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1.
Angew Chem Int Ed Engl ; 63(23): e202402435, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38566410

RESUMO

Strong metal-support interaction (SMSI) is widely proposed as a key factor in tuning catalytic performances. Herein, the classical SMSI between Au nanoparticles (NPs) and BiVO4 (BVO) supports (Au/BVO-SMSI) is discovered and used innovatively for photoelectrochemical (PEC) water splitting. Owing to the SMSI, the electrons transfer from V4+ to Au NPs, leading to the formation of electron-rich Au species (Auδ-) and strong electronic interaction (i.e., Auδ--Ov-V4+), which readily contributes to extract photogenerated holes and promote charge separation. Benefitted from the SMSI effect, the as-prepared Au/BVO-SMSI photoanode exhibits a superior photocurrent density of 6.25 mA cm-2 at 1.23 V versus the reversible hydrogen electrode after the deposition of FeOOH/NiOOH cocatalysts. This work provides a pioneering view for extending SMSI effect to bimetal oxide supports for PEC water splitting, and guides the interfacial electronic and geometric structure modulation of photoanodes consisting of metal NPs and reducible oxides for improved solar energy conversion efficiency.

2.
Angew Chem Int Ed Engl ; : e202405594, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38638107

RESUMO

Conjugated polymers with tailorable composition and microarchitecture are propitious for modulating catalytic properties and deciphering inherent structure-performance relationships. Herein, we report a facile linker engineering strategy to manipulate the electronic states of metallophthalocyanine conjugated polymers and uncover the vital role of organic linkers in facilitating electrocatalytic oxygen reduction reaction (ORR). Specifically, a set of cobalt phthalocyanine conjugated polymers (CoPc-CPs) wrapped onto carbon nanotubes (denoted CNTs@CoPc-CPs) are judiciously crafted via in situ assembling square-planar cobalt tetraaminophthalocyanine (CoPc(NH2)4) with different linear aromatic dialdehyde-based organic linkers in the presence of CNTs. Intriguingly, upon varying the electronic characteristic of organic linkers from terephthalaldehyde (TA) to 2,5-thiophenedicarboxaldehyde (TDA) and then to thieno/thiophene-2,5-dicarboxaldehyde (bTDA), their corresponding CNTs@CoPc-CPs exhibit gradually improved electrocatalytic ORR performance. More importantly, theoretical calculations reveal that the charge transfer from CoPc units to electron-withdrawing linkers (i.e., TDA and bTDA) drives the delocalization of Co d-orbital electrons, thereby downshifting the Co d-band energy level. Accordingly, the active Co centers with more positive valence state exhibit optimized binding energy toward ORR-relevant intermediates and thus a balanced adsorption/desorption pathway that endows significant enhancement in electrocatalytic ORR. This work demonstrates a molecular-level engineering route for rationally designing efficient polymer catalysts and gaining insightful understanding of electrocatalytic mechanisms.

3.
Chem Commun (Camb) ; 60(27): 3661-3664, 2024 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-38456200

RESUMO

Homogeneous integration of ultrafine TiO2 nanoparticles into a conductive sulfur-doped carbon skeleton was readily crafted by unusual space-confined twin-polymerization of a titanium-containing single-source coupled monomer and subsequent carbonization, producing a robust hetero-architecture for boosting lithium storage with large reversible capacity, high rate capability, and long-term cycling stability.

4.
Angew Chem Int Ed Engl ; 63(19): e202401253, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38491764

RESUMO

Cyano-containing electrodes usually promise high theoretical potentials while suffering from uncontrollable self-dissolution and sluggish reaction kinetics. Herein, to remedy their limitations, an unprecedented core-shell heterostructured electrode of carbon nanotubes encapsulated in poly(1,4-dicyanoperfluorobenzene sulfide) (CNT@PFDCB) is rationally crafted via molecule and microstructure modulations. Specifically, the linkage of sulfide bridges of PFDCB prevents the active cyano groups from dissolving, resulting in a robust structure. The fluorinations modulate the electronic configurations in frontier orbitals, allowing higher electrical conductivity and elevated output voltage. Combined with the core-shell architecture to unlock the sluggish diffusion kinetics for both electrons and guest ions, the CNT@PFDCB exhibits an impressive capacity (203.5 mAh g-1), remarkable rate ability (127.6 mAh g-1 at 3.0 A g-1), and exceptional cycling stability (retaining 81.1 % capacity after 3000 cycles at 1.0 A g-1). Additionally, the Li-storage mechanisms regarding PFDCB are thoroughly revealed by in situ attenuated total reflection infrared spectroscopy, in situ Raman spectroscopy, and theoretical simulations, which involve the coordination interaction between Li ions and cyano groups and the electron delocalization along the conjugated skeleton. More importantly, a practical fully organic cell based on the CNT@PFDCB is well-validated that demonstrates a tremendous potential of cyanopolymer as the cathode to replace its inorganic counterparts.

5.
Front Microbiol ; 15: 1275865, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38419639

RESUMO

Introduction: The dietary protein level plays a crucial role in maintaining the equilibrium of rumen microbiota in yaks. To explore the association between dietary protein levels, rumen microbiota, and muscle metabolites, we examined the rumen microbiome and muscle metabolome characteristics in yaks subjected to varying dietary protein levels. Methods: In this study, 36 yaks were randomly assigned to three groups (n = 12 per group): low dietary protein group (LP, 12% protein concentration), medium dietary protein group (MP, 14% protein concentration), and high dietary protein group (HP, 16% protein concentration). Results: 16S rDNA sequencing revealed that the HP group exhibited the highest Chao1 and Observed_species indices, while the LP group demonstrated the lowest. Shannon and Simpson indices were significantly elevated in the MP group relative to the LP group (P < 0.05). At the genus level, the relative abundance of Christensenellaceae_R-7_group in the HP group was notably greater than that in the LP and MP groups (P < 0.05). Conversely, the relative abundance of Rikenellaceae_RC9_gut_group displayed an increasing tendency with escalating feed protein levels. Muscle metabolism analysis revealed that the content of the metabolite Uric acid was significantly higher in the LP group compared to the MP group (P < 0.05). The content of the metabolite L-(+)-Arabinose was significantly increased in the MP group compared to the HP group (P < 0.05), while the content of D-(-)-Glutamine and L-arginine was significantly reduced in the LP group (P < 0.05). The levels of metabolites 13-HPODE, Decanoylcarnitine, Lauric acid, L-(+)-Arabinose, and Uric acid were significantly elevated in the LP group relative to the HP group (P < 0.05). Furthermore, our observations disclosed correlations between rumen microbes and muscle metabolites. The relative abundance of NK4A214_group was negatively correlated with Orlistat concentration; the relative abundance of Christensenellaceae_R-7_group was positively correlated with D-(-)-Glutamine and L-arginine concentrations. Discussion: Our findings offer a foundation for comprehending the rumen microbiome of yaks subjected to different dietary protein levels and the intimately associated metabolic pathways of the yak muscle metabolome. Elucidating the rumen microbiome and muscle metabolome of yaks may facilitate the determination of dietary protein levels.

6.
Chem Soc Rev ; 53(3): 1447-1494, 2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38164808

RESUMO

Cost-effective and high-efficiency catalysts play a central role in various sustainable electrochemical energy conversion technologies that are being developed to generate clean energy while reducing carbon emissions, such as fuel cells, metal-air batteries, water electrolyzers, and carbon dioxide conversion. In this context, a recent climax in the exploitation of advanced earth-abundant catalysts has been witnessed for diverse electrochemical reactions involved in the above mentioned sustainable pathways. In particular, polymer catalysts have garnered considerable interest and achieved substantial progress very recently, mainly owing to their pyrolysis-free synthesis, highly tunable molecular composition and microarchitecture, readily adjustable electrical conductivity, and high stability. In this review, we present a timely and comprehensive overview of the latest advances in organic polymers as emerging materials for powerful electrocatalysts. First, we present the general principles for the design of polymer catalysts in terms of catalytic activity, electrical conductivity, mass transfer, and stability. Then, the state-of-the-art engineering strategies to tailor the polymer catalysts at both molecular (i.e., heteroatom and metal atom engineering) and macromolecular (i.e., chain, topology, and composition engineering) levels are introduced. Particular attention is paid to the insightful understanding of structure-performance correlations and electrocatalytic mechanisms. The fundamentals behind these critical electrochemical reactions, including the oxygen reduction reaction, hydrogen evolution reaction, CO2 reduction reaction, oxygen evolution reaction, and hydrogen oxidation reaction, as well as breakthroughs in polymer catalysts, are outlined as well. Finally, we further discuss the current challenges and suggest new opportunities for the rational design of advanced polymer catalysts. By presenting the progress, engineering strategies, insightful understandings, challenges, and perspectives, we hope this review can provide valuable guidelines for the future development of polymer catalysts.

