Sulfide-based all-solid-state battery (ASSB) with a lithium metal anode (LMA) is a promising candidate to surpass conventional Li-ion batteries owing to their inherent safety against fire hazards and potential to achieve a higher energy density. However, the narrow electrochemical stability window and chemical reactivity of the sulfide solid electrolyte towards the LMA results in interfacial degradation and poor electrochemical performance. In this direction, we introduce an organic additive approach, that is the mixing of prelithiated trithiocyanuric acid, LiTCA, with LiPSCl, to establish a stable interface while preserving high ionic conductivity.
View Article and Find Full Text PDFCellulose nanocrystals (CNCs) are bio-based, rod-like, high-aspect-ratio nanoparticles with high stiffness and strength and are widely used as a reinforcing nanofiller in polymer nanocomposites. However, due to hydrogen-bond formation between the large number of hydroxyl groups on their surface, CNCs are prone to aggregate, especially in nonpolar polymer matrices. One possibility to overcome this problem is to graft polymers from the CNCs' surfaces and to process the resulting "hairy nanoparticles" (HNPs) into one-component nanocomposites (OCNs) in which the polymer matrix and CNC filler are covalently connected.
View Article and Find Full Text PDFWe report the synthesis of two-dimensional and three-dimensional porous polyphenylenes (2D/3D-pPPs) the Diels-Alder cycloaddition polymerization reaction. The resulting 2D and 3D-pPPs showed surface areas up to 1553 m g, pore volumes of 1.45 cm g and very high H uptake capacities of 7.
View Article and Find Full Text PDFPhthalocyanines (PCs) are intriguing building blocks owing to their stability, physicochemical and catalytic properties. Although PC-based polymers have been reported before, many suffer from relatively low stability, crystallinity, and low surface areas. Utilizing a mixed-metal salt ionothermal approach, we report the synthesis of a series of metallophthalocyanine-based covalent organic frameworks (COFs) starting from 1,2,4,5-tetracyanobenzene and 2,3,6,7-tetracyanoanthracene to form the corresponding COFs named M-pPPCs and M-anPPCs, respectively.
View Article and Find Full Text PDFWe addressed the poor interfacial stability of the Li metal anode in Li-S batteries through molecular regulation of electrolytes using arylthiol additives with various numbers of anchoring sites. The dual functional tetrathiol additive markedly enhanced the Li anode interfacial stability, controlled the sulfur redox kinetics and suppressed side reactions towards polysulfides, thus leading to an improved capacity retention of 70% after 500 cycles at 1 C.
View Article and Find Full Text PDFPorous organic polymers (POPs) have gained tremendous attention owing to their chemical tunability, stability and high surface areas. Whereas there are several examples of fully conjugated two-dimensional (2D) POPs, three-dimensional (3D) ones are rather challenging to realize in the absence of structural templates. Herein, we report the base-catalyzed direct synthesis of a fully conjugated 3D POPs, named benzyne-derived polymers (BDPs), containing biphenylene and tetraphenylene moieties starting from a simple bisbenzyne precursor, which undergoes [2+2] and [2+2+2+2] cycloaddition reactions to form BDPs primarily composed of biphenylene and tetraphenylene moieties.
View Article and Find Full Text PDFPorous organic polymers (POPs) have long been considered as prime candidates for carbon dioxide (CO) capture, separation, and conversion. Especially their permanent porosity, structural tunability, stability and relatively low cost are key factors in such considerations. Whereas heteratom-rich microporous networks as well as their amine impregnation/functionalization have been actively exploited to boost the CO affinity of POPs, recently, the focus has shifted to engineering the pore environment, resulting in a new generation of highly microporous POPs rich in heteroatoms and featuring abundant catalytic sites for the capture and conversion of CO into value-added products.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2022
Tetraoxa[8]circulenes (TOCs) are a class of hetero[8]circulenes featuring a planar cyclooctatetraene core with a mixed aromatic/antiaromatic motif that governs their electronic properties. Polymeric TOCs (pTOCs) have been the subject of several computational simulations because they are predicted to be low-band-gap semiconductors, but they have not been available synthetically yet. Here, we report the first example of pTOCs, a new family of porous semiconductors, synthesized under ionothermal conditions through the intermolecular cyclization of 1,4,5,8-anthracene tetrone.
View Article and Find Full Text PDFWith the advent of silicon-based semiconductors, a plethora of previously unknown technologies became possible. The development of lightweight low-dimensional organic semiconductors followed soon after. However, the efficient charge/electron transfers enabled by the non-porous 3D structure of silicon is rather challenging to be realized by their (metal-)organic counterparts.
View Article and Find Full Text PDFDimensionality plays an important role in the charge transport properties of organic semiconductors. Although three-dimensional semiconductors, such as Si, are common in inorganic materials, imparting electrical conductivity to covalent three-dimensional organic polymers is challenging. Now, the synthesis of a three-dimensional π-conjugated porous organic polymer (3D p-POP) using catalyst-free Diels-Alder cycloaddition polymerization followed by acid-promoted aromatization is presented.
View Article and Find Full Text PDFDimethylaminocinnamaldehyde was re-evaluated as a wet contact reagent for the treatment of latent fingermarks on porous substrates. A new formulation (consisting of 0.028 g p-dimethylaminocinnamaldehyde, 0.
View Article and Find Full Text PDFThere are many groups and organizations across the government, private, and nonprofit sectors that are passionately engaged in the fight against Alzheimer's disease (AD), but they have constraints on their funding and scope and, therefore, cannot tackle the problem holistically. Addressing the complexities of this epidemic strategically will require the collective efforts of committed stakeholders. Individuals and organizations must work together to identify mutual interests and forge new relationships and partnerships.
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