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1.
Comp Immunol Microbiol Infect Dis ; 111: 102214, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-39002176

RESUMO

MicroRNAs (miRNAs) have been shown to play an important regulatory role in the process of pathogenic infection. However, the miRNAs that regulate the pathogenic process of G. parasuis and their functions are still unknown. Here, high-throughput sequencing was used to quantify the expression of miRNA in piglet lung tissue after G. parasuis XX0306 strain infection. A total of 25 differentially expressed microRNAs (DEmiRNAs) were identified. GO and KEGG pathway enrichment analysis showed that many of the functions of genes that may be regulated by DEmiRNA are related to inflammatory response and immune regulation. Further studies found that ssc-miR-135 may promote the expression of inflammatory factors through NF-κB signaling pathway. Whereas, ssc-miR-155-3p inhibited the inflammatory response induced by G. parasuis, and its regulatory mechanism remains to be further investigated. This study provides a valuable reference for revealing the regulatory effects of miRNAs on the pathogenesis of G. parasuis. DATA AVAILABILITY: The datasets generated during the current study are not publicly available due to this study is currently in the ongoing research stage, and some of the data cannot be made public sooner yet, but are available from the corresponding author on reasonable request.

2.
Pest Manag Sci ; 2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38895838

RESUMO

BACKGROUND: Telosma mosaic virus (TelMV, Potyvirus, Potyviridae) is an emerging viral pathogen that threatens passion fruit plantations worldwide. However, an efficient strategy for controlling such a virus is not yet available. Cross protection is a phenomenon in which pre-infection of a plant with one mild strain prevents or delays subsequent infection by the same or closely related virus. HC-Pro is the potyviral encoded multifunctional protein involved in several steps of viral infection, including multiplication, movement, transmission and RNA silencing suppression. In this study, we tested whether it is possible to generate attenuated viral strains capable of conferring protection against severe TelMV infection by manipulating the HC-Pro gene. RESULTS: By introducing point mutation into the conserved motif FRNK of HC-Pro that is essential for RNA silencing suppression, we have successfully obtained three attenuated mutants of TelMV (R181K, R181D, and R181E, respectively). These attenuated TelMV mutants could systemically infect passion fruit plants without noticeable symptoms. Pre-inoculation of one of these attenuated mutants confers efficient protection against subsequent infection by severe TelMV strain. Moreover, we demonstrated that the HC-Pros harbored by the attenuated mutants exhibit reduced RNA silencing suppression activity in Nicotiana benthamiana leaves. CONCLUSION: The attenuated TelMV mutants developed in this study that are suitable for cross protection offer a practical, powerful tool to fight against TelMV for sustainable passion fruit production. © 2024 Society of Chemical Industry.

3.
Adv Mater ; 36(24): e2400288, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38411357

RESUMO

Photocatalytic hydrogen peroxide (H2O2) synthesis from water and O2 is an economical, eco-friendly, and sustainable route for H2O2 production. However, single-component photocatalysts are subjected to limited light-harvesting range, fast carrier recombination, and weak redox power. To promote photogenerated carrier separation and enhance redox abilities, an organic/inorganic S-scheme photocatalyst is fabricated by in situ growing In2S3 nanosheets on a covalent organic framwork (COF) substrate for efficient H2O2 production in pure water. Interestingly, compared to unitary COF and In2S3, the COF/In2S3 S-scheme photocatalysts exhibit significantly larger light-harvesting range and stronger visible-light absorption. Partial density of state calculation, X-ray photoelectron spectroscopy, and femtosecond transient absorption spectroscopy reveal that the coordination between In2S3 and COF induces the formation of mid-gap hybrid energy levels, leading to smaller energy gaps and broadened absorption. Combining electron spin resonance spectroscopy, radical-trapping experiments, and isotope labeling experiments, three pathways for H2O2 formation are identified. Benefited from expanded light-absorption range, enhanced carrier separation, strong redox power, and multichannel H2O2 formation, the optimal composite shows an impressive H2O2-production rate of 5713.2 µmol g-1 h-1 in pure water. This work exemplifies an effective strategy to ameliorate COF-based photocatalysts by building S-scheme heterojunctions and provides molecular-level insights into their impact on energy level modulation.

4.
J Colloid Interface Sci ; 659: 486-494, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38184991

RESUMO

Various adsorbents for CO2 capture have been developed to mitigate the greenhouse effect. In this work, a novel CO2 adsorbent was fabricated by depositing triethanolamine (TEOA) onto the surface of nickel-cobalt-aluminum layered double oxide (NiCoAl-LDO) via the impregnation method. The CO2 capacity of the TEOA-LDO composite reached 1.27 mmol/g at 0 °C and 100 kPa, which was twice that of unmodified NiCoAl-LDO. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) showed that the hydroxyl groups (-OH) on the surface of NiCoAl-LDO played a significant role in facilitating CO2 adsorption, similar to CO2 adsorption in the presence of H2O, where CO2 is not converted to carbamates but to bicarbonates through base-catalyzed hydration. This bicarbonate pathway doubles the theoretical amine efficiency, increases the CO2 capacity, and reduces the energy consumption during CO2 desorption. The work provides valuable insights into the development of CO2 adsorbents with high capacity, excellent cycling stability, and low regeneration energy.

5.
Mol Cell Endocrinol ; 580: 112109, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-37956789

RESUMO

Recurrent non-severe hypoglycemia (RH) in patients with diabetes might be associated with cognitive impairment. Previously, we found that mitochondrial dysfunction plays an important role in this pathological process; however, the mechanism remains unclear. The objective of this study was to determine the molecular mechanisms of mitochondrial damage associated with RH in diabetes mellitus (DM). We found that RH is associated with reduced hippocampal mitophagy in diabetic mice, mainly manifested by reduced autophagosome formation and impaired recognition of impaired mitochondria, mediated by the PINK1/Parkin pathway. The same impaired mitophagy initiation was observed in an in vitro high-glucose cultured astrocyte model with recurrent low-glucose interventions. Promoting autophagosome formation and activating PINK1/Parkin-mediated mitophagy protected mitochondrial function and cognitive function in mice. The results showed that impaired mitophagy is involved in the occurrence of mitochondrial dysfunction, mediating the neurological impairment associated with recurrent low glucose under high glucose conditions.


Assuntos
Disfunção Cognitiva , Diabetes Mellitus Experimental , Hipoglicemia , Doenças Mitocondriais , Camundongos , Humanos , Animais , Mitofagia , Diabetes Mellitus Experimental/metabolismo , Hipoglicemia/complicações , Glucose , Disfunção Cognitiva/complicações , Ubiquitina-Proteína Ligases/metabolismo , Proteínas Quinases/metabolismo , Doenças Mitocondriais/complicações
6.
Metabolites ; 13(11)2023 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-37999218

RESUMO

High-sugar and high-fat diets cause significant harm to health, especially via metabolic diseases. In this study, the protective effects of the antidiabetic drug exenatide (synthetic exendin-4), a glucagon-like peptide 1 (GLP-1) receptor agonist, on high-fat and high-glucose (HFHG)-induced renal injuries were investigated in vivo and in vitro. In vivo and in vitro renal injury models were established. Metabolomic analysis based on 1H-nuclear magnetic resonance was performed to examine whether exenatide treatment exerts a protective effect against kidney injury in diabetic rats and to explore its potential molecular mechanism. In vivo, 8 weeks of exenatide treatment resulted in the regulation of most metabolites in the diabetes mellitus group. In vitro results showed that exendin-4 restored the mitochondrial functions of mesangial cells, which were perturbed by HFHG. The effects of exendin-4 included the improved antioxidant capacity of mesangial cells, increased the Bcl-2/Bax ratio, and reduced protein expression of cyt-c and caspase-3 activation. In addition, exendin-4 restored mesangial cell energy metabolism by increasing succinate dehydrogenase and phosphofructokinase activities and glucose consumption while inhibiting pyruvate dehydrogenase E1 activity. In conclusion, GLP-1 agonists improve renal injury in diabetic rats by ameliorating metabolic disorders. This mechanism could be partially related to mitochondrial functions and energy metabolism.

7.
Front Plant Sci ; 14: 1236838, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37636087

RESUMO

Passion fruit (Passiflora edulis) is a perennial evergreen vine that grows mainly in tropical and subtropical regions due to its nutritional, medicinal and ornamental values. However, the molecular biology study of passion fruit is extremely hindered by the lack of an easy and efficient method for transformation. The protoplast transformation system plays a vital role in plant regeneration, gene function analysis and genome editing. Here, we present a new method ('Cotyledon Peeling Method') for simple and efficient passion fruit protoplast isolation using cotyledon as the source tissue. A high yield (2.3 × 107 protoplasts per gram of fresh tissues) and viability (76%) of protoplasts were obtained upon incubation in the enzyme solution [1% (w/v) cellulase R10, 0.25% (w/v) macerozyme R10, 0.4 M mannitol, 10 mM CaCl2, 20 mM KCl, 20 mM MES and 0.1% (w/v) BSA, pH 5.7] for 2 hours. In addition, we achieved high transfection efficiency of 83% via the polyethylene glycol (PEG)-mediated transformation with a green fluorescent protein (GFP)-tagged plasmid upon optimization. The crucial factors affecting transformation efficiency were optimized as follows: 3 µg of plasmid DNA, 5 min transfection time, PEG concentration at 40% and protoplast density of 100 × 104 cells/ml. Furthermore, the established protoplast system was successfully applied for subcellular localization analysis of multiple fluorescent organelle markers and protein-protein interaction study. Taken together, we report a simple and efficient passion fruit protoplast isolation and transformation system, and demonstrate its usage in transient gene expression for the first time in passion fruit. The protoplast system would provide essential support for various passion fruit biology studies, including genome editing, gene function analysis and whole plant regeneration.

8.
J Phys Chem Lett ; 14(20): 4803-4814, 2023 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-37191275

RESUMO

Photocatalysis opens a new door to H2O2 formation via a low-cost, clean, mild, and sustainable process, which holds great promise for the next generation of massive H2O2 production. However, fast photogenerated electron-hole recombination and slow reaction kinetics are the main obstacles for its practical application. An effective solution is to construct the step-scheme (S-scheme) heterojunction, which remarkably promotes carrier separation and boosts the redox power for efficient photocatalytic H2O2 production. Considering the superiority of S-scheme heterojunctions, this Perspective summarizes the recent advances of S-scheme photocatalysts for H2O2 production, including photocatalysts for building S-scheme heterojunctions, H2O2-production performance, and S-scheme photocatalytic mechanisms. Lastly, some prospects are given to motivate future research in this promising field, other promising strategies are provided to further improve H2O2 yields, and future research directions are suggested.

9.
BMC Plant Biol ; 23(1): 56, 2023 Jan 26.
Artigo em Inglês | MEDLINE | ID: mdl-36698067

RESUMO

BACKGROUND: Areca palm (Areca catechu) is a woody perennial plant of both economical and medicinal importance grown in tropical and subtropical climates. Yet, the molecular biology study of areca palm is extremely impeded by its unavailability of a transformation method. An efficient protoplast isolation and transformation system could be highly desirable to overcome this barrier. RESULTS: Here, we described a simple and efficient method for protoplast isolation and transformation from the perennial plant areca palm. A high yield of protoplasts (2.5 × 107 protoplasts per gram of fresh leaf tissues) was obtained from the fresh light green leaflet from the newly-emerged leaf digested overnight in the enzyme solution [2% (w/v) cellulase R10, 0.5% (w/v) macerozyme R10, 0.7 M mannitol, 10 mM CaCl2, 20 mM KCl, 20 mM MES and 0.1% (w/v) BSA, pH 5.7] by the direct leaf-peeling method. The isolated areca protoplasts maintain viability of 86.6% and have been successfully transformed with a green fluorescent protein (GFP)-tagged plasmid (pGreen0029-GFP, 6.0 kb) via the polyethylene glycol (PEG)-mediated transformation. Moreover, the mannitol concentration (optimal: 0.7 M) was determined as a key factor affecting areca protoplast isolation. We also demonstrated that the optimal density of areca protoplast for efficient transformation was at 1.0-1.5 × 106 cells/ml. With the optimization of transformation parameters, we have achieved a relatively high transformation efficiency of nearly 50%. CONCLUSION: We have established the first efficient protocol for the high-yield isolation and transformation of areca palm protoplasts. This method shall be applied in various biological studies of areca palm, such as gene function analysis, genome editing, protein trafficking and localization and protein-protein interaction. In addition, the protoplast system offers a great genetic transformation approach for the woody perennial plant-areca palm. Moreover, the established platform may be applied in protoplast isolation and transformation for other important species in the palm family, including oil palm and coconut.


Assuntos
Areca , Arecaceae , Protoplastos/metabolismo , Folhas de Planta
10.
J Virol ; 97(2): e0144422, 2023 02 28.
Artigo em Inglês | MEDLINE | ID: mdl-36688651

RESUMO

P1 is the first protein translated from the genomes of most viruses in the family Potyviridae, and it contains a C-terminal serine-protease domain that cis-cleaves the junction between P1 and HCPro in most cases. Intriguingly, P1 is the most divergent among all mature viral factors, and its roles during viral infection are still far from understood. In this study, we found that telosma mosaic virus (TelMV, genus Potyvirus) in passion fruit, unlike TelMV isolates present in other hosts, has two stretches at the P1 N terminus, named N1 and N2, with N1 harboring a Zn finger motif. Further analysis revealed that at least 14 different potyviruses, mostly belonging to the bean common mosaic virus subgroup, encode a domain equivalent to N1. Using the newly developed TelMV infectious cDNA clones from passion fruit, we demonstrated that N1, but not N2, is crucial for viral infection in both Nicotiana benthamiana and passion fruit. The regulatory effects of N1 domain on P1 cis cleavage, as well as the accumulation and RNA silencing suppression (RSS) activity of its cognate HCPro, were comprehensively investigated. We found that N1 deletion decreases HCPro abundance at the posttranslational level, likely by impairing P1 cis cleavage, thus reducing HCPro-mediated RSS activity. Remarkably, disruption of the Zn finger motif in N1 did not impair P1 cis cleavage and HCPro accumulation but severely debilitated TelMV fitness. Therefore, our results suggest that the Zn finger motif in P1s plays a critical role in viral infection that is independent of P1 protease activity and self-release, as well as HCPro accumulation and silencing suppression. IMPORTANCE Viruses belonging to the family Potyviridae represent the largest group of plant-infecting RNA viruses, including a variety of agriculturally and economically important viral pathogens. Like all picorna-like viruses, potyvirids employ polyprotein processing as the gene expression strategy. P1, the first protein translated from most potyvirid genomes, is the most variable viral factor and has attracted great scientific interest. Here, we defined a Zn finger motif-encompassing domain (N1) at the N terminus of P1 among diverse potyviruses phylogenetically related to bean common mosaic virus. Using TelMV as a model virus, we demonstrated that the N1 domain is key for viral infection, as it is involved both in regulating the abundance of its cognate HCPro and in an as-yet-undefined key function unrelated to protease processing and RNA silencing suppression. These results advance our knowledge of the hypervariable potyvirid P1s and highlight the importance for infection of a previously unstudied Zn finger domain at the P1 N terminus.


Assuntos
Especificidade de Hospedeiro , Peptídeo Hidrolases , Potyviridae , Proteínas Virais , Dedos de Zinco , Especificidade de Hospedeiro/genética , Peptídeo Hidrolases/genética , Peptídeo Hidrolases/metabolismo , Potyviridae/genética , Potyviridae/metabolismo , Proteínas Virais/genética , Proteínas Virais/metabolismo , Dedos de Zinco/genética
11.
J Vet Med Sci ; 84(11): 1527-1535, 2022 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-36216558

RESUMO

Glaesserella parasuis is a pathogen causing Glässer's disease characterized by fibrinous polyserositis, polyarthritis, and meningitis. Owing to the low cross-immunogenicity of different bacterial antigens in commercial vaccines, finding and identifying effective immunoprotective antigens will facilitate the development of novel subunit vaccines. In this study, LolA, identified by bioinformatics approaches, was cloned and successfully expressed as a recombinant protein in Escherichia coli, and its immunogenicity and protection were evaluated in a mouse model. The results showed that the recombinant protein LolA can stimulate mice to produce high levels of IgG antibodies and confer 50% protection against challenge with the highly virulent G. parasuis CY1201 strain (serotype 13). By testing the cytokine levels of interleukin 4 (IL-4), IL-10, and interferon-γ (IFN-γ), it was found that the recombinant protein LolA can induce both Th1 and Th2 immune responses in mice. These results suggest that the recombinant protein LolA has the potential to serve as an alternative antigen for a novel vaccine to prevent G. parasuis infection.


Assuntos
Proteínas de Escherichia coli , Infecções por Haemophilus , Haemophilus parasuis , Proteínas Periplásmicas de Ligação , Doenças dos Roedores , Doenças dos Suínos , Camundongos , Animais , Suínos , Sorogrupo , Anticorpos Antibacterianos , Infecções por Haemophilus/prevenção & controle , Infecções por Haemophilus/veterinária , Proteínas Recombinantes , Vacinação/veterinária , Vacinas de Subunidades Antigênicas , Escherichia coli , Doenças dos Suínos/prevenção & controle
12.
Angew Chem Int Ed Engl ; 61(44): e202212045, 2022 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-36086940

RESUMO

The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual-cocatalyst-modified photocatalyst is constructed based on CdS/MoO2 /MoS2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic acid (LA) oxidation. MoS2 and MoO2 are simultaneously obtained from the conversion of CdMoO4 in one step. In a photocatalytic process, the MoS2 and MoO2 function as the reduction and oxidation centers on which photogenerated electrons and holes accumulate and are used for hydrogen evolution reaction (HER) and PA synthesis, respectively. By monitoring the intermediates, a two-step single-electron route for PA production is proposed, initiated by the cleavage of the α-C(sp3 )-H bond in the LA. The conversion of LA and the selectivity of PA can reach ca. 29 % and 95 % after a five-hour reaction, respectively.

13.
Neurotoxicology ; 92: 166-179, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35985417

RESUMO

Diabetes mellitus can result in severe complications, such as neurodegenerative diseases including cognitive impairment and dementia. The glucagon-like peptide-1 (GLP-1) receptor agonist, liraglutide, is a novel antidiabetic drug with neuroprotective effects against neurodegenerative diseases. In this study, we explored the protective effect of liraglutide on SH-SY5Y cells exposed to methylglyoxal (MG), a byproduct of glucose metabolism that plays a key role in the development of diabetic encephalopathy. We found that liraglutide reduced the MG-induced oxidative stress, increased the activity of superoxide dismutase (SOD) and expression levels of P22phox, Gp91phox, and Xdh genes, and reduced reactive oxygen species (ROS) content. Metabolomics analysis based on 1H nuclear magnetic resonance showed that liraglutide induced alterations in metabolites involved in energy metabolism,including promotion of gluconeogenesis. Moreover, we found that liraglutide promoted oxidative phosphorylation and inhibited glycolysis in SH-SY5Y cells. This study revealed that liraglutide improved diabetes-related neuropathy damage by reducing the level of oxidative stress and maintaining the balance of energy metabolism, thus offering new insights into the potential mechanism of liraglutide in neuronal protection.


Assuntos
Neuroblastoma , Doenças Neurodegenerativas , Fármacos Neuroprotetores , Metabolismo Energético , Glucose/farmacologia , Humanos , Hipoglicemiantes/farmacologia , Liraglutida/farmacologia , Fármacos Neuroprotetores/farmacologia , Estresse Oxidativo , Aldeído Pirúvico/toxicidade , Espécies Reativas de Oxigênio/metabolismo , Superóxido Dismutase/metabolismo
14.
J Phys Chem Lett ; 13(21): 4695-4700, 2022 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-35605285

RESUMO

Step-scheme heterojunctions formed between two firmly bound photocatalysts facilitate charge separation due to interfacial charge transfer, which is usually illustrated by the gain or loss of electrons in the constituent photocatalysts characterized by in situ irradiated X-ray photoelectron spectroscopy. This technique provides a steady-state view of charge distribution but overlooks the transient and complex dynamics of charge transfer, trapping, and recombination. To provide a molecular-level and dynamic view of these processes, we investigated the behaviors of photogenerated charge carriers within an inorganic/organic TiO2/polydopamine S-scheme heterojunction using ultrafast transient absorption spectroscopy and time-resolved photoluminescence spectroscopy. We found the interfacial charge transfer within the step-scheme heterojunction occurred at a smaller shorter time scale than recombination, leading to efficient charge separation. Moreover, the charge-discharge property of polydopamine induces electron backflow, which should be avoided in practical photocatalytic applications. The composite showed higher photocatalytic H2O2-production activities due to faster H2O2 formation and suppressed H2O2 decomposition.

15.
RSC Adv ; 12(6): 3227-3237, 2022 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-35425375

RESUMO

In order to achieve efficient micron-scale water-in-oil emulsion separation, a facile and effective strategy is developed to prepare a super-hydrophobic/super-oleophilic fiberglass filter membrane (FGm). Methyl-trichlorosilane (MTS) is successfully cross-linked on the surface of the fiberglass filter membrane (FGm) and aggregates into a 3D nanowire array to provide low surface energy. Nano fumed hydrophobic silica (SH-SiO2) is used to construct the well-defined nanosphere structure on the surface of FGm and enhance the ability of the membrane to resist extreme conditions. The optimally modified membrane displays outstanding super-hydrophobic properties with a contact angle of 156.2°. It is impressive to find that the MTS@SH-SiO2@FGm not only demonstrates the ability to separate water-in-oil emulsions with a particle size of less than 20 µm, but also the removal efficiency of separation has reached 99.98%. More attractively, the membrane still has stable super-hydrophobic features and reusable water-in-oil emulsion separation performance even under exposure to diverse harsh conditions, including extremely acidic corrosive solutions and ultra-high temperature systems.

16.
Small ; 18(8): e2104561, 2022 02.
Artigo em Inglês | MEDLINE | ID: mdl-34716646

RESUMO

Hydrogen peroxide (H2 O2 ) is a mild but versatile oxidizing agent with extensive applications in bleaching, wastewater purification, medical treatment, and chemical synthesis. The state-of-art H2 O2 production via anthraquinone oxidation is hardly considered a cost-efficient and environment-friendly process because it requires high energy input and generates hazardous organic wastes. Photocatalytic H2 O2 production is a green, sustainable, and inexpensive process which only needs water and gaseous dioxygen as the raw materials and sunlight as the power source. Inorganic metal oxide semiconductors are good candidates for photocatalytic H2 O2 production due to their abundance in nature, biocompatibility, exceptional stability, and low cost. Progress has been made to enhance the photocatalytic activity toward H2 O2 production, however, H2 O2 photosynthesis is still in the laboratory research phase since the productivity is far from satisfaction. To inspire innovative ideas for boosting the H2 O2 yield in photocatalysis, the most well-studied metal oxide photocatalysts are selected and the modification strategies to improve their activity are listed. The mechanisms for H2 O2 production over modified photocatalysts are discussed to highlight the facilitating role of the modification methods. Besides, methods for the quantification of H2 O2 and associated radical intermediates are provided to guide future studies in this field.


Assuntos
Purificação da Água , Fontes de Energia Elétrica , Peróxido de Hidrogênio , Semicondutores , Luz Solar
17.
Adv Mater ; 34(6): e2108475, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34811811

RESUMO

Low-cost transition-metal chalcogenides (MSx ) are demonstrated to be potential candidate cocatalyst for photocatalytic H2 generation. However, their H2 -generation performance is limited by insufficient quantities of exposed sulfur (S) sites and their strong bonding with adsorbed hydrogen atoms (SHads ). To address these issues, an efficient coupling strategy of active-site-enriched regulation and electronic structure modification of active S sites is developed by rational design of core-shell Au@NiS1+ x nanostructured cocatalyst. In this case, the Au@NiS1+ x cocatalyst can be skillfully fabricated to synthesize the Au@NiS1+ x modified TiO2 (denoted as TiO2 /Au@NiS1+ x ) by a two-step route. Photocatalytic experiments exhibit that the resulting TiO2 /Au@NiS1+ x (1.7:1.3) displays a boosted H2 -generation rate of 9616 µmol h-1 g-1 with an apparent quantum efficiency of 46.0%  at 365 nm, which is 2.9 and 1.7 times the rate over TiO2 /NiS1+ x and TiO2 /Au, respectively. In situ/ex situ XPS characterization and density functional theory calculations reveal that the free-electrons of Au can transfer to sulfur-enriched NiS1+ x to induce the generation of electron-enriched Sδ - active centers, which boosts the desorption of Hads for rapid hydrogen formation via weakening the strong SHads bonds. Hence, an electron-enriched Sδ - -mediated mechanism is proposed. This work delivers a universal strategy for simultaneously increasing the active site number and optimizing the binding strength between the active sites and hydrogen adsorbates.

18.
Small Methods ; 5(11): e2100979, 2021 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-34927971

RESUMO

Coupling photocatalytic H2 production with organic synthesis attracts immense interest in the energy and chemical engineering field for the low-cost, clean, and sustainable generation of green energy and value-added products. Nevertheless, the performance of current photocatalysts is greatly limited by grievous charge recombination and tardy H2 evolution. To tackle these issues, a Pt nanocluster-modified ZnCdS solid solution is fabricated for photocatalytic H2 production and selective furfuralcohol oxidation. The internal electric field inside the ZnCdS and Schottky junction between ZnCdS and Pt nanoclusters drastically ameliorate charge separation. Meanwhile, the Pt nanoclusters remarkably expedite the H2 evolution kinetics on ZnCdS. As a result, the H2 production rate over Pt-loaded ZnCdS reaches 1045 µmol g-1 h-1 , which is about 26- and 70-fold that of CdS and ZnS, respectively. Under light irradiation for 3 h, the conversion of furfuralcohol to furfural reaches 71% with 89% furfural selectivity. The photocatalytic mechanism is investigated by in situ characterizations and theoretical calculations.

19.
Langmuir ; 37(48): 14114-14124, 2021 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-34808051

RESUMO

The design of photocatalysts with hierarchical pore sizes is an effective method to improve mass transport, enhance light absorption, and increase specific surface area. Moreover, the construction of a heterojunction at the interface of two semiconductor photocatalysts with suitable band positions plays a crucial role in separating and transporting charge carriers. Herein, ZIF-8 and urea are used as precursors to prepare hierarchically porous ZnO/g-C3N4 S-scheme heterojunction photocatalysts through a two-step calcination method. This S-scheme heterojunction photocatalyst shows high activity toward photocatalytic H2O2 production, which is 3.4 and 5.0 times higher than that of pure g-C3N4 and ZnO, respectively. The mechanism of charge transfer and separation within the S-scheme heterojunction is studied by Kelvin probe, in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS), and electron paramagnetic resonance (EPR). This research provides an idea of designing S-scheme heterojunction photocatalysts with hierarchical pores in efficient photocatalytic hydrogen peroxide production.

20.
Adv Mater ; 33(49): e2105135, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34622513

RESUMO

Single-atom photocatalysis has been demonstrated as a novel strategy to promote heterogeneous reactions. There is a diversity of monoatomic metal species with specific functions; however, integrating representative merits into dual-single-atoms and regulating cooperative photocatalysis remain a pressing challenge. For dual-single-atom catalysts, enhanced photocatalytic activity would be realized through integrating bifunctional properties and tuning the synergistic effect. Herein, dual-single-atoms supported on conjugated porous carbon nitride polymer are developed for effective photocatalytic CO2 reduction, featuring the function of cobalt (Co) and ruthenium (Ru). A series of in situ characterizations and theoretical calculations are conducted for quantitative analysis of structure-performance correlation. It is concluded that the active Co sites facilitate dynamic charge transfer, while the Ru sites promote selective CO2 surface-bound interaction during CO2 photoreduction. The combination of atom-specific traits and the synergy between Co and Ru lead to the high photocatalytic CO2 conversion with corresponding apparent quantum efficiency (AQE) of 2.8% at 385 nm, along with a high turnover number (TON) of more than 200 without addition of any sacrificial agent. This work presents an example of identifying the roles of different single-atom metals and regulating the synergy, where the two metals with unique properties collaborate to further boost the photocatalytic performance.

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