7.
Free Radic Biol Med ; 209(Pt 1): 70-83, 2023 11 20.
Artigo em Inglês | MEDLINE | ID: mdl-37806597

RESUMO

The gut microbiota plays a crucial role in maintaining host nutrition, metabolism, and immune homeostasis, particularly in extreme environmental conditions. However, the regulatory mechanisms of the gut microbiota in animal organisms hypobaric hypoxia exposure require further study. We conducted a research by comparing SD rats treated with an antibiotic (ABX) cocktail and untreated SD rats that were housed in a low-pressure oxygen chamber (simulating low pressure and hypoxic environment at 6000 m altitude) for 30 days. After the experiment, blood, feces, and lung tissues from SD rats were collected for analysis of blood, 16S rRNA amplicon sequencing, and non-targeted metabolomics. The results demonstrated that the antibiotic cocktail-treated SD rats exhibited elevated counts of neutrophil (Neu) and monocyte (Mon) cells, an enrichment of sulfate-reducing bacteria (SBC), reduced levels of glutathione, and accumulated phospholipid compounds. Notably, the accumulation of phospholipid compounds, particularly lysophosphatidic acid (LPA), lipopolysaccharide (LPS), and lysophosphatidylcholine (LPC), along with the aforementioned changes, contributed to heightened oxidative stress and inflammation in the organism. In addition, we explored the resistance mechanisms of SD rats in low-oxygen and low-pressure environments and found that increasing the quantity of the Prevotellaceae and related beneficial bacteria (especially Lactobacillus) could reduce oxidative stress and inflammation. These findings offer valuable insights into enhancing the adaptability of low-altitude animals under hypobaric hypoxia exposure.


Assuntos
Hipóxia , Estresse Oxidativo , Ratos , Animais , RNA Ribossômico 16S/genética , Ratos Sprague-Dawley , Hipóxia/tratamento farmacológico , Hipóxia/metabolismo , Oxigênio , Inflamação , Fosfolipídeos
8.
Nanomicro Lett ; 15(1): 232, 2023 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-37861885

RESUMO

Regulating the local configuration of atomically dispersed transition-metal atom catalysts is the key to oxygen electrocatalysis performance enhancement. Unlike the previously reported single-atom or dual-atom configurations, we designed a new type of binary-atom catalyst, through engineering Fe-N4 electronic structure with adjacent Co-N2C2 and nitrogen-coordinated Co nanoclusters, as oxygen electrocatalysts. The resultant optimized electronic structure of the Fe-N4 active center favors the binding capability of intermediates and enhances oxygen reduction reaction (ORR) activity in both alkaline and acid conditions. In addition, anchoring M-N-C atomic sites on highly graphitized carbon supports guarantees of efficient charge- and mass-transports, and escorts the high bifunctional catalytic activity of the entire catalyst. Further, through the combination of electrochemical studies and in-situ X-ray absorption spectroscopy analyses, the ORR degradation mechanisms under highly oxidative conditions during oxygen evolution reaction processes were revealed. This work developed a new binary-atom catalyst and systematically investigates the effect of highly oxidative environments on ORR electrochemical behavior. It demonstrates the strategy for facilitating oxygen electrocatalytic activity and stability of the atomically dispersed M-N-C catalysts.

9.
Microorganisms ; 11(8)2023 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-37630524

RESUMO

A relatively stable microbial ecological balance system in the rumen plays an important role in rumen environment stability and ruminant health maintenance. No studies have reported how rumen fluid transplantation (RFT) affects the composition of rumen microorganisms and yak growth performance. In this experiment, we transplanted fresh rumen fluid adapted to house-feeding yaks to yaks transitioned from natural pastures to house-feeding periods to investigate the effects of rumen fluid transplantation on rumen microbial community regulation and production performance. Twenty yaks were randomly divided into the control group (CON; n = 10) and the rumen fluid transplantation group (RT; n = 10). Ten yaks that had been adapted to stall fattening feed in one month were selected as the rumen fluid donor group to provide fresh rumen fluid. Ruminal fluid transplantation trials were conducted on the 1st, 3rd, and 5th. Overall, 1 L of ruminal fluid was transplanted to each yak in the RT and CON group. The formal trial then began with both groups fed the same diet. After this, growth performance was measured, rumen fluid was collected, and rumen microbial composition was compared using 16s rRNA sequencing data. The results showed that rumen fluid transplantation had no significant effect on yak total weight gain or daily weight gain (p > 0.05), and feed efficiency was higher in the RT group than in the CON group at 3 months (treatment × month: p < 0.01). Ruminal fluid transplantation significantly affected rumen alpha diversity (p < 0.05). Up to day 60, the RT group had significantly higher OTU numbers, Shannon diversity, and Simpson homogeneity than the CON group. Principal coordinate analysis showed that the rumen microbiota differed significantly on days 4 and 7 (p < 0.05). Bacteroidota, Firmicutes, Proteobacteria, and Spirochaetes were the most abundant phyla in the rumen. The relative abundances of Bacteroidota, Proteobacteria, and Spirochaetes were lower in the RT group than in the CON group, with a decrease observed in Bacteroidota in the RT group on days 7 and 28 after rumen fluid transplantation (p = 0.013), while Proteobacteria showed a decreasing trend in the CON group and an increasing trend in RT; however, this was only at day 4 (p = 0.019). The relative abundance of Firmicutes was significantly higher in the RT group than in the CON group on days 4, 7, and 28 (p = 0.001). Prevotella and Rikenellaceae_RC9_gut_group were the predominant genera. In conclusion, our findings suggest that rumen fluid transplantation improves yak growth performance and rumen microbial reshaping. The findings of this study provide new insights into yak microbial community transplantation and a reference for improving feed efficiency in the yak industry.

10.
Chem Commun (Camb) ; 59(8): 1082-1085, 2023 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-36621890

RESUMO

In situ polymerization of acrylonitrile and graphene oxide in combination with thermal treatment was readily performed to produce robust hierarchical hybrids containing flower-like oxidized-polyacrylonitrile, which synergistically couple conductive graphene and a multi-electron redox-active matrix, affording large reversible capacity, high rate capability, and long cycle life toward cost-efficient and sustainable batteries.


Assuntos
Grafite , Lítio , Resinas Acrílicas , Eletrodos , Íons
11.
Front Microbiol ; 13: 957152, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36246255

RESUMO

Ruminal microflora is closely correlated with the ruminant's diet. However, information regarding the effect of high concentrate diets on rumen microflora in yaks is lacking. In the current study, 24 healthy male yaks were randomly assigned to two groups, each fed with different diets: less concentrate (LC; concentrate: coarse = 40: 60) and high concentrate (HC; concentrate: coarse = 80: 20) diets. Subsequently, a 21-day feeding trial was performed with the yaks, and rumen fluid samples were collected and compared using 16 s rRNA sequencing. The results showed that NH3-N, total VFA, acetate, butyrate, isobutyrate, and isovalerate were significantly higher in the HC group than that in the LC group (p < 0.05), while microbial diversity and richness were significantly lower in the HC group (p < 0.05). Principal coordinate analysis indicated that rumen microflora was significantly different in LC and HC groups (p < 0.05). In the rumen, phyla Firmicutes and Bacteroidota were the most abundant bacteria, with Firmicutes being more abundant, and Bacteroidota being less abundant in the HC group than those found in the LC group. Christensenellaceae_R-7_group and Prevotella are the highest abundant ones at the genus level. The relative abundance of Acetitomaculum, Ruminococcus, and Candidatus_Saccharimonas were significantly higher in the HC group than that in the LC group (p < 0.05), while the relative abundance of Olsenella was significantly lower in the HC group than in the LC group (p < 0.05). Compared to the LC group, the relative abundance of Prevotella, Ruminococcus, and Candidatus_Saccharimonas was significantly higher in the HC group. The relative abundances of Prevotella, Prevotellaceae_UCG-003, Olsenella, Ruminococcus, Acetitomaculum, Candidatus_Saccharimonas, and NK4A214_group were correlated with ruminal fermentation parameters (p < 0.05). Furthermore, PICRUSt 2 estimation indicated that microbial genes associated with valine, leucine, and isoleucine biosynthesis were overexpressed in the rumen microflora of yaks in the HC group (p < 0.05). Conclusively, our results suggest that high concentrate diets affect the microflora composition and fermentation function in yak rumen. The present findings would provide new insights into the health of yaks under high concentrate feeding conditions and serve as a potent reference for the short-term fattening processes of yaks.

12.
Animals (Basel) ; 12(18)2022 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-36139194

RESUMO

(1) Background: This study aimed to investigate the effects of different dietary concentrate to roughage ratios on growth performance and fecal microbiota composition of yaks by 16S rRNA gene sequencing. (2) Methods: In the present study, three diets with different dietary forage-to-concentrate ratios (50:50, 65:35, and 80:20) were fed to 36 housed male yaks. (3) Results: The result shows that Final BW, TWG, and ADG were higher in the C65 group than in the C50 and C80 groups, but the difference was not significant (p > 0.05). DMI in the C65 group was significantly higher than in the other two groups (p < 0.05). The DMI/ADG of the C65 group was lower than that of the other two groups, but the difference was insignificant (p > 0.05). At the phylum level, Firmicutes were the most abundant in the C65 group, and the relative abundance of Bacteroidetes was lower in the C65 group than in the other two groups. At the genus level, the relative abundances of Ruminococcaceae_UCG_005, Romboutsia, and Christensenellaceae_R-7 were higher in the C56 group than in the C50 and C80 groups. The relative abundance of Lachnospiraceae_NK3A20 and Rikenellaceaewas_RC9_gut is lower in the C65 group, but the difference was insignificant (p > 0.05). At KEGG level 2, the relative abundance of lipid metabolism and energy metabolism were lowest in the C50 group, and both showed higher relative abundance in the C65 group. (4) Conclusions: In conclusion, the structure of fecal microbiota was affected by different concentrate-to-forage ratios. We found that feeding diets with a concentrate-to-forage ratio of 65:35 improved yaks' growth and energy metabolism.

13.
Front Microbiol ; 13: 964564, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36033892

RESUMO

To improve the rumen fermentation function and growth performance of yaks (Bos grunniens), better understanding of the effect of different dietary forage to concentrate ratios on rumen microbiota and metabolites is needed. In the present study, three diets with different dietary forage to concentrate ratios (50:50, 65:35, and 80:20) were fed to 36 housed male yaks. The changes in the distribution of rumen microorganisms and metabolites and the interactions between them were studied by 16S rRNA gene sequencing and liquid chromatography-mass spectrometry (LC-MS). The diversity and richness of microorganisms in the rumen varied according to diet. The most abundant phyla were Firmicutes and Bacteroidetes. Firmicutes was the most abundant in the C50 group, and the relative abundance of Bacteroidetes was significantly lower in the C65 group than in the C80 group (p < 0.05). The Christensenellaceae_R-7_group, Rikenellaceae_RC9_gut_group, and Methanobrevibacter had the highest relative abundances at the genus level. Among them, Christensenellace_R-7_group had the highest relative abundance in the C50 group. The Rikenellaceae_RC9_gut_group was significantly abundant in the C80 group compared with the C50 group. The Methanobrevibacter content was higher in the C65 group than in the other two groups. Both the concentration and metabolic pathways of rumen metabolites were influenced by the dietary concentrate ratio; lipids, lipid-like molecules, organic acid metabolites, and organic oxide-related metabolites differed between the groups. Significant changes were found for six metabolic pathways, including arginine and proline metabolism; glycine, serine, and threonine metabolism; glyoxylate and dicarboxylate metabolism; arginine biosynthesis; glycerophospholipid metabolism; glycerolipid metabolism; and nitrogen metabolism.

14.
Chem Commun (Camb) ; 58(62): 8622-8625, 2022 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-35822672

RESUMO

Herein, we report a robust strategy to markedly promote charge separation and transfer via electrodepositing ZnO nanosheets into a cross-linked porous three-dimensional reduced graphene oxide (3DrGO) network structure to form a ZnO/3DrGO photoanode. In addition to the high electrical conductivity and 3D porous architecture, the photothermal effect of 3DrGO activated by a near-infrared (NIR) laser or NIR light of solar radiation can be used to increase the temperature of the photoanodes in situ, further enhancing the charge transfer efficiency of ZnO nanosheets. With the synergistic effect of 3DrGO, the photocurrent density of the ZnO/3DrGO photoanode (2.03 mA cm-2) is about three times higher than that of the pure ZnO photoanode (0.51 mA cm-2) at 1.23 V vs. reversible reference electrode (VRHE). This work provides an effective strategy for improving the PEC water splitting performance of photoanodes via the incorporation of multifunctional 3D porous architecture rGO.

15.
Nano Converg ; 9(1): 34, 2022 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-35867176

RESUMO

Single-metal-atom catalysts (SMACs) have garnered extensive attention for various electrocatalytic applications, owing to their maximum atom-utilization efficiency, tunable electronic structure, and remarkable catalytic performance. In particular, carbon-based SMACs exhibit optimal electrocatalytic activity for the oxygen reduction reaction (ORR) which is of paramount importance for several sustainable energy conversion and generation technologies, such as fuel cells and metal-air batteries. Despite continuous endeavors in developing various advanced carbon-based SMACs for electrocatalytic ORR, the rational regulation of coordination structure and thus the electronic structure of carbon-based SMACs remains challenging. In this review, we critically examine the role of coordination structure, including local coordination structure (i.e., metal atomic centers and the first coordination shell) and extended local coordination structure (i.e., the second and higher coordination shells), on the rational design of carbon-based SMACs for high-efficiency electrocatalytic ORR. Insights into the relevance between coordination structures and their intrinsic ORR activities are emphatically exemplified and discussed. Finally, we also propose the major challenges and future perspectives in the rational design of advanced carbon-based SMACs for electrocatalytic ORR. This review aims to emphasize the significance of coordination structure and deepen the insightful understanding of structure-performance relationships.

16.
Animals (Basel) ; 12(11)2022 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-35681862

RESUMO

This study aimed to evaluate the effects of concentrate supplementation on the growth performance, serum biochemical parameters, rumen fermentation, and bacterial community composition of grazing yaks during the warm season. Eight male yaks (body weight, 123.96 ± 7.43 kg; 3-years) were randomly allocated to two treatments groups: grazing (n = 4, GY) and concentrate supplement group (n = 4, GYS). Concentrate supplementation increased the average daily gain (ADG) (p < 0.05). Glucose (GLU), total protein (TP), and aspartate aminotransferase (AST) serum concentrations were significantly higher in the GYS group than in the GY group (p < 0.05). Ammonia-N, MCP: microbial protein, and total volatile fatty acid concentrations were significantly higher in the GYS group than in the GY group (p < 0.01), whereas the pH and acetate: propionate values were significantly decreased (p < 0.01). The relative abundance of Firmicutes in the rumen fluid was significantly higher in the GYS group than in the GY group (p < 0.01). At the genus level, the relative abundances of Succiniclasticum, Prevotellaceae_UCG_003, Prevotellaceae_UCG_005, and Ruminococcus_1 were significantly greater in the GY group than in the GYS group (p < 0.01). In conclusion, concentrate supplementation improved yaks' growth potential during the warm season, improved ruminal fermentation, and altered core bacteria abundance.

17.
ACS Nano ; 16(4): 5454-5462, 2022 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-35311253

RESUMO

The formation of lyotropic liquid crystals (LCs) in two-dimensional (2D) colloidal dispersions enables the production of mesoscopic/macroscopic ordered materials from nanoscale building blocks. In contrast to graphene oxide (GO) LCs, the practical applications of MXene LCs are less exploited. This study bridges the gap by utilizing a simple and versatile fabrication method to prepare Ti3C2Tx MXene LC that can be applied as a background-free alignment medium for the residual dipolar coupling (RDC) measurement of organic molecules. Ti3C2Tx LC displays the size- and concentration-dependent alignment degree. Ti3C2Tx nanoflakes with an average size of around 600 nm can provide the quadrupolar 2H splitting of 71 Hz at a concentration of 50 mg/mL and show excellent fluidity at such a high concentration. Compared with other alignment media, Ti3C2Tx LC exhibits the features of no-background and narrow line broadening, which actualizes the acquirement of clean and high-quality NMR spectra for the accurate RDC extraction. Notably, the alignment of LCs is determined to be maintainable in the redispersed solution after freeze-drying, providing the great convenience for the preparation of alignment Ti3C2Tx media, long-term sample preservation, and quantitative evaluation of alignment degree. Meanwhile, the alignment LC media for RDC measurement can be established in other MXenes such as Ti2CTx and Ti3CNTx. Collectively, our findings demonstrate the potential of creating various alignment media from the fascinating MXene family.

18.
Adv Sci (Weinh) ; 9(2): e2103798, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34741443

RESUMO

Lithium-sulfur batteries (LSBs) hold great promise as one of the next-generation power supplies for portable electronics and electric vehicles due to their ultrahigh energy density, cost effectiveness, and environmental benignity. However, their practical application has been impeded owing to the electronic insulation of sulfur and its intermediates, serious shuttle effect, large volume variation, and uncontrollable formation of lithium dendrites. Over the past decades, many pioneering strategies have been developed to address these issues via improving electrodes, electrolytes, separators and binders. Remarkably, polymers can be readily applied to all these aspects due to their structural designability, functional versatility, superior chemical stability and processability. Moreover, their lightweight and rich resource characteristics enable the production of LSBs with high-volume energy density at low cost. Surprisingly, there have been few reviews on development of polymers in LSBs. Herein, breakthroughs and future perspectives of emerging polymers in LSBs are scrutinized. Significant attention is centered on recent implementation of polymers in each component of LSBs with an emphasis on intrinsic mechanisms underlying their specific functions. The review offers a comprehensive overview of state-of-the-art polymers for LSBs, provides in-depth insights into addressing key challenges, and affords important resources for researchers working on electrochemical energy systems.

19.
Bioresour Technol ; 344(Pt A): 126220, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34715343

RESUMO

Hydrogen-nanobubble water was proposed to enhance methane production by anaerobic digestion (AD) with corn straw. The effects of H2-nanobubble water (H2-NBW) amounts (0%, 20%, 40%, 60%, 80%, and 100%) on methane production characteristics of corn straw were explored. The results showed that the methane yields were increased by 11.54%∼25.29% compared with the control group(CK), and the maximum cumulative methane production reached to 254.36 mL·g-VS-1 when the H2-NBW addition was of 60%. Interestingly, the maximum methane concentration increased by 4.37% compared with CK. H2-NBW addition can destroy the cellulose structure of corn straw, reduce the crystallinity of cellulose, and promote the hydrolysis. The degradation rate of cellulose and hemicellulose were increased by 20%∼33% and 13% ∼25.7% respectively, and the removal rate of TS and VS were increased by 6.82%-27.93% and 8.52%-21.47%, respectively. The modified Gompertz equation fitted the cumulative methane production curves very well, with high correlation coefficients (R2 > 0.992).


Assuntos
Hidrogênio , Zea mays , Anaerobiose , Biocombustíveis , Metano , Água
20.
Chem Commun (Camb) ; 57(40): 4966-4969, 2021 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-33876789

RESUMO

In situ uniform confinement of ultrasmall Mo2C nanocrystals into micropore-enriched N-doped carbons was achieved by carbonizing phosphomolybdic acid/polyimide precursors to craft a surface-dominated capacitive battery-type anode. Upon coupling with a capacitor-type cathode, the as-fabricated lithium-ion capacitors exhibit superior power and energy outputs by improving the kinetics and capacity imbalance between two electrodes.

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