Binary Nd-Ce oxides encapsuled in carbon nanotubes (CNTs) catalysts were synthesized and evaluated in the coupling reaction of ethylbenzene (EB) dehydrogenation and NO decomposition, a promising strategy for styrene (ST) production while mitigating greenhouse gas emissions. The optimized Nd - Ce@CNTs exhibited competitive catalytic performance with an EB conversion of 76 % and a ST selectivity of 71 % compared to Ce@CNTs, highlighting a synergic effect between Ce and Nd in the oxidation dehydrogenation of EB with NO as an oxidant (NO-ODEB). Characterization results indicated that Nd incorporation induced lattice distortions, evident in the expansion or contraction of Ce - O bonds surrounding Nd.
View Article and Find Full Text PDFVinyl-bearing triazine-functionalized covalent organic frameworks (COFs) have emerged as promising materials for electrocatalysis and energy storage. Guided by density functional theory calculations, a vinyl-enriched COF (VCOF-1) featuring a donor-acceptor structure was synthesized based on the Knoevenagel reaction. Moreover, the VCOF-1@Ru without pyrolysis was obtained through chemical coordination interactions between VCOF-1 and RuCl, exhibiting enhanced electrocatalytic performance in the hydrogen evolution reaction when exposed to 0.
View Article and Find Full Text PDFIt is significant to tailor multifunctional electrode materials for storing sustainable energy in lithium-sulfur (Li-S) batteries and converting intermittent solar energy into H, facilitated by electricity. In this context, COF-1@CNT obtained through interfacial interaction fulfilled both requisites via post-functionalization. Upon integrating COF-1@CNT with S as the cathode for Li-S batteries, the system exhibited an initial discharge capacity of 1360 mAh g.
View Article and Find Full Text PDFIt is worthwhile to explore and develop multifunctional composites with unique advantages for energy conversion and utilization. Post-synthetic modification (PSM) strategies can endow novel properties to already excellent covalent organic frameworks (COFs). In this study, we prepared a range of COF-based composites via a multi-step PSM strategy.
View Article and Find Full Text PDFCovalent organic frameworks (COFs) are considered as a class of potential candidates for energy storage and catalysis. In this work, a COF containing sulfonic groups was prepared to be a modified separator in lithium-sulfur batteries (LSBs). Benefiting from the charged sulfonic groups, the COF-SO cell exhibited higher ionic conductivity (1.
View Article and Find Full Text PDFACS Appl Mater Interfaces
March 2023
Lithium-ion capacitors (LICs) attract enormous attention because of the urgent demands for high power and energy density devices. However, the intrinsic imbalance between anodes and cathodes with different charge-storage mechanisms blocks the further improvement in energy and power density. MXenes, novel two-dimensional materials with metallic conductivity, accordion-like structure, and regulable interlayer spacing, are widely employed in electrochemical energy storage devices.
View Article and Find Full Text PDFA unique porous material, namely, MXene/SiO hybrid aerogel, with a high surface area, was prepared via sol-gel and freeze-drying methods. The hierarchical porous hybrid aerogel possesses a three-dimensional integrated network structure of SiO cross-link with two-dimensional MXene; it is used not only as a scaffold to prepare sulfur-based cathode material, but also as an efficient functional separator to block the polysulfides shuttle. MXene/SiO hybrid aerogel as sulfur carrier exhibits good electrochemical performance, such as high discharge capacities (1007 mAh g at 0.
View Article and Find Full Text PDFNovel covalent organic framework (COF) composites containing a bipyridine multimetal complex were designed and obtained via the coordination interaction between bipyridine groups and metal ions. The obtained Pt and polyoxometalate (POM)-loaded COF complex (POM-Pt@COF-TB) exhibited excellent oxidation of methane. In addition, the resultant Co/Fe-based COF composites achieved great performance in an electrocatalytic oxygen evolution reaction (OER).
View Article and Find Full Text PDFThe development of functional covalent organic frameworks (COFs) with specific properties is an emerging research field. In the current work, COF-SQ-Ph was synthesized through the aza-Diels-Alder reaction between phenylacetylene and the matrix COF-SQ (triazine-based COF) generated from the organic monomers 2, 4, 6-tris(4-aminophenyl)-1, 3, 5-triazine and 2, 5-dimethoxyterephthalaldehyde in flask. The functionalized COF-SQ-Ph with an extended π-conjugated structure and enhanced structural stability was used as the sulfur loading recipient to prepare sulfur cathodes for lithium-sulfur batteries.
View Article and Find Full Text PDFA pyrimidine-modified covalent organic framework (COF-Pyr) was designed to be synthesized via the Povarov reaction. The nitrogen atom on the pyrimidine showed excellent coordination ability to metal ions. Their stable metal composite material (Co@COF-Pyr) exhibited remarkable performance for electrocatalytic oxygen evolution reaction (OER) in 1.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2021
In order to reduce the negative impact of the extra carbon coating on the electrochemical properties of the commonly sandwiched carbon nanotubes@tin dioxide@carbon (CNT@SnO@C) composites, the external C coating has been designed as a porous carbon in this work. The well-designed porous carbon coating offers an attractive advantage compared to the common carbon coatings, namely, it can not only better mitigate the volumetric variation of SnO by means of its spongy structure with better flexibility and rich free space, but also accelerate the lithium-ions diffusion by virtue of its open tunnel-like architecture. For this reason, this composite prepared here shows outstanding electrochemical performance stemming from the cooperative effect of inner CNT supporting and externally porous carbon coating, displaying 819.
View Article and Find Full Text PDFThe structure of Ni films is essential to their electrocatalytic performance for hydrogen evolution reaction (HER). The pH value and EDTA (ethylene diamine tetraacetic acid) additive are important factors for the structure control of electrodeposited metal films due to their adjustment of metal electrocrystallization and hydrogen evolution side reactions. The structures of Ni films from 3D (three-dimensional) porous to compact and flat structure are electrodeposited by adjusting solution pH values or adding EDTA.
View Article and Find Full Text PDFCovalent organic frameworks (COFs) with pre-designed structure and customized properties have been employed as sulfur storage materials for lithium-sulfur (Li-S) batteries. In this work, a cationic mesoporous COF (COF-NI) was synthesized by grafting a quaternary ammonium salt group onto the pore channel of COFs via a one-pot three components tandem reaction strategy. The post-functionalized COFs were utilized as the matrix framework to successfully construct the Li-S battery with high-speed capacity and long-term stability.
View Article and Find Full Text PDFThe first convergent total synthesis for the proposed structures of microcyclamides MZ602 () and MZ568 () has been accomplished in 11 linear steps with 12.5 and 16.8% overall yield, respectively.
View Article and Find Full Text PDFOwing to specific formation of five-membered or six-membered cyclic esters between boric acid groups and cis-diol molecules, boric acid bearing fluorescent materials can not only selectively capture but also specifically identify cis-diol substances. In this work, a novel covalent organic framework containing boric acid groups (COF-BA) was prepared through post-modification via the aza-Diels-Alder cycloaddition reaction. COF-BA with good stability, a permanent pore structure, a high specific surface area (606 m2 g-1) and a uniform pore size (2.
View Article and Find Full Text PDFLithium-sulfur batteries are considered as the next generation of energy storage systems because of their high theoretical specific capacity and energy density. Unfortunately, the sluggish reaction kinetics, weak adsorption toward to lithium polysulfides, and slow lithium ion diffusion impede the smooth electrochemical process, resulting in the lithium-sulfur batteries with the unsatisfactory cycling stability and rate performance. Since it is recognized that polar metal oxides and doped nitrogen in carbon materials have chemical interaction with lithium polysulfides, a nanostructured nitrogen-doped porous carbon/MoO composite is synthesized through a simple hydrothermal method by using graphene oxide nanoribbon and phosphomolybdic acid hydrate as precursors.
View Article and Find Full Text PDFDespite the fact that lithium-sulfur batteries are regarded as promising next-generation rechargeable battery systems owning to high theoretical specific capacity (1675 mA h g) and energy density (2600 W h kg), several issues such as poor electrical conductivity, sluggish redox kinetics, and severe "shuttle effect" in electrodes still hinder their practical application. MXenes, novel two-dimensional materials with high conductivity, regulable interlayer spacing, and abundant functional groups, are widely applied in energy storage and conversion fields. In this work, a TiC/carbon hybrid with expanded interlayer spacing is synthesized by one-step heat treatment in molten potassium hydroxide.
View Article and Find Full Text PDFIn this study, we have prepared novel pyrrole-formaldehyde polymers through polymerizing pyrrole and formaldehyde in the mixture solvent of water and ethanol by using hydrochloric acid as a catalyst. The as-synthesized polymers possess a nitrogen content of 6.7 atom % and are composed of spherical particles with the diameter of approximately 1-3 μm.
View Article and Find Full Text PDFA nanostructured porous carbon (NPC) is prepared by using a facile physical activation method, with nitrogen-doped graphene nanoribbon aerogel and carbon dioxide as a precursor and an activating agent, respectively. The morphology, porosity parameters, and chemical properties of the as-prepared NPC have been revealed by using various characterization methods, including scanning electron microscopy, nitrogen sorption analysis, and X-ray photoelectron spectroscopy (XPS). The NPC with a moderate nitrogen content (5.
View Article and Find Full Text PDFIn this work, a series of highly porous sulfur-doped carbons are prepared through physical activation methods by using polythiophene as a precursor. The morphology, structure, and physicochemical properties are revealed by a variety of characterization methods, such as scanning electron microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, and nitrogen sorption measurement. Their porosity parameters and chemical compositions can be well-tuned by changing the activating agents (steam and carbon dioxide) and reaction temperature.
View Article and Find Full Text PDFMetal-organic frameworks (MOFs) are hybrid inorganic-organic materials that can be used as effective precursors to prepare various functional nanomaterials for energy-related applications. Nevertheless, most MOF-derived metal oxides exhibit low electrical conductivity and mechanical strain. These characteristics limit their electrochemical performance and hamper their practical application.
View Article and Find Full Text PDFLithium-sulfur batteries have attracted great concern because of the high theoretical capacity of sulfur (1675 mA h g). However, the poor electrical conductivity and volumetric expansion of sulfur along with the dissolution of lithium polysulfides largely limit their practical application. In this study, nitrogen-doped graphene aerogel (NGA) with high nitrogen content and porosity is used as a host for the impregnation of sulfur.
View Article and Find Full Text PDFCore-shell structured nitrogen-doped porous carbon@silica material with uniform structure and morphology was synthesized via a sol-gel method. During this process, a commercial triblock copolymer and the in situ formed pyrrole-formaldehyde polymer acted as cotemplates, while tetraethyl orthosilicate acted as silica precursor. The synergetic effect of the triblock copolymer and the pyrrole-formaldehyde polymer enables the formation of the core-shell structure.
View Article and Find Full Text PDFIn this study, a facile method for synthesizing a novel graphene oxide/pyrrole-formaldehyde (GOP-1) composite hydrogel was developed via in situ polymerization of pyrrole and formaldehyde in the presence of graphene oxide sheets without any additional catalyst. During the polymerization, graphene oxide can act as a two-dimensional template to regulate the aggregation state of polymer and as an acid catalyst to accelerate the reaction rate of pyrrole and formaldehyde. The morphology and microstructure were investigated by scanning electron microscopy, transmission electron microscopy, and X-ray diffraction, respectively.
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