemical bond on GAT preferentially brake to generate methyl radical, which underwent a substitution reaction at the para position of phenol. This reaction also occurred during the thermal decomposition of antibiotic analogues, balofloxacin and moxifloxacin, whose thermolysis products also showed significant antibacterial activity. Furthermore, these thermolysis products may present potentially cardiotoxic and pose higher risks to human health than their parent forms, based on the comparison with a group of drugs withdrawn from the market.
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Antibacterianos , Antiinfecciosos , Animales , Humanos , Antibacterianos/química , Escherichia coli/metabolismo , Tetraciclinas , GatifloxacinaRESUMEN
Recently, Fenton-like systems have been widely explored and applied for the removal of organic matter from wastewater. Two-dimensional (2D) MXene-based materials exhibit excellent adsorption and catalysis capacity for organic pollutants removal, which has been reported widely. However, there is no summary on the application of MXene-based materials in Fenton-like systems for organic matter removal. In this review, four types of MXene-based materials were introduced, including 2D MXene, MXene/Metal complex, MXene/Metal oxide complex, and MXene/3D carbon material complex. In addition, the Fenton-like system usually consists of adsorption and degradation processes. The oxidation process might contain hydrogen peroxide (H2O2) or persulfate (PS) oxidants. This review summarizes the performance and mechanisms of organic pollutants adsorption and oxidants activation by MXene-based materials systematically. Finally, the existing problems and future research directions of MXene-based materials are proposed in Fenton-like wastewater treatment systems.
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Aguas Residuales , Contaminantes Químicos del Agua , Peróxido de Hidrógeno , Contaminantes Químicos del Agua/análisis , Oxidantes , Oxidación-ReducciónRESUMEN
A biomass gasification ash disposal method, recirculating it to gasification process, was proposed in this work. The recirculation reusability was analyzed via reusing corn straw (CS) gasification ash for six recirculation in a gasifier. Metals, especially K, got enriched in ash during ash recirculation. Under the 1st ash recirculation, CO content, H2 content and lower heating value of gas products increased from 16.02 to 19.97 vol%, from 11.30 to 15.72 vol%, from 5.38 to 6.47 MJ/Nm3, respectively. Moreover, it also exhibited an ability in tar decomposition, resulting in a tar reduction (4.63 g/Nm3 for raw CS gasification and 3.62 g/Nm3 for 1st ash recirculation). These positive effects gradually increased during the first four ash recirculation. The positive effects highly depended on the accumulation of metals (K, Na, Ca, Mg, and Fe) in ash. The positive effect did not increase as the fifth and sixth ash recirculation were conducted, resulting from the constant metals content in ash. Grey relational analysis showed that the total content of these metals was the most significant influencing parameter, followed by K content, water-soluble K content, Ca content, respectively. Moreover, pollutant SO2 could be captured by CaO during ash recirculation. This reaction competed with simultaneous CaO carbonation reaction, while it was inferior to the latter. Thus, only the first and second ash recirculation exhibited satisfactory ability in SO2 capture. In summary, ash recirculation in gasification process was feasible for upgrading gasification performance and its effect was persistent.
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Biochar (e.g. pyrochar and hydrochar) is considered a promising adsorbent for Cd removal from aqueous solution. Considering the vastly different physicochemical properties between pyrochar and hydrochar, the Cd2+ sorption capacity and mechanisms of pyrochars and hydrochars should be comparatively determined to guide the production and application of biochar. In this study, the hydrochars and pyrochars were prepared from Napier grass by hydrothermal carbonization (200 and 240 °C) and pyrolysis (300 and 500 °C), respectively, and the physicochemical properties and Cd2+ sorption performances of biochars were systematically determined. The pyrochars had higher pH and ash content as well as better stability, while the hydrochars showed more oxygen-containing functional groups (OFGs) and greater energy density. The pseudo second order kinetic model best fitted the Cd2+ sorption kinetics data of biochars, and the isotherm data of pyrochar and hydrochar were well described by Langmuir and Freundlich models, respectively. In comparison with hydrochar, the pyrochar exhibited better Cd2+ sorption capacity (up to 71.47 mg/g). With increasing production temperature, the Cd2+ sorption capacity of pyrochar elevated, while the reduction was found for hydrochar. The mineral interaction, complexation with surface OFGs, and coordination with π electron were considered the main mechanisms of Cd2+ removal by biochars. The minerals interaction and the complexation with OFGs was the dominant mechanism of Cd2+ removal by pyrochars and hydrochars, respectively. Therefore, the preparation technique and temperature have significant impacts on the sorption capacity and mechanisms of biochar, and pyrochar has better potential for Cd2+ removal than the congenetic hydrochar.
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Cadmio , Carbón Orgánico , Adsorción , Cadmio/química , Carbón Orgánico/química , Minerales , OxígenoRESUMEN
Today, domestic cats are important human companion animals for their appearance and favorable personalities. During the history of their domestication, the morphological and genetic portraits of domestic cats changed significantly from their wild ancestors, and the gut microbial communities of different breeds of cats also apparently differ. In the current study, the gut microbiota of Ragdoll cats and Felinae cats were analyzed and compared. Our data indicated that the diversity and richness of the gut microbiota in the Felinae cats were much higher than in the Ragdoll cats. The taxonomic analyses revealed that the most predominant phyla of the feline gut microbiota were Firmicutes, Bacteroidota, Fusobacteriota, Proteobacteria, Actinobacteriota, Campilobacterota, and others, while the most predominant genera were Anaerococcus, Fusobacterium, Bacteroides, Escherichia-Shigella, Finegoldia, Porphyromonas, Collinsella, Lactobacillus, Ruminococcus_gnavus_group, Prevotella, and others. Different microbial communities between the Ragdoll group and the Felinae group were observed, and the compared results demonstrated that the relative abundances of beneficial microbes (such as Lactobacillus, Enterococcus, Streptococcus, Blautia, Roseburia, and so on) in the Ragdoll group were much higher than in the Felinae group. The co-occurrence network revealed that the number of nodes and links in the Felinae group was significantly higher than the Ragdoll group, which meant that the network of the Felinae group was larger and more complex than that of the Ragdoll group. PICRUSt function analyses indicated that the differences in microbial genes might influence the energy metabolism and immune functions of the host. In all, our data demonstrated that the richness and diversity of beneficial microbes in the Ragdoll group were much higher than the Felinae group. Therefore, it is possible to isolate and identify more candidate probiotics in the gut microbiota of growing Ragdoll cats.