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1.
Chem Commun (Camb) ; 60(24): 3287-3290, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38421350

RESUMO

Frustrated Lewis pair (FLP) hydrogenation catalysts predominantly use alkyl- and aryl-substituted Lewis acids (LA) that offer a limited number of combinations of substituents, limiting our ability to tune their properties and, ultimately, their reactivity. Nevertheless, main-group complexes have numerous ligands available for such purposes, which could enable us to broaden the range of FLP catalysis. Supporting this hypothesis, we demonstrate here that hexacoordinated tin complexes with Schiff base ligands catalyse imine hydrogenation via activation of H2(g). As shown by hydrogen-deuterium scrambling, [Sn(tBu2Salen)(OTf)2] activated H2(g) at 25 °C and 10 bar of H2. After tuning the ligands, we found that [Sn(Salen)Cl2] was the most efficient imine hydrogenation catalyst despite having the lowest activity in H2(g) activation. Moreover, various imines were hydrogenated in yields up to 98% thereby opening up opportunities for developing novel FLP hydrogenation catalysts based on hexacoordinated LA of main-group elements.

2.
Sci Total Environ ; 816: 151662, 2022 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-34780822

RESUMO

Per- and polyfluorinated alkyl substances (PFASs) represent a group of highly recalcitrant micropollutants, that continuously endanger the environment. The present work describes the geographical trends of fish contamination by individual PFASs (including new compounds, e.g., Gen-X) assessed by analyzing the muscle tissues of 5 separate freshwater fish species from 10 locations on the Czech section of the Elbe River and its largest tributary, the Vltava River. The data of this study also showed that the majority of the detected PFASs consisted of long-chain representatives (perfluorooctane sulfonate (PFOS), perfluorononanoic acid, perfluorodecanoic acid, and perfluoroundecanoic acid), whereas short-chain PFASs as well as other compounds such as Gen-X were detected in relatively small quantities. The maximum concentrations of the targeted 32 PFASs in fish were detected in the lower stretches of the Vltava and Elbe Rivers, reaching 289.9 ng/g dw, 140.5 ng/g dw, and 162.7 ng/g dw for chub, roach, and nase, respectively. Moreover, the relationships between the PFAS (PFOS) concentrations in fish muscle tissue and isotopic ratios (δ15N and δ13C) were studied to understand the effect of feed composition and position in the river continuum as a proxy for anthropogenic activity. Redundancy analysis and variation partitioning showed that the largest part of the data variability was explained by the interaction of position in the river continuum and δ15N (δ13C) of the fish. The PFAS concentrations increased downstream and were positively correlated with δ15N and negatively correlated with δ13C. A detailed study at one location also demonstrated the significant relationship between δ15N (estimated trophic position) and PFASs (PFOS) concentrations. From the tested physicochemical properties, the molecular mass and number of fluorine substituents seem to play crucial roles in PFAS bioaccumulation.


Assuntos
Ácidos Alcanossulfônicos , Cyprinidae , Poluentes Ambientais , Fluorocarbonos , Poluentes Químicos da Água , Ácidos Alcanossulfônicos/análise , Animais , Monitoramento Ambiental , Fluorocarbonos/análise , Rios , Poluentes Químicos da Água/análise
3.
Front Microbiol ; 12: 676251, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34163452

RESUMO

Elucidating dynamics of soil microbial communities after disturbance is crucial for understanding ecosystem restoration and sustainability. However, despite the widespread practice of swidden agriculture in tropical forests, knowledge about microbial community succession in this system is limited. Here, amplicon sequencing was used to investigate effects of soil ages (spanning at least 60 years) after disturbance, geographic distance (from 0.1 to 10 km) and edaphic property gradients (soil pH, conductivity, C, N, P, Ca, Mg, and K), on soil bacterial and fungal communities along a chronosequence of sites representing the spontaneous succession following swidden agriculture in lowland forests in Papua New Guinea. During succession, bacterial communities (OTU level) as well as its abundant (OTU with relative abundance > 0.5%) and rare (<0.05%) subcommunities, showed less variation but more stage-dependent patterns than those of fungi. Fungal community dynamics were significantly associated only with geographic distance, whereas bacterial community dynamics were significantly associated with edaphic factors and geographic distance. During succession, more OTUs were consistently abundant (n = 12) or rare (n = 653) for bacteria than fungi (abundant = 6, rare = 5), indicating bacteria were more tolerant than fungi to environmental gradients. Rare taxa showed higher successional dynamics than abundant taxa, and rare bacteria (mainly from Actinobacteria, Proteobacteria, Acidobacteria, and Verrucomicrobia) largely accounted for bacterial community development and niche differentiation during succession.

4.
FEMS Microbiol Ecol ; 97(5)2021 05 10.
Artigo em Inglês | MEDLINE | ID: mdl-33899919

RESUMO

Microbial interconnections in soil are pivotal to ecosystem services and restoration. However, little is known about how soil microbial interconnections respond to slash-and-burn agriculture and to the subsequent ecosystem restoration after the practice. Here, we used amplicon sequencing and co-occurrence network analyses to explore the interconnections within soil bacterial and fungal communities in response to slash-and-burn practice and a spontaneous restoration (spanning ca. 60 years) of tropical forests after the practice, in Papua New Guinea. We found significantly higher complexity and greater variations in fungal networks than in those of bacteria, despite no significant changes observed in bacterial or fungal networks across successional stages. Within most successional stages, bacterial core co-occurrences (co-occurrences consistently present across all sub-networks in a stage) were more frequent than those of fungi, indicating higher stability of interconnections between bacteria along succession. The stable interconnections occurred frequently between bacterial taxa (i.e. Sporosarcina, Acidimicrobiale and Bacillaceae) and between ectomycorrhizal fungi (Boletaceae and Russula ochroleuca), implying important ecological roles of these taxa in the ecosystem restoration. Collectively, our results provide new insight into microbial interconnections in response to slash-and-burn agriculture and the subsequent ecosystem restoration, thus promoting a better understanding of microbial roles in ecosystem services and restoration.


Assuntos
Queimaduras , Solo , Agricultura , Basidiomycota , Ecossistema , Florestas , Fungos/genética , Humanos , Papua Nova Guiné , Microbiologia do Solo
5.
Mycorrhiza ; 27(8): 775-789, 2017 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-28752181

RESUMO

The arbuscular mycorrhizal (AM) grass Calamagrostis epigejos and predominantly ectomycorrhizal (EcM) tree Salix caprea co-occur at post-mining sites spontaneously colonized by vegetation. During succession, AM herbaceous vegetation is replaced by predominantly EcM woody species. To better understand the interaction of AM and EcM plants during vegetation transition, we studied the reciprocal effects of these species' coexistence on their root-associated fungi (RAF). We collected root and soil samples from three different microenvironments: stand of C. epigejos, under S. caprea canopy, and contact zone where roots of the two species interacted. RAF communities and mycorrhizal colonization were determined in sampled roots, and the soil was tested for EcM and AM inoculation potentials. Although the microenvironment significantly affected composition of the RAF communities in both plant species, the effect was greater in the case of C. epigejos RAF communities than in that of S. caprea RAF communities. The presence of S. caprea also significantly decreased AM fungal abundance in soil as well as AM colonization and richness of AM fungi in C. epigejos roots. Changes observed in the abundance and community composition of AM fungi might constitute an important factor in transition from AM-dominated to EcM-dominated vegetation during succession.


Assuntos
Ecossistema , Micorrizas/fisiologia , Poaceae/microbiologia , Salix/microbiologia , Microbiologia do Solo , República Tcheca , Árvores/microbiologia
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