The electrochemical CO reduction reaction (CORR) occurs at the nanoscale interface of the electrode-electrolyte. Therefore, tailoring the interfacial properties in the interface microenvironment provides a powerful strategy to optimise the activity and selectivity of electrocatalysts towards the desired products. Here, the microenvironment at the electrode-electrolyte interface of the flow-through Ag-based hollow fibre gas diffusion electrode (Ag HFGDE) is modulated by introducing surfactant cetyltrimethylammonium bromide (CTAB) as the electrolyte additive.
View Article and Find Full Text PDFUnwanted processes in metal anode batteries, e.g., non-uniform metal electrodeposition, electrolyte decomposition, and/or short-circuiting, are not fully captured by the electrolyte bulk solvation structure but rather defined by the electrode-electrolyte interface and its changes induced by cycling conditions.
View Article and Find Full Text PDFLithium-ion batteries are commonly used for energy storage due to their long lifespan and high energy density, but the use of unsafe electrolytes poses significant health and safety concerns. An alternative source is necessary to maintain electrochemical efficacy. This research demonstrates new safe glyme-based electrolytes for silica/carbon (SiO/C) nanocomposite derived from Australian rice husk (RH).
View Article and Find Full Text PDFδ-MnO is a promising cathode material for aqueous aluminium-ion batteries (AAIBs) for its layered crystalline structure with large interlayer spacing. However, the excellent Al ion storage performance of δ-MnO cathode remains elusive due to the frustrating structural collapse during the intercalation of high ionic potential Al ion species. Here, it is discovered that introducing heterogeneous metal dopants with high bond dissociation energy when bonded to oxygen can significantly reinforce the structural stability of δ-MnO frameworks.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs) represent a relatively new family of materials that attract lots of attention thanks to their unique features such as hierarchical porosity, active metal centers, versatility of linkers/metal nodes, and large surface area. Among the extended list of MOFs, Zr-based-MOFs demonstrate comparably superior chemical and thermal stabilities, making them ideal candidates for energy and environmental applications. As a Zr-MOF, NU-1000 is first synthesized at Northwestern University.
View Article and Find Full Text PDFCurrent energy and environmental challenges demand the development and design of multifunctional porous materials with tunable properties for catalysis, water purification, and energy conversion and storage. Because of their amenability to de novo reticular chemistry, metal-organic frameworks (MOFs) have become key materials in this area. However, their usefulness is often limited by low chemical stability, conductivity and inappropriate pore sizes.
View Article and Find Full Text PDFExploration of advanced carbon anode material is the key to circumventing the sluggish kinetics and poor rate capability for potassium ion storage. Herein, a synergistic synthetic strategy of engineering both surface and structure is adopted to design N, S co-doped carbon nanotubes (NS-CNTs). The as-designed NS-CNTs exhibit unique features of defective carbon surface, hollow tubular channel, and enlarged interlayer space.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs), or porous coordination polymers, are crystalline porous materials formed by coordination bonding between inorganic and organic species on the basis of the self-assembly of the reacting units. The typical characteristics of MOFs, including their large specific surface areas, ultrahigh porosities and excellent thermal and chemical stabilities, as well as their great potential for chemical and structural modifications, make them excellent candidates for versatile applications. Their poor electrical conductivity, however, has meant that they have not been useful for electrochemical applications.
View Article and Find Full Text PDFNanostructured copper selenide (Cu Se) attracts much interest as it shows outstanding performance as thermoelectric, photo-thermal, and optical material. The mesoporous structure is also a promising morphology to obtain better performance for electrochemical and catalytic applications, thanks to its high surface area. A simple one-step electrochemical method is proposed for mesoporous chalcogenides synthesis.
View Article and Find Full Text PDFA heterostructured porous carbon framework (PCF) composed of reduced graphene oxide (rGO) nanosheets and metal organic framework (MOF)-derived microporous carbon is prepared to investigate its potential use in a lithium-ion battery. As an anode material, the PCF exhibits efficient lithium-ion storage performance with a high reversible specific capacity (771 mA h g at 50 mA g), an excellent rate capability (448 mA h g at 1000 mA g), and a long lifespan (75% retention after 400 cycles). The transmission electron microscopy (TEM) study demonstrates that its unique three-dimensional (3D) heterostructure can largely tolerate the volume expansion.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2021
Effective dye separation and desalination are critical for the treatment of highly saline textile wastewater with dye mixtures. In this study, a graphene oxide (GO) membrane with a tunable interlayer distance () was fabricated to generate clean water two-stage filtration, namely, the dye/salt separation and desalination stages. In the first stage, under low pressure (e.
View Article and Find Full Text PDFThe conversion of nitrogen to ammonia offers a sustainable and environmentally friendly approach for producing precursors for fertilizers and efficient energy carriers. Owing to the large energy density and significant gravimetric hydrogen content, NH is considered an apt next-generation energy carrier and liquid fuel. However, the low conversion efficiency and slow production of ammonia through the nitrogen reduction reaction (NRR) are currently bottlenecks, making it an unviable alternative to the traditional Haber-Bosch process for ammonia production.
View Article and Find Full Text PDFSolid-state polymer electrolytes (SPEs) for high electrochemical performance lithium-ion batteries have received considerable attention due to their unique characteristics; they are not prone to leakage, and they exhibit low flammability, excellent processability, good flexibility, high safety levels, and superior thermal stability. However, current SPEs are far from commercialization, mainly due to the low ionic conductivity, low Li transference number (t ), poor electrode/electrolyte interface contact, narrow electrochemical oxidation window, and poor long-term stability of Li metal. Recent work on improving electrochemical performance and these aspects of SPEs are summarized systematically here with a particular focus on the underlying mechanisms, and the improvement strategies are also proposed.
View Article and Find Full Text PDFHerein, the synergistic effects of hollow nanoarchitecture and high specific surface area of hollow activated carbons (HACs) are reported with the superior supercapacitor (SC) and capacitive deionization (CDI) performance. The center of zeolite imidazolate framework-8 (ZIF-8) is selectively etched to create a hollow cavity as a macropore, and the resulting hollow ZIF-8 (HZIF-8) is carbonized to obtain hollow carbon (HC). The distribution of nanopores is, subsequently, optimized by KOH activation to create more nanopores and significantly increase specific surface area.
View Article and Find Full Text PDFNitrogen-doped mesoporous carbon microspheres have been successfully synthesized via a spray drying-vapor deposition method for the first time, using commercial Ludox silica nanoparticles as hard templates. Compared to freeze-drying and air-drying methods, mesoporous carbon with a higher packing density can be achieved through the spray drying method. Vapor deposition of polypyrrole followed by carbonization and etching is beneficial for the generation of ultra-thin carbon network.
View Article and Find Full Text PDFThe development of pseudocapacitive materials for energy-oriented applications has stimulated considerable interest in recent years due to their high energy-storing capacity with high power outputs. Nevertheless, the utilization of nanosized active materials in batteries leads to fast redox kinetics due to the improved surface area and short diffusion pathways, which shifts their electrochemical signatures from battery-like to the pseudocapacitive-like behavior. As a result, it becomes challenging to distinguish "pseudocapacitive" and "battery" materials.
View Article and Find Full Text PDFOrganic polymers have attracted significant interest as electrodes for energy storage devices because of their advantages, including molecular flexibility, cost-effectiveness, and environmentally friendly nature. Nevertheless, the real implementation of polymer-based electrodes is restricted by their poor stability, low capacity, and slow electron-transfer/ion diffusion kinetics. In this work, a sandwich-structured composite of ordered mesoporous polydopamine (OMPDA)/TiCT has been fabricated by in situ polymerization of dopamine on the surface of TiCT via employing the PS--PEO block polymer as a soft template.
View Article and Find Full Text PDFSelenium (Se)-based rechargeable aluminum batteries (RABs), known as aluminum-selenium (Al-Se) batteries, are an appealing new battery design that holds great promise for addressing the low-capacity problem of current RAB technology. However, their applications are hindered by mediocre high-rate capacity (≈100 mAh g at 0.5 A g ) and insufficient cycling life (50 cycles).
View Article and Find Full Text PDFTo sustainably satisfy the growing demand for energy, organic carbonyl compounds (OCCs) are being widely studied as electrode active materials for batteries owing to their high capacity, flexible structure, low cost, environmental friendliness, renewability, and universal applicability. However, their high solubility in electrolytes, limited active sites, and low conductivity are obstacles in increasing their usage. Here, the nucleophilic addition reaction of aromatic carbonyl compounds (ACCs) is first used to explain the electrochemical behavior of carbonyl compounds during charge-discharge, and the relationship of the molecular structure and electrochemical properties of ACCs are discussed.
View Article and Find Full Text PDFUnderstanding how mesoporous noble metal architectures affect electrocatalytic performance is very important for the rational design and preparation of high-performance electrocatalysts. Herein, by using polymeric micelle-assembled structures as templates, mesoporous Pd nanoparticles with tunable porous constructions are synthesized by simply tuning the solvent compositions. The effect of porous Pd nanoparticles on the electrocatalytic performance is thoroughly studied.
View Article and Find Full Text PDFIn large-scale, hydrogen production from water-splitting represents the most promising solution for a clean, recyclable, and low-cost energy source. The realization of viable technological solutions requires suitable efficient electrochemical catalysts with low overpotentials and long-term stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) based on cheap and nontoxic materials. Herein, we present a unique molecular approach to monodispersed, ultra-small, and superiorly active iron phosphide (FeP) electrocatalysts for bifunctional OER, HER, and overall water-splitting.
View Article and Find Full Text PDFThe shuttling phenomena in lithium-sulfur batteries lead to drastic attenuation of the capacity. This can be suppressed effectively by modifying the separator. Herein, a double-layered separator composed of a macroporous polypropylene (PP) matrix layer and an arrayed poly(methyl methacrylate) (PMMA) microsphere retarding layer is designed as the separator for lithium-sulfur batteries.
View Article and Find Full Text PDFPseudocapacitance, which is the storage of charge based on continuous and fast reversible redox reactions at the surface of electrode materials, is commonly observed for electrodes in lithium ion batteries, especially for transition metal oxide anodes. In this report, bare Fe2O3 of granular morphology (∼30 nm in diameter) with high purity and decent crystallinity as well as recommendable electrochemical performances is fabricated hydrothermally and employed as the subject to clarify pseudocapacitive behavior in transition metal oxide anodes. Electrochemical technologies such as galvanostatic charging/discharging, differential capacity analysis (dQ/dV) and the power law relationship (i = aνb), which can distinguish pseudocapacitive behaviors of an electrode reaction were employed to analyze the electrodes.
View Article and Find Full Text PDFHerein, we report a novel method for the formation of hollow Prussian blue analogue (CoFe-PBA) nanocubes, using spherical silica particles as sacrificial templates. In the first step, silica cores are coated by a CoFe-PBA shell and then removed by etching with hydrofluoric acid (HF). The cubic shape of CoFe-PBA is well-retained even after the removal of the silica cores, resulting in the formation of hollow CoFe-PBA cubes.
View Article and Find Full Text PDFOrdered mesoporous nitrogen-doped carbon (OMNC) materials are considered as the most promising material for supercapacitors. In this study, a highly ordered two-dimensional (2D) hexagonal mesostructured polymer was synthesized through a facile assembly of triblock polymer micelles and phenol-melamine/formaldehyde resin via an organic-organic assembly process in aqueous solution. After calcination, the novel OMNC materials with 2D hexagonal mesostructures were obtained.
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