Electron spin polarization is identified as a promising avenue for enhancing the oxygen evolution reaction (OER), which is the bottleneck that limits the energy efficiency of water-splitting. Here, we report that both ferrimagnetic (f-FeO) and superparamagnetic iron oxide (s-FeO) catalysts can exhibit external magnetic field (Hext)-induced OER enhancement, and the activity is proportional to their intrinsic magnetic moment. Additionally, the chirality-induced spin selectivity (CISS) effect was utilized in synergy with Hext to get a maximum enhancement of up to 89% improvement in current density (at 1.
View Article and Find Full Text PDFAdditive manufacturing, also called 3D printing, has the potential to enable the development of flexible, wearable and customizable batteries of any shape, maximizing energy storage while also reducing dead-weight and volume. In this work, for the first time, three-dimensional complex electrode structures of high-energy density LiNiMnCoO (NMC 111) material are developed by means of a vat photopolymerization (VPP) process combined with an innovative precursor approach. This innovative approach involves the solubilization of metal precursor salts into a UV-photopolymerizable resin, so that detrimental light scattering and increased viscosity are minimized, followed by the in-situ synthesis of NMC 111 during thermal post-processing of the printed item.
View Article and Find Full Text PDFTailoring the curvature-directed lattice strain in GNRs along with optimal surface anchoring of molybdenum disulfide (MoS) quantum dots (QDs) can lead to a unique heterostructure with Pt-like HER activity (onset potential -60 mV). The curvature-induced electronic charge redistribution at the curved region in the graphene nanoribbons allows a facile GNR-MoS interfacial charge transfer in the heterostructure, making the interfacial sulfur (S) more active towards the HER. The density functional theory (DFT) calculations confirmed electronically activated interfacial S-based catalytic centers in the curved GNR-based heterostructure leading to Pt-like HER activity.
View Article and Find Full Text PDFThe objective of the current study is to evaluate both the positive and negative effects of manganese-doped graphene quantum dots (GQD-Mn) on Capsicum annuum L. grown under salt stress. GQD-Mn was synthesized, characterized, and foliar-applied (250 mg/L, 120 mg/L, 60 mg/L) to C.
View Article and Find Full Text PDFA new isolation protocol was recently reported for highly purified metallic Fullertubes D -C , D -C , and D -C which exhibit unique electronic features. Here, we report the oxygen reduction electrocatalytic behavior of C , C (spheroidal fullerenes), and C , C , and C (tubular fullerenes) using a combination of experimental and theoretical approaches. C (a metal-free catalyst) displayed remarkable oxygen reduction reaction (ORR) activity, with an onset potential of 0.
View Article and Find Full Text PDFConsiderable efforts are being made to find cheaper and more efficient alternatives to the currently commercially available catalysts based on precious metals for the Hydrogen Evolution Reaction (HER). In this context, fullerenes have started to gain attention due to their suitable electronic properties and relatively easy functionalization. We found that the covalent functionalization of C, C and ScN@C with diazonium salts endows the fullerene cages with ultra-active charge polarization centers, which are located near the carbon-diazonium bond and improve the efficiency towards the molecular generation of hydrogen.
View Article and Find Full Text PDFFacile electron transport and intimate electronic contact at the catalyst-electrode interface are critical for the ideal performance of electrochemical devices such as glucose biofuel cells and biosensors. Here, through a comprehensive experimental-theoretical exploration, we demonstrate that engineering of interfacial properties, including interfacial electron dynamics, electron affinity, electrode-catalyst-adsorbate electrical synergy, and electrocatalytically active surface area, can lead to highly efficient graphene-based electrochemical devices. We selected two closely related but electronically and surface chemically different functionalized graphene analogues-graphene acid (GA) and reduced graphene oxide (rGO)-as the model graphenic platforms.
View Article and Find Full Text PDFThe electrocatalytic properties of some endohedral fullerenes for hydrogen evolution reactions (HER) were recently predicted by DFT calculations. Nonetheless, the experimental catalytic performance under realistic electrochemical environments of these 0D-nanomaterials have not been explored. Here, for the first time, we disclose the HER electrocatalytic behavior of seven MN@2 (2 = 68, 78, and 80) fullerenes (GdN@(7)-C, YN@(7)-C, LuN@(7)-C, ScN@(7)-C, ScN@(6)-C, ScN@(5)-C, and ScN@(6140)-C) using a combination of experimental and theoretical techniques.
View Article and Find Full Text PDFPlatinum (Pt)-based-nanomaterials are currently the most successful catalysts for the oxygen reduction reaction (ORR) in electrochemical energy conversion devices such as fuel cells and metal-air batteries. Nonetheless, Pt catalysts have serious drawbacks, including low abundance in nature, sluggish kinetics, and very high costs, which limit their practical applications. Herein, we report the first rationally designed nonprecious Co-Cu bimetallic metal-organic framework (MOF) using a low-temperature hydrothermal method that outperforms the electrocatalytic activity of Pt/C for ORR in alkaline environments.
View Article and Find Full Text PDFFullerene-based low-dimensional (LD) heterostructures have emerged as excellent energy conversion materials. We constructed van der Waals 1T-MoS/C 0D-2D heterostructures via a one-pot synthetic approach for catalytic hydrogen generation. The interfacial 1T-MoS-C and C-C interactions as well as their electrocatalytic properties were finely controlled by varying the weight percentages of the fullerenes.
View Article and Find Full Text PDFThe rational design of multifunctional catalysts that use non-noble metals to facilitate the interconversion between H, O, and HO is an intense area of investigation. Bimetallic nanosystems with highly tunable electronic, structural, and catalytic properties that depend on their composition, structure, and size have attracted considerable attention. Herein, we report the synthesis of bimetallic nickel-copper (NiCu) alloy nanoparticles confined in a sp carbon framework that exhibits trifunctional catalytic properties toward hydrogen evolution (HER), oxygen reduction (ORR), and oxygen evolution (OER) reactions.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2020
Antioxidants derived from nature, such as ellagic acid (EA), demonstrated high potency to mitigate neuronal oxidative stress and related pathologies, including Parkinson's disease. However, the application of EA is limited due to its toxicity at moderate doses and poor solubility, cellular permeability, and bioavailability. Here, we introduce a sustainably resourced, green nanoencasement strategy to overcome the limitations of EA and derive synergistic effects to prevent oxidative stress in neuronal cells.
View Article and Find Full Text PDFThis work for the first time unfurls the fundamental mechanisms and sets the stage for an approach to derive electrocatalytic activity, which is otherwise not possible, in a traditionally known wide band-gap oxide material. Specifically, we report on the tunable optical properties, in terms of wide spectral selectivity and red-shifted band gap, and electrocatalytic behavior of iron (Fe)-doped gallium oxide (β-GaO) model system. X-ray diffraction (XRD) studies of sintered Ga Fe O (GFO) (0.
View Article and Find Full Text PDFThe presence of highly modifiable chemical functional groups, abundance of functional groups, and their biological origin make proteins an important class of biomaterials from a fundamental science and applied engineering perspective. Hence, the utilization of proteins from the animal rendering industry (animal protein, AP) for high-value, nonfeed, and nonfertilizer applications is intensely pursued. Although this leads to the exploration of protein-derived plastics as a plausible alternative, the proposed methods are energy-intensive and not based on protein in its native form, which leads to high processing and production costs.
View Article and Find Full Text PDFThe 1990s saw a revolution in our understanding of the protein folding pathways of both disulfide-bond-containing proteins and purely conformational folders. High-resolution maps of the folding trajectories, made possible by innovative experimental design, revealed the presence of multiple intermediates, their formation and consumption, and the network of interactions between them that lead to the formation of the folded protein from its unfolded state. The same level of detail has heretofore remained elusive as far as the amyloid aggregation pathways of prion-like proteins are concerned.
View Article and Find Full Text PDFInroads into understanding the process by which amyloid proteins become toxic have been hampered by the lack of experimental techniques that adequately resolve the process. Recently, tip-enhanced Raman spectroscopy, with its unique capability to spectroscopically image and chemically identify reaction mixtures with nanoscale precision, was used to obtain a high-resolution roadmap of the soluble-to-toxic conversion of amyloid beta. This technique opens the door for studying the toxic aggregation pathways of other amyloid proteins and spurs efforts devoted to prophylactic and therapeutic intervention in neurodegenerative and protein-misfolding-related disorders.
View Article and Find Full Text PDFCurvature-induced dipole moment and orbital rehybridization in graphene wrinkles modify its electrical properties and induces transport anisotropy. Current wrinkling processes are based on contraction of the entire substrate and do not produce confined or directed wrinkles. Here we show that selective desiccation of a bacterium under impermeable and flexible graphene via a flap-valve operation produces axially aligned graphene wrinkles of wavelength 32.
View Article and Find Full Text PDFThe walnut peptides and zinc ions were combined to generate a walnut peptides-zinc complex (WP1-Zn) with enhanced antiproliferative ability as well as reduced toxicity. The result indicated that Zn ions were successfully combined with WP1 through Zn-N and Zn-O covalent bonds. WP1-Zn compounds exhibited strong antiproliferative ability against the selected human cell lines, especially MCF-7 cells, whose survival rate reduced to 20.
View Article and Find Full Text PDF