Chem Commun (Camb)
September 2025
Aqueous batteries have garnered significant attention as compelling contenders for large-scale energy storage owing to their inherent safety, cost-effectiveness, and environmental sustainability. Significant endeavors have been dedicated to develop redox-active organic cathode materials, which is considered a crucial factor driving the development of aqueous batteries. Among various cathodes, carbonyl-rich organic compounds demonstrate exceptional potential in view of their strong electroactivity, ion-coupling sensitivity and structural versatility.
View Article and Find Full Text PDFCarbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors, but their tailor-made design to optimize the capacitive activity remains a confusing topic. Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures (SCSs) for Zn-ion storage with double-high capacitive activity and durability. Tetrachlorobenzoquinone (H-bond acceptor) and dimethylbenzidine (H-bond donator) can interact to form organic nanosheet modules, which are sequentially assembled, orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds (N-H···O).
View Article and Find Full Text PDFHigh-voltage p-type organic cathodes are attracting broad attention for boosting zinc batteries, but are hindered by single-electron reactions and low utilization of redox sites due to high reaction energy barriers with incompatible anions. Here we design polyheterocycle organics (PHOs) grafting dual-site-active phenothiazine and piperazine motifs to form donor-acceptor-extended structures which show multi-electron p-type redox reactions for superior anion storage. With the decrease in anionic Stokes radius and the increase in charge density (TFSI → OTF → SO ), SO exhibits the strongest bipedal ion-pairing ability with PHOs during oxidation an ultralow activation energy (0.
View Article and Find Full Text PDFNH/H ions with small hydration sizes, light weight and rapid (de)coordination dynamics have emerged as promising charge carriers for advanced aqueous zinc-organic batteries (ZOBs). However, the limited-density redox sites and high redox barrier of NH/H migration in organics pose significant challenges for advancing ZOBs. Herein, conjugated nanofibrous organic (CFO) cathodes with high-density carbonyl/imine redox sites are designed for superior non-metallic ion co-storage through π-π stacking interactions between benzene-1,3,5-tricarbaldehyde and 2,6-diaminoanthraquinone nanofibrous polymer molecular chains.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2025
Organic p-type cathode materials with high redox potentials and fast kinetics have captured widespread attention in propelling Zn-organic batteries (ZOBs). However, their anion-accessible capacity is insufficient due to single electron reaction and/or high energy barrier of each redox-active unit. Here, we design two-electron-donating p-type organic chalcogen small molecules (phenoxazine (PO), phenothiazine (PS), and phenoselenazine (PSe)) with tuned charge distributions and electron transfer behaviors as cathode materials for ZOBs.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2025
Optimizing the crystalline orientation to achieve stable Zn (0002) plane growth is pursued for highly reversible zinc metal batteries (ZMBs). However, the lattice strain of Zn substrate hinders stable Zn plating/stripping and sustainable epitaxial growth of Zn (0002) texture. Herein, we present a low-strain strategy to mediate nucleated-Zn grains for stabilizing Zn electrodeposition/stripping process and guiding sustainable Zn growth along (0002) surfaces.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2025
Protons (H) with the smallest size and fastest redox kinetics are regarded as competitive charge carriers in the booming Zn-organic batteries (ZOBs). Developing new H-storage organic cathode materials with multiple ultralow-energy-barrier protophilic sites and super electron delocalization routes to propel superior ZOBs is crucial but still challenging. Here we design multiple protophilic redox-active reticular organic skeletons (ROSs) for activating better proton storage, triggered by intermolecular H-bonding and π-π stacking interactions between 2,6-diaminoanthraquinone and 2,4,6-triformylphloroglucinol nanofibrous polymer.
View Article and Find Full Text PDFNanomicro Lett
January 2025
A series of CoFeO materials derived from metal-organic framework were successfully constructed by the solvent-thermal method. The morphology of a typical sample CoFeO-1 was mostly in the form of a cubic rod-like structure with a size distribution of 3.2±0.
View Article and Find Full Text PDFSimultaneous monitoring of key metabolites like dopamine, ascorbic acid, and uric acid is essential for early disease diagnosis and evaluating treatment. Electrochemical techniques are increasingly used for precise, point-of-care testing (POCT) of these metabolites. Herein, a sample pretreatment method called effervescent solid-phase extraction (ESPE) was proposed for efficient enrichment of trace analytes for electrochemical detection.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2025
Multiple redox-active amphoteric organics with more n-p fused electron transfer is an ongoing pursuit for superior zinc-organic batteries (ZOBs). Here we report multi-heterocycle-site donor-acceptor conjugated amphoteric organic superstructures (AOSs) by integrating three-electron-accepting n-type triazine motifs and dual-electron-donating p-type piperazine units via H-bonding and π-π stacking. AOSs expose flower-shaped N-heteromacrocyclic electron delocalization topologies to promise full accessibility of built-in n-p redox-active motifs with an ultralow activation energy, thus liberating superior capacity (465 mAh g) for Zn||AOSs battery.
View Article and Find Full Text PDFOrganosulfides are considered promising cathode materials for zinc batteries due to their merits of high-density active sites and multielectron reactions, but often suffer from sluggish kinetics and limited electrochemical stability. Here organic iodide-catalyzed is reported and stabilized multielectron-redox bis(dimethylthiocarbamyl) sulfide (BS) cathode for superior zinc-organosulfide batteries. Activated by 2e I/I conversion in 1-methyl-3-propylimidazolium iodide (MPII)-modulated electrolyte, the electron-deficient structure of BS can stretch the electron cloud of two adjacent C═S bonds to form bipedal C─S bonds, affording high-kinetics and stable 2e Zn─S storage electrochemistry.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Surface modification is one of the effective strategies to control the morphology and electrocatalytic performance of noble metal/transition metal oxide matrix composite catalysts. In this work, we successfully introduced modification groups such as -NH, -COOH, and -SH on the surface of FeO using the hydrothermal method. It was found that when the modification group -COOH was introduced, the regular spherical morphology of FeO was still maintained in FeO-COOH, while FeO-COOH had a relatively smaller spherical particle size (≈155.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
Presented herein is a series of chain compounds based on pre-designed heterometallic aluminum-lanthanide (Al-Ln) AlLn molecular rings. Their photoluminescence quantum yield (PLQY) with Eu (30.41%) and Tb (41.
View Article and Find Full Text PDFIon-selective nanochannel membranes assembled from two-dimensional (2D) nanosheets hold immense promise for power conversion using salinity gradient. However, they face challenges stemming from insufficient surface charge density, which impairs both permselectivity and durability. Herein, we present a novel vacancy-engineered, oxygen-deficient NiCo layered double hydroxide (NiCoLDH)/cellulose nanofibers-wrapped carbon nanotubes (VOLDH/CNF-CNT) composite membrane.
View Article and Find Full Text PDFDendrite growth and parasitic reactions of a Zn metal anode in aqueous media hinder the development of up-and-coming Zn-ion batteries. Optimizing the crystal growth after Zn nucleation is promising to enable stable cyclic performance of the anode, but directly regulating specific crystal plane growth for homogenized Zn electrodeposition remains highly challenging. Herein, a perfluoropolymer (Nafion) is introduced into an aqueous electrolyte to activate a thermodynamically ultrastable Zn/electrolyte interface for long-term Zn-ion batteries.
View Article and Find Full Text PDFZinc-organic batteries (ZOBs) are receiving widespread attention as up-and-coming energy-storage systems due to their sustainability, operational safety and low cost. Charge carrier is one of the critical factors affecting the redox kinetics and electrochemical performances of ZOBs. Compared with conventional large-sized and sluggish Zn storage, non-metallic charge carriers with small hydrated size and light weight show accelerated interfacial dehydration and fast reaction kinetics, enabling superior electrochemical metrics for ZOBs.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2024
Understanding the self-stacking interactions in precursors can facilitate the preparation of high-performance carbon materials and promote the commercial application of zinc ion hybrid capacitors (ZIHCs). Here, a π-conjugated molecule mediated pyrolysis strategy is presented to prepare carbon materials. Taking intermolecular force simulation (reduced density gradient plots) as a guide, the relationship between the self-stacking interactions in π-conjugated molecules and the structural parameters of carbon materials can be extrapolated.
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