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1.
Small ; 20(22): e2309226, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38126680

RESUMO

Developing efficient electrocatalysts for methanol oxidation reaction (MOR) is crucial in advancing the commercialization of direct methanol fuel cells (DMFCs). Herein, carbon-supported 0D/2D PtCuBi/C (0D/2D PtCuBi/C) catalysts are fabricated through a solvothermal method, followed by a partial electrochemical dealloying process to form a novel mixed-dimensional electrochemically dealloyed PtCuBi/C (0D/2D D-PtCuBi/C) catalysts. Benefiting from distinctive mixed-dimensional structure and composition, the as-obtained 0D/2D D-PtCuBi/C catalysts possess abundant accessible active sites. The introduction of Cu as a water-activating element weakens the COads, and oxophilic metal Bi facilitates the OHads, thereby enhancing its tolerance to CO poisoning and promoting MOR activity. The X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure spectroscopy (XAFS) collectively reveal the electron transfer from Cu and Bi to Pt, the electron-enrichment effect induced by dealloying, and the strong interactions among Pt-M (Cu, Pt, and Bi) multi-active sites, which improve the tuning of the electronic structure and enhancement of electron transfer ability. Impressively, the optimized 0D/2D D-PtCuBi/C catalysts exhibit the superior mass activity (MA) of 17.68 A mgPt -1 for MOR, which is 14.86 times higher than that of commercial Pt/C. This study offers a proposed strategy for Pt-based alloy catalysts, enabling their use as efficient anodic materials in fuel cell applications.

2.
Planta ; 258(4): 79, 2023 Sep 12.
Artigo em Inglês | MEDLINE | ID: mdl-37698688

RESUMO

MAIN CONCLUSION: Multiplexed Cas9-based genome editing of cotton resulted in reduction of viral load with asymptomatic cotton plants. In depth imaging of proteomic dynamics of resulting CLCuV betasatellite and DNA-A protein was also performed. The notorious  cotton leaf curl virus (CLCuV), which is transmitted by the sap-sucking insect whitefly, continuously damages cotton crops. Although the application of various toxins and RNAi has shown some promise, sustained control has not been achieved. Consequently, CRISPR_Cas9 was applied by designing multiplex targets against DNA-A (AC2 and AC3) and betasatellite (ßC1) of CLCuV using CRISPR direct and ligating into the destination vector of the plant using gateway ligation method. The successful ligation of targets into the destination vector was confirmed by the amplification of 1049 bp using a primer created from the promoter and target, while restriction digestion using the AflII and Asc1 enzymes determined how compact the plasmid developed and the nucleotide specificity of the plasmid was achieved through Sanger sequencing. PCR confirmed the successful introduction of plasmid into CKC-1 cotton variety. Through Sanger sequencing and correlation with the mRNA expression of DNA-A and betasatellite in genome-edited cotton plants subjected to agroinfiltration of CLCuV infectious clone, the effectiveness of knockout was established. The genome-edited cotton plants demonstrated edited efficacy of 72% for AC2 and AC3 and 90% for the (ßC1) through amplicon sequencing, Molecular dynamics (MD) simulations were used to further validate the results. Higher RMSD values for the edited ßC1 and AC3 proteins indicated functional loss caused by denaturation. Thus, CRISPR_Cas9 constructs can be rationally designed using high-throughput MD simulation technique. The confidence in using this technology to control plant virus and its vector was determined by the knockout efficiency and the virus inoculation assay.


Assuntos
Sistemas CRISPR-Cas , Gossypium , Carga Viral , Gossypium/genética , Sistemas CRISPR-Cas/genética , Proteômica , DNA
3.
Chem Commun (Camb) ; 59(81): 12152-12155, 2023 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-37740343

RESUMO

Mo-doped NiCo Prussian blue analogue (PBA) electrocatalysts self-supported on Ni foam are elaborately designed, which exhibit a low potential of 1.358 V (vs. RHE) to reach 100 mA cm-2 for catalyzing the urea oxidation reaction (UOR). The incorporation of high-valence Mo (+6) modifies the electronic structure and improves the electron transfer ability. Using X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) techniques, we confirm the effect of Mo doping on the NiCo PBA electronic structure.

4.
Nat Commun ; 12(1): 6766, 2021 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-34799571

RESUMO

Single-atom-catalysts (SACs) afford a fascinating activity with respect to other nanomaterials for hydrogen evolution reaction (HER), yet the simplicity of single-atom center limits its further modification and utilization. Obtaining bimetallic single-atom-dimer (SAD) structures can reform the electronic structure of SACs with added atomic-level synergistic effect, further improving HER kinetics beyond SACs. However, the synthesis and identification of such SAD structure remains conceptually challenging. Herein, systematic first-principle screening reveals that the synergistic interaction at the NiCo-SAD atomic interface can upshift the d-band center, thereby, facilitate rapid water-dissociation and optimal proton adsorption, accelerating alkaline/acidic HER kinetics. Inspired by theoretical predictions, we develop a facile strategy to obtain NiCo-SAD on N-doped carbon (NiCo-SAD-NC) via in-situ trapping of metal ions followed by pyrolysis with precisely controlled N-moieties. X-ray absorption spectroscopy indicates the emergence of Ni-Co coordination at the atomic-level. The obtained NiCo-SAD-NC exhibits exceptional pH-universal HER-activity, demanding only 54.7 and 61 mV overpotentials at -10 mA cm-2 in acidic and alkaline media, respectively. This work provides a facile synthetic strategy for SAD catalysts and sheds light on the fundamentals of structure-activity relationships for future applications.

5.
ACS Omega ; 5(41): 26845-26854, 2020 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-33111010

RESUMO

Recently, a new class of two-dimensional (2D) materials, called MXene, consisting of layers of transition-metal carbides and nitrides/carbonitrides has been introduced. MXene, a multifunctional material with hydrophilic nature and excellent electrical conductivity and chemical stabilities, can be applied in diverse research areas such as energy harvesting and its storage, water purification, thermal dissipation, and gas sensing. To achieve the best quality of MXene, optimization of some important synthetic parameters is highly required such as an optimized etchant concentration to remove an "A" element from the MAX phase and sonication time for the efficient exfoliation of MXene flakes. Besides, there is a need to disclose that particular solvent through which intercalation can easily be achieved. In this work, we optimized the abovementioned critical parameters for the synthesis of good-quality MXene. Our results clearly explain the variations in the quality of MXene under applied etchant concentrations, solvents for better intercalation, and optimization of sonication time for better exfoliation. The obtained results suggest that 30% HF as an etchant, dimethyl sulfoxide (DMSO) as a solvent, and 135 min as the sonication time are effective parameters for the synthesis of good-quality MXene. We expect that this report will be helpful for the young research community to synthesize good-quality MXene with the required properties.

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