Sustainably transforming biomass into advanced carbon materials for solid-state supercapacitors: a review
Biomass-derived carbon materials (BDCMs) are widely considered as promising and practical candidates for electrode materials of solid-state supercapacitors (SSCs), due to their low cost, good chemical and mechanical stabilities, excellent electrical conductivity, and high deployment feasibility. Numerous investigations have recently been conducted for sustainably transforming biomass into electrode materials with high electrochemical performance in SSCs, even guided by data-driven approaches. Therefore, this review addresses conventional and emerging synthesis routes for BDCM-based electrode materials and discusses recent advances in energy storage mechanisms and electrochemical performance enhancement of BDCMs for SSCs, improving electrode preparation and performance optimization of BDCMs in a practical and efficient manner. As two of the most powerful tools for novel material discovery and design, machine learning (ML) and 3D printing technologies are introduced to provide closed-loop guidelines for accurately and efficiently producing BDCMs with excellent electrochemical performance; main challenges for successfully applying ML and 3D printing methodologies are also addressed, providing critical guidelines for potential innovation and future development of BDCM-based SSCs. In this review, from life-cycle perspective, environmental benefits are assessed for BDCM-based SSCs, being highlighted as a promising and practical alternative to solidify energy security and achieve sustainable biomass management. The concluding remarks and future prospects are finally discussed to provide valuable insights for academic researchers and governmental policymakers. With concerted efforts, sustainably transforming biomass into high-performance electrode materials for SSCs is beneficial to achieving UN Sustainable Development Goals 7, 11-13.
A stable HOF-embedded alginate hydrogel membrane for selective adsorption of cationic dyes
Targeted at organic dye pollutants, a stable HOF was combined with an alginate (SA) hydrogel to enhance the affinity for cationic dyes. The as-obtained HOF@SA membrane (weight ratio: 1/1) shows a high adsorption capacity (729.21 mg g), adsorption selectivity and good recycling performance towards methylene blue.
Ceria-based supported metal catalysts for the low-temperature water-gas shift reaction
Water-gas shift (WGS) reaction is a crucial step for the industrial production of hydrogen or upgrading the hydrogen generated from fossil or biomass sources by removing the residual CO. However, current industrial catalysts for this process, comprising Cu/ZnO and FeO-CrO, suffer from safety or environmental issues. In the past decades, ceria-based materials have attracted wide attention as WGS catalysts due to their abundant oxygen vacancies and tunable metal-support interaction. Strategies through engineering the shape or crystal facet, size of both metal and ceria, interfacial-structure, , to alter the performances of ceria-based catalysts have been extensively studied. Additionally, the developments in the techniques and DFT calculations are favorable for deepening the understanding of the reaction mechanism and structure-function relationship at the molecular level, comprising active sites, reaction path/intermediates, and inducements for deactivation. This article critically reviews the literature on ceria-based catalysts toward the WGS reaction, covering the fundamental insight of the reaction path and development in precisely designing catalysts.
Efficient organic solar cells with benzo[]phenazine-core acceptors: insights into the effects of halogenation
A series of new small-molecule acceptors-NA9, NA10, and NA11-based on benzo[]phenazine are synthesized. The chlorinated NA10 and brominated NA11 exhibit improved molecular packing and enhanced charge transport, resulting in higher power conversion efficiencies (PCEs) of 15.65% and 16.64%, respectively, compared to 11.66% for the non-halogenated NA9. These results underscore the great potential of peripheral halogenation particularly bromination, in achieving high-performance OSCs.
Electroreduction of CO and nitrate for urea synthesis on a low-coordinated copper catalyst
Electroreduction of CO and NO to urea (ECNU) offers a fascinating route for migrating NO pollutants and synthesizing valuable urea. Herein, low-coordinated copper (L-Cu) is developed as an effective ECNU catalyst, delivering the highest urea yield rate of 30.96 mmol h g and urea-faradaic efficiency of 50.42% in a flow cell. Theoretical calculations reveal that Cu sites and low-coordinated Cu (Cu) sites on L-Cu can synergistically promote C-N coupling and inhibit the competing side reactions, leading to a high CO/NO-to-urea efficiency.
Bright colloidal gallium-doped CuInS quantum dots for luminescent solar concentrators
We have developed an efficient strategy to improve the brightness and stability of CuInS quantum dots Ga doping combined with the overgrowth of a ZnS shell. The incorporation of Ga into crystal lattices greatly suppresses the diffusion of Cu and reduces the formation of Cu-related defects, leading to a photoluminescence quantum yield as high as 92%. These nanocrystals can be integrated into luminescent solar concentrators and the devices exhibit a power conversion efficiency reaching 3.87%.
Rational design of water splitting electrocatalysts through computational insights
Electrocatalytic water splitting is vital for the sustainable production of green hydrogen. Electrocatalysts, including those for the hydrogen evolution reaction at the cathode and the oxygen evolution reaction at the anode, are crucial in determining the overall performance of water splitting. Traditional methods for electrocatalyst development often rely on trial-and-error, which can be time-consuming and inefficient. Recent advancements in computational techniques provide more systematic and predictive strategies for catalyst design. This review article explores the role of computational insights in the development of water-splitting electrocatalysts. We start by giving an introduction of electrocatalytic water splitting mechanisms. Then, fundamental theories such as the Sabatier principle and scaling relationships are reviewed, which provide a theoretical basis for catalytic activity. We also discuss thermodynamic, electronic, and geometric descriptors used to guide catalyst design and provide an in-depth discussion of their applications and limitations. Advanced computational approaches, including high-throughput screening, machine learning, solvation models and molecular dynamics, are also highlighted for their ability to accelerate catalyst discovery and simulate realistic reaction conditions. Finally, we propose future research directions aimed at searching universal descriptors, expanding data sets, and integrating developing interpretable models with catalyst design.
Synthesis of phosphate stabilised iodanes and their application in intramolecular aryl migrations
A diverse set of hydroxy-benzo[]iodadioxaphosphinine oxides and derived diaryl iodonium salts are prepared and two examples are characterized by X-ray crystallography, featuring an out-of-plane geometry of the hypervalent bond for both compound classes. Treatment of the phosphate-stabilized diaryliodonium salts with Ca(OH) results in an efficient base-induced intramolecular aryl migration under aqueous conditions, yielding iodo-substituted diaryl ethers with yields up to 94%. Our findings highlight the synthetic potential of this previously underexplored compound class in organic transformations.
Living plant-assisted recycling of nano gold into Murray porous carbon electrode materials
Based on the enrichment potential of living plants for nanoparticles, this paper develops a new strategy to utilize Murray's law in plants to remove various shapes of gold nanoparticles and, , convert them into Murray porous carbon. The inherent Murray network serves as an optimized hierarchical design and ensures the mechanical stability of the material, and Murray's law is employed to achieve uniform dispersion of nanoparticles , facilitating the preparation of metal nanoparticle-supported carbon materials.
Scaling up electrochemical CO reduction: enhancing the performance of metalloporphyrin complexes in zero-gap electrolyzers
Metalloporphyrins are widely studied in the field of electrochemical CO reduction (COR), with the main focus on homogenous catalysis. Herein, six metalloporphyrins (M = Fe, Co, Ni, Cu, Zn, Ag) were incorporated in gas diffusion electrodes and used in zero-gap electrolyzers to reach varying FEs for CO of <1% (Fe,Ni), 11% (Cu), 37% (Zn), 75% (Co) and nearly 100% (Ag) at a current density of 50 mA cm.
Synergistic effect of hydrogen-bond interaction and interface regulation for stable aqueous sodium-ion batteries
The narrow voltage window of aqueous electrolytes hinders the energy density of aqueous sodium-ion batteries (SIBs). Herein, a thermally and electrochemically stable hybrid electrolyte is developed with NaCFSO, 1,3-dioxolane (DOL), urea and HO. The intermolecular interactions between DOL, urea and HO regulate the hydrogen-bond network. Furthermore, the formation of an interfacial layer between the electrode and the electrolyte enables stable cycling of the manganese-based Prussian blue analogs (NaFeMnPBAs). As a result, a NaFeMnPBAs‖NaTi(PO) full cell is constructed and it exhibits high energy density and superior stability in the hybrid electrolyte.
One-step selective synthesis of doubly and triply fused chiral boroloborole derivatives
Chiral 3,6-dihydroborolo[3,2-]boroles are obtained in one diastereoselective step from the reactions of -(dihaloboryl)arenes with stannole derivatives a complex rearrangement of 1-borolyl-2-(dihaloboryl)arene intermediates.
A Janus structured TaO/TaN heterojunction as an efficient oxygen reduction electrocatalyst for HO production
A Janus TaO/TaN heterojunction hybrid with graphene exhibited excellent activity, selectivity and durability for the 2e oxygen reduction reaction (ORