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1.
Front Microbiol ; 15: 1402653, 2024.
Artículo en Inglés | MEDLINE | ID: mdl-38860218

RESUMEN

Banana wilt caused by Fusarium oxysporum f. sp. cubense tropical race 4 (Foc TR4) is a devastating fungal disease. Biocontrol strategies hold immense potential for inhibiting the spread of Foc TR4. Here, 30 actinobacteria were isolated from soils and screened for their antagonistic activity against Foc TR4. Strain SCA4-21T was selected due to its strongest antagonistic activity against Foc TR4. Strain SCA4-21T also exhibited strong antagonistic activity against the other eight phytopathogenic fungi. The strain was identified as the genus Streptomyces according to its physiological, biochemical, and phenotypic characteristics. The phylogenetic trees of 16S rRNA sequences demonstrated that strain SCA4-21T formed a subclade with S. iranensis HM 35T and/or S. rapamycinicus NRRL B-5491T with low bootstrap values. Considering that 16S rRNAs did not provide sufficient resolution for species-level identification, the whole genome of strain SCA4-21T was sequenced. Multilocus sequence analysis (MLSA) based on five housekeeping gene alleles (atpD, gyrB, recA, rpoB, and trpB) revealed that strain SCA4-21T clustered into S. hygroscopicus subsp. hygroscopicus NBRC 13472T with 100% of bootstrap value. The analysis of the genome-based phylogeny also approved the results. Average nucleotide identity (ANI) and digital DNA-DNA hybridization (dDDH) were 91.26 and 44.30%, respectively, with values below the respective species level threshold of 95 and 70%. Hence, strain SCA 4-21T represented a novel species within the genus Streptomyces, named Streptomyces luomodiensis sp. nov. The type strain is SCA4-21T (=GDMCC4.340T = JCM36555T). By the CAZymes analysis, 348 carbohydrate-active enzymes (CAZymes) were detected, including 15 chitinases and eight ß-1,3-glucanases. The fermentation broth of strain SCA4-21T, exhibiting strong antagonistic activity against Foc TR4, demonstrated high activities of chitinase and ß-1,3-glucanase, which might be involved in antifungal activity. Our results showed an innovative potential biocontrol agent for managing plant fungal diseases, specifically banana fusarium wilt.

2.
J Integr Plant Biol ; 2024 May 28.
Artículo en Inglés | MEDLINE | ID: mdl-38804840

RESUMEN

The Sapindaceae family, encompassing a wide range of plant forms such as herbs, vines, shrubs, and trees, is widely distributed across tropical and subtropical regions. This family includes economically important crops like litchi, longan, rambutan, and ackee. With the wide application of genomic technologies in recent years, several Sapindaceae plant genomes have been decoded, leading to an accumulation of substantial omics data in this field. This surge in data highlights the pressing need for a unified genomic data center capable of storing, sharing, and analyzing these data. Here, we introduced SapBase, that is, the Sapindaceae Genome Database. SapBase houses seven published plant genomes alongside their corresponding gene structure and functional annotations, small RNA annotations, gene expression profiles, gene pathways, and synteny block information. It offers user-friendly features for gene information mining, co-expression analysis, and inter-species comparative genomic analysis. Furthermore, we showcased SapBase's extensive capacities through a detailed bioinformatic analysis of a MYB gene in litchi. Thus, SapBase could serve as an integrative genomic resource and analysis platform for the scientific exploration of Sapinaceae species and their comparative studies with other plants.

3.
Microbiol Res ; 283: 127694, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38520836

RESUMEN

Tomato fusarium wilt caused by Fusarium oxysporum f. sp. lycopersici (Fol) is a highly destructive disease, resulting in severe economic losses of global tomato production annually. An eco-friendly alternative to chemical fungicide using biological control agents (BCAs) is urgently needed. Here, Bacillus siamensis QN2MO-1 was isolated from Noli fruit and had a strong antagonistic activity against Fol in vitro and in vivo. Strain QN2MO-1 also exhibited a broad-spectrum antifungal activity against the selected 14 phytopathogenic fungi. The crude protein produced by strain QN2MO-1 could inhibit the spore germination of Fol and destroy the spore structure. It was closely related with the generation of chitinase and ß-1,3-glucanase secreted by strain QN2MO-1. In a pot experiment, the application of B. siamensis QN2MO-1 effectively alleviated the yellowing and wilting symptoms of tomato plants. The disease index and incidence rate were decreased by 72.72% and 80.96%, respectively. The rhizospheric soil in tomato plants owed a high abundance of microbial community. Moreover, strain QN2MO-1 also enhanced the plant growth and improved the fruit quality of tomato. Therefore, B. siamensis QN2MO-1 will be explored as a potential biocontrol agent and biofertilizer.


Asunto(s)
Bacillus , Fusarium , Solanum lycopersicum , Frutas , Enfermedades de las Plantas/prevención & control , Enfermedades de las Plantas/microbiología
4.
Planta ; 259(1): 26, 2023 Dec 18.
Artículo en Inglés | MEDLINE | ID: mdl-38110586

RESUMEN

MAIN CONCLUSION: It was proved for the first time that the miR172e-LbrAP2 module regulated the vegetative growth phase transition in Lilium, which provided a new approach to shorten the juvenile stage of Lilium, improved the reproduction rate, and reduced the propagation cost of Lilium commercial bulbs. Lilium is an ornamental bulb plant that takes at least 3 years to cultivate into commercial seed bulbs under natural conditions. The aim of this study was to shorten the Lilium expansion cycle. In this study, the growth cycle of lily tubers induced by low temperature of 15 °C was significantly shorter than that of tubers grown at a conventional temperature. Quantitative real-time PCR analysis showed that the expression patterns of miR172e and LbrAP2 were negatively correlated. GUS histochemical staining confirmed that miR172e and LbrAP2 in tobacco leaves interacted with each other after co-transformation. The shear sites of miR172e and its target gene, LbrAP2, upon binding, were identified by RLM 5' RACE analysis. In addition, miR172e and LbrAP2 showed opposite expression patterns after the transformation of Arabidopsis. miR172e overexpression accelerated the transition from juvenile to adult plants, whereas LbrAP2 overexpression inhibited this process, thus indicating that miR172e negatively regulated the target gene LbrAP2. Upregulation of the transcription factor LbrAP2 delayed the phase transition of plants, whereas miR172 inhibited the transcriptional translation of LbrAP2, thereby accelerating the phase transition. Low-temperature treatment of Lilium bulbs can shorten Lilium development, which provides a new approach to accelerating Lilium commercial bulb breeding and reducing breeding costs.


Asunto(s)
Lilium , Lilium/genética , Lilium/metabolismo , Flores/genética , Fitomejoramiento , Factores de Transcripción/genética , Raíces de Plantas/genética , Regulación de la Expresión Génica de las Plantas
5.
Front Plant Sci ; 14: 1289959, 2023.
Artículo en Inglés | MEDLINE | ID: mdl-37941669

RESUMEN

Banana Fusarium wilt caused by Fusarium oxysporum f. sp. cubense tropical race4 (Foc TR4) is one of the most destructive soil-borne fungal diseases and currently threatens banana production around the world. Until now, there is lack of an effective method to control banana Fusarium wilt. Therefore, it is urgent to find an effective and eco-friendly strategy against the fungal disease. In this study, a strain of Trichoderma sp. N4-3 was isolated newly from the rhizosphere soil of banana plants. The isolate was identified as Trichoderma parareesei through analysis of TEF1 and RPB2 genes as well as morphological characterization. In vitro antagonistic assay demonstrated that strain N4-3 had a broad-spectrum antifungal activity against ten selected phytopathogenic fungi. Especially, it demonstrated a strong antifungal activity against Foc TR4. The results of the dual culture assay indicated that strain N4-3 could grow rapidly during the pre-growth period, occupy the growth space, and secrete a series of cell wall-degrading enzymes upon interaction with Foc TR4. These enzymes contributed to the mycelial and spore destruction of the pathogenic fungus by hyperparasitism. Additionally, the sequenced genome proved that strain N4-3 contained 21 genes encoding chitinase and 26 genes encoding ß-1,3-glucanase. The electron microscopy results showed that theses cell wall-degrading enzymes disrupted the mycelial, spore, and cell ultrastructure of Foc TR4. A pot experiment revealed that addition of strain N4-3 significantly reduced the amount of Foc TR4 in the rhizosphere soil of bananas at 60 days post inoculation. The disease index was decreased by 45.00% and the fresh weight was increased by 63.74% in comparison to the control. Hence, Trichoderma parareesei N4-3 will be a promising biological control agents for the management of plant fungal diseases.

6.
ACS Appl Mater Interfaces ; 15(41): 48135-48146, 2023 Oct 18.
Artículo en Inglés | MEDLINE | ID: mdl-37792067

RESUMEN

A carbon matrix-supported Ni catalyst with surface/subsurface S species is prepared using a sacrificial metal-organic framework synthesis strategy. The resulting highly dispersed Ni-S/C catalyst contains surface discontinuous and electron-deficient Niδ+ sites modified by p-block S elements. This catalyst proved to be extremely active and selective for alkyne hydrogenation. Specifically, high intrinsic activity (TOF = 0.0351 s-1) and superior selectivity (>90%) at complete conversion were achieved, whereas an analogous S-free sample prepared by the same synthetic route performed poorly. That is, the incorporation of S in Ni particles and the carbon matrix exerts a remarkable positive effect on catalytic behavior for alkyne hydrogenation, breaking the activity-selectivity trade-off. Through comprehensive experimental studies, enhanced performance of Ni-S/C was ascribed to the presence of discontinuous Ni ensembles, which promote desorption of weakly π-bonded ethylene and an optimized electronic structure modified via obvious p-d orbital hybridization.

7.
Mol Plant ; 16(11): 1733-1742, 2023 11 06.
Artículo en Inglés | MEDLINE | ID: mdl-37740491

RESUMEN

Since the official release of the stand-alone bioinformatics toolkit TBtools in 2020, its superior functionality in data analysis has been demonstrated by its widespread adoption by many thousands of users and references in more than 5000 academic articles. Now, TBtools is a commonly used tool in biological laboratories. Over the past 3 years, thanks to invaluable feedback and suggestions from numerous users, we have optimized and expanded the functionality of the toolkit, leading to the development of an upgraded version-TBtools-II. In this upgrade, we have incorporated over 100 new features, such as those for comparative genomics analysis, phylogenetic analysis, and data visualization. Meanwhile, to better meet the increasing needs of personalized data analysis, we have launched the plugin mode, which enables users to develop their own plugins and manage their selection, installation, and removal according to individual needs. To date, the plugin store has amassed over 50 plugins, with more than half of them being independently developed and contributed by TBtools users. These plugins offer a range of data analysis options including co-expression network analysis, single-cell data analysis, and bulked segregant analysis sequencing data analysis. Overall, TBtools is now transforming from a stand-alone software to a comprehensive bioinformatics platform of a vibrant and cooperative community in which users are also developers and contributors. By promoting the theme "one for all, all for one", we believe that TBtools-II will greatly benefit more biological researchers in this big-data era.


Asunto(s)
Biología Computacional , Programas Informáticos , Filogenia , Minería de Datos , Macrodatos
8.
Int J Mol Sci ; 24(3)2023 Jan 30.
Artículo en Inglés | MEDLINE | ID: mdl-36768952

RESUMEN

Plant height is an important and valuable agronomic trait associated with yield and resistance to abiotic and biotic stresses. Dwarfism has positive effects on plant development and field management, especially for tall monocotyledon banana (Musa spp.). However, several key genes and their regulation mechanism of controlling plant height during banana development are unclear. In the present study, the popular cultivar 'Brazilian banana' ('BX') and its dwarf mutant ('RK') were selected to identify plant height-related genes by comparing the phenotypic and transcriptomic data. Banana seedlings with 3-4 leaves were planted in the greenhouse and field. We found that the third and fourth weeks are the key period of plant height development of the selected cultivars. A total of 4563 and 10507 differentially expressed genes (DEGs) were identified in the third and fourth weeks, respectively. Twenty modules were produced by the weighted gene co-expression network analysis (WGCNA). Eight modules were positively correlated with the plant height, and twelve other modules were negatively correlated. Combining with the analysis of DEGs and WGCNA, 13 genes in the signaling pathway of gibberellic acid (GA) and 7 genes in the signaling pathway of indole acetic acid (IAA) were identified. Hub genes related to plant height development were obtained in light of the significantly different expression levels (|log2FC| ≥ 1) at the critical stages. Moreover, GA3 treatment significantly induced the transcription expressions of the selected candidate genes, suggesting that GA signaling could play a key role in plant height development of banana. It provides an important gene resource for the regulation mechanism of banana plant development and assisted breeding of ideal plant architecture.


Asunto(s)
Musa , Transcriptoma , Regulación de la Expresión Génica de las Plantas , Fitomejoramiento , Perfilación de la Expresión Génica , Transducción de Señal/genética , Proteínas de Plantas/genética , Proteínas de Plantas/metabolismo
9.
Angew Chem Int Ed Engl ; 62(15): e202216527, 2023 Apr 03.
Artículo en Inglés | MEDLINE | ID: mdl-36599818

RESUMEN

We reported a strategy of carbon-negative H2 production in which CO2 capture was coupled with H2 evolution at ambient temperature and pressure. For this purpose, carbonate-type Cux Mgy Fez layered double hydroxide (LDH) was preciously constructed, and then a photocatalysis reaction of interlayer CO3 2- reduction with glycerol oxidation was performed as driving force to induce the electron storage on LDH layers. With the participation of pre-stored electrons, CO2 was captured to recover interlayer CO3 2- in presence of H2 O, accompanied with equivalent H2 production. During photocatalysis reaction, Cu0.6 Mg1.4 Fe1 exhibited a decent CO evolution amount of 1.63 mmol g-1 and dihydroxyacetone yield of 3.81 mmol g-1 . In carbon-negative H2 production process, it showed an exciting CO2 capture quantity of 1.61 mmol g-1 and H2 yield of 1.44 mmol g-1 . Besides, this system possessed stable operation capability under simulated flu gas condition with negligible performance loss, exhibiting application prospect.

10.
Dalton Trans ; 52(7): 1950-1961, 2023 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-36683445

RESUMEN

Aiming at the comprehensive utilization of waste carbon resources and renewable carbon resources, we put forward the photocatalytic coupling process of CO2 reduction and 5-hydroxymethylfurfural (5-HMF) oxidation mediated by the anionic compound of layered double hydroxides (LDHs). Specifically, a ZnNiFe-LDH was synthesized by co-precipitation method, during which CO2 was stored between LDH layers in the form of carbonate. Then, a certain amount of metal vacancies were introduced into LDH nanosheets by selectively etching Zn2+ ions. ICP-AES, EPR and XPS showed that the concentration of Zn vacancies gradually increased with the etching time prolonging, which thus optimized the electronic structure of LDH layers. Under the catalysis of the electron-rich metal cations and hydroxyl groups on the layers, the interlayer carbonate was in situ reduced into CO coupled accompanied with the 5-HMF oxidation to 2.5-furandiformaldehyde (DFF). Compared with the unetched ZnNiFe-LDHs, the CO and DFF yields over the LDHs etched for 3 h were increased by 2.84 and 2.82 times under UV-vis irradiation with a density of 500 mW cm-2. Finally, combined with isotope-labeled 13CO2 experiments and in situ FTIR characterization, we revealed the possible coupling mechanism and defect-induced performance enhancement mechanism.

11.
Artículo en Inglés | MEDLINE | ID: mdl-35666270

RESUMEN

Revealing the structural evolution of the real active site during photocatalysis is very important for understanding the catalytic mechanism, but it remains a great challenge. By employing single atoms (SAs) as the mechanism research platform, we investigated the variation of the SA structure under light and the corresponding reaction pathway controlment mechanism. In particular, taking the defect anchoring strategy, Pt SAs are anchored on the metal ion vacancy-rich ZnNiTi layered double hydroxide-etched (ZnNiTi-LDHs-E) support. It is proved by CO-Fourier transform infrared and X-ray absorption fine structure characterization methods that the Pt SAs could gain photoelectrons to form cationic Pt(IV), electron-rich Pt(II), and near-neutral Ptδ+ species at different light intensities. By in situ inducing the above different Pt SAs in photocatalytic CO2 reduction, a dramatic product distribution is observed: (1) under weak light, Pt(IV) SAs cannot activate CO, so CO cannot be further transformed into hydrocarbons; (2) under the moderate light, electron-rich Pt(II) SAs could cooperate with adjacent LDH surface sites (Ni2+/Ti4+) to open up the C-C coupling route for C2H6 generation; and (3) Pt SAs in the state of near-neutral Ptδ+ could directly hydrogenate CO into CH4. This work reveals the structural evolution of Pt SAs in photocatalysis and the corresponding effect on catalytic performance, which provides a new idea for the construction of highly efficient photocatalysts.

12.
Nat Genet ; 54(1): 73-83, 2022 01.
Artículo en Inglés | MEDLINE | ID: mdl-34980919

RESUMEN

Lychee is an exotic tropical fruit with a distinct flavor. The genome of cultivar 'Feizixiao' was assembled into 15 pseudochromosomes, totaling ~470 Mb. High heterozygosity (2.27%) resulted in two complete haplotypic assemblies. A total of 13,517 allelic genes (42.4%) were differentially expressed in diverse tissues. Analyses of 72 resequenced lychee accessions revealed two independent domestication events. The extremely early maturing cultivars preferentially aligned to one haplotype were domesticated from a wild population in Yunnan, whereas the late-maturing cultivars that mapped mostly to the second haplotype were domesticated independently from a wild population in Hainan. Early maturing cultivars were probably developed in Guangdong via hybridization between extremely early maturing cultivar and late-maturing cultivar individuals. Variable deletions of a 3.7 kb region encompassed by a pair of CONSTANS-like genes probably regulate fruit maturation differences among lychee cultivars. These genomic resources provide insights into the natural history of lychee domestication and will accelerate the improvement of lychee and related crops.


Asunto(s)
Domesticación , Genoma de Planta , Litchi/genética , China , Productos Agrícolas/genética , Evolución Molecular , Flores/genética , Haplotipos , Heterocigoto , Litchi/crecimiento & desarrollo , Anotación de Secuencia Molecular , Polimorfismo de Nucleótido Simple , Análisis de Secuencia de ADN , Especificidad de la Especie
13.
Small ; 18(1): e2103852, 2022 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-34766728

RESUMEN

Aiming at regulating and controlling the localized electronic states while maintaining the metal atoms in the isolation form, an in situ adsorbate induced strategy is proposed at a programmed temperature to activate Zr-based metal-organic framework (MOF) supported single Pd atom catalyst. It is discovered that in situ treatment environments trigger the change of lattice parameters in MOF materials by reaction heat effect, observed by in situ X-ray diffraction, spherical aberration-corrected electron microscope, and X-ray adsorption fine structure (XAFS). The as-obtained electron-deficient Pd single atoms are critical to the high intrinsic activity (turnover frequency of 0.132 s-1 ) and selectivity of 93% with the long-term stability in the semihydrogenation of acetylene, which can be comparable to the state-of-the-art Pd catalysts. This superior catalytic behavior correlates with the reduced C2 H4 desorption energy and the activation barriers for the hydrogenation, confirmed by density functional theory calculation.

14.
Fundam Res ; 2(3): 412-421, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-38933400

RESUMEN

Qualitatively identifying the dominant catalytic site for each step of a semi-continuous reaction and semi-quantitatively correlating such different sites to the catalytic performance is of great significance toward the integration of multiple well-optimized sites on a heterogeneous catalyst. Herein, a series of structurally defined TiOx-based catalysts were synthesized to provide a feasible approach to investigate the aforementioned issues using the semi-continuous oxidation of glycerol as a model reaction. Detailed investigations have verified the simultaneous presence of two kinds of Pt active sites: 1) Negatively charged Pt bound to the oxygen vacancies of modified TiOx in the form of Ptδ--Ov-Ti3+ sites and 2) metallic Pt (Pt0 site) located away from the interface. Meanwhile, the proportion of surficial and interfacial sites varies over this series of catalysts. Combined in situ FTIR experiments revealed that the reaction network was well-tuned via a site cooperation mechanism: The surficial Pt0 sites dissociatively adsorb the OH group of glycerol with a monodentate bonding geometry and the Ptδ--Ov-Ti3+ sites dissociate the C=O bond of the aldehyde group in a bidentate form. Furthermore, CO-FTIR spectroscopy confirmed a correlation between the reaction rate/product selectivity and the fraction of surficial/interfacial sites. A rational proportion of surficial and interfacial sites is key to enabling a high yield of glyceric acid. The most active catalyst with 32% surface sites and 68% interfacial sites exhibited 90.0% glycerol conversion and 68.5% GLYA selectivity. These findings provide a deeper understanding of the structure-activity relationships using qualitative identification and semi-quantitative analysis.

15.
ACS Appl Mater Interfaces ; 13(19): 22292-22303, 2021 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-33973464

RESUMEN

In this work, we synthesized a series of Cu/ZrO2 catalysts with tunable Vo-Cu0 (oxygen vacancy adjacent to Cu metal) and VZr-Cuδ+ (zirconium vacancy adjacent to electron-deficient Cu species) dual-interface sites and investigated the role of the dual-interface sites in the 5-hydroxymethylfurfural (5-HMF) hydrogenolysis reaction with isopropanol as the hydrogen source. By combining a series of in situ infrared characterization and catalytic performance analysis, it is identified that Vo-Cu0 interface sites were responsible for activating isopropanol dehydrogenation and C═O dissociation of 5-HMF, while the VZr-Cuδ+ interface sites were responsible for the dehydroxylation of an intermediate product 5-methyl-2-furfuryl alcohol (5-MFA). Specifically, C-OH was first deprotonated on the VZr at the VZr-Cuδ+ interface site to reduce the activation energy of 5-MFA dehydroxylation and then adjacent Cuδ+ promoted the dissociation of the C-O bond by enhancing the adsorption energy while elongating the C-O bond, as confirmed by the density functional theory calculations. Because the dual-interface sites provided separate sites for activating intermediate products and reactants, the coupling reaction caused by competitive adsorption is thus well avoided. Therefore, the optimized Cu/ZrO2 catalyst with the most VZr-Cuδ+ and moderate Vo-Cu0 sites exhibited 98.4% of 2,5-dimethylfuran yield under the conditions of 180 °C and self-vapor pressure.

16.
Hortic Res ; 8(1): 45, 2021 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-33642576

RESUMEN

Small RNAs (sRNAs) are essential regulatory molecules, and there are three major sRNA classes in plants: microRNAs (miRNAs), phased small interfering RNAs (phased siRNAs or phasiRNAs), and heterochromatic siRNAs (hc-siRNAs). Excluding miRNAs, the other two classes are not well annotated or available in public databases for most sequenced plant genomes. We performed a comprehensive sRNA annotation of 143 plant species that have fully sequenced genomes and next-generation sequencing sRNA data publicly available. The results are available via an online repository called sRNAanno ( www.plantsRNAs.org ). Compared with other public plant sRNA databases, we obtained was much more miRNA annotations, which are more complete and reliable because of the consistent and highly stringent criteria used in our miRNA annotations. sRNAanno also provides free access to genomic information for >22,721 PHAS loci and >22 million hc-siRNA loci annotated from these 143 plant species. Both miRNA and PHAS loci can be easily browsed to view their main features, and a collection of archetypal trans-acting siRNA 3 (TAS3) genes were annotated separately for quick access. To facilitate the ease of sRNA annotation, sRNAanno provides free service for sRNA annotations to the community. In summary, the sRNAanno database is a great resource to facilitate genomic and genetic research on plant small RNAs.

17.
Dalton Trans ; 48(43): 16402-16411, 2019 Nov 21.
Artículo en Inglés | MEDLINE | ID: mdl-31641719

RESUMEN

The base-free styrene epoxidation with H2O2 as an oxidant was strongly in accordance with the requirements for a sustainable chemical industry. Aiming at the low efficiency of a non-noble metal catalyst system, we proposed utilizing the synergistic effect and manipulating the surface acid-basic property of materials to increase the catalytic performance in this reaction. Herein, to combine two promoting approaches, we synthesized a series of mixed metal oxide (MMO) materials to screen promising active components with a suitable acid-basic property for H2O2-styrene epoxidation. As a result, the highest styrene conversion (82.8%) and best styrene oxide selectivity (79.7%) were achieved over a CuCr-MMO catalyst. The catalytic performance was considerably enhanced compared with the CuO and CrOx references. Detailed characterizations were performed to investigate the dispersion, electronic structure, and acid-basic property to explain the structure-performance relationship. On one hand, the promoted dispersion of the Cu and Cr components contributed to more catalytic sites and the electron transfer between Cu and Cr improved the intrinsic activity, which were both responsible for the enhanced activity. On the other hand, the unique structure modulated the acid-basic properties to be suitable for this catalytic system. In particular, a suitable basicity was facilitated to selectively transform H2O2 into HOO˙ radicals, while a low acidity suppressed the epoxide ring opening to form phenylacetaldehyde. By combining the high accessibility, suitable basic-acid property, and fast electron transfer, CuCr-MMO exhibited a high styrene conversion and selectivity to styrene oxide.

18.
Chem Sci ; 10(12): 3556-3566, 2019 Mar 28.
Artículo en Inglés | MEDLINE | ID: mdl-30996947

RESUMEN

The impregnation method is commonly employed to prepare supported multi-metallic catalysts but it is often difficult to achieve homogeneous and stable alloy structures. In this work, we revealed the dependence of alloying behavior on the support morphology by fabricating Ni-Cu over different shaped CeO2. Specifically, nanocube ceria favoured the formation of monometallic Cu and Ni-rich phases whereas polycrystalline and nanorod ceria induced the formation of a mixture of Cu-rich alloys with monometallic Ni. Surprisingly, nanopolyhedron (NP) ceria led to the generation of homogeneous Ni-Cu nanoalloys owing to the equivalent interactions of Ni and Cu species with CeO2 (111) facets which exposed relatively few coordinative unsaturated sites. More importantly, a strong interfacial effect was observed for Ni-Cu/CeO2-NP due to the presence of CeO x adjacent to metal sites at the interface, resulting in excellent stability of the alloy structure. With the aid of CeO x , NiCu nanoalloys showed outstanding catalytic behaviour in acetylene and hexyne hydrogenation reactions. This study provides valuable insights into how fully alloyed and stable catalysts may be prepared by tailoring the support morphology while still employing a universal impregnation method.

19.
Nat Commun ; 8(1): 591, 2017 09 19.
Artículo en Inglés | MEDLINE | ID: mdl-28928359

RESUMEN

Bio-oil, produced by the destructive distillation of cheap and renewable lignocellulosic biomass, contains high energy density oligomers in the water-insoluble fraction that can be utilized for diesel and valuable fine chemicals productions. Here, we show an efficient hydrodeoxygenation catalyst that combines highly dispersed palladium and ultrafine molybdenum phosphate nanoparticles on silica. Using phenol as a model substrate this catalyst is 100% effective and 97.5% selective for hydrodeoxygenation to cyclohexane under mild conditions in a batch reaction; this catalyst also demonstrates regeneration ability in long-term continuous flow tests. Detailed investigations into the nature of the catalyst show that it combines hydrogenation activity of Pd and high density of both Brønsted and Lewis acid sites; we believe these are key features for efficient catalytic hydrodeoxygenation behavior. Using a wood and bark-derived feedstock, this catalyst performs hydrodeoxygenation of lignin, cellulose, and hemicellulose-derived oligomers into liquid alkanes with high efficiency and yield.Bio-oil is a potential major source of renewable fuels and chemicals. Here, the authors report a palladium-molybdenum mixed catalyst for the selective hydrodeoxygenation of water-insoluble bio-oil to mixtures of alkanes with high carbon yield.

20.
Dalton Trans ; 46(39): 13463-13471, 2017 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-28951906

RESUMEN

A highly dispersed CuO catalyst was prepared by the deposition-precipitation method and evaluated for the catalytic epoxidation of styrene with tert-butyl hydroperoxide (TBHP) as the oxidant under solvent acetonitrile conditions. Compared with MgAl hydrotalcite (MgAl-HT)-, MgO-, TiO2-, C-, and MCM-22-supported catalysts, CuO/CoAl-HT exhibited preferable activity and selectivity towards styrene oxide (72% selectivity at 99.5% styrene conversion) due to its high dispersion of CuO and surface area of Cu. The improved dispersion of CuO/CoAl-HT could be ascribed to the nature of HT support, especially the synergistic effect of acidic and basic sites on the surface, which facilitated the formation of highly dispersed CuO species. A structure-performance relationship study indicated that copper(ii) in CuO was the active site for the epoxidation and oxidation of styrene, and that CuII of rich electronic density favored the improvement of selectivity of styrene oxide. Based on these results, a reaction mechanism was proposed. Moreover, the preferred catalytic performance of CuO/CoAl-HT could be maintained in five reused cycles.

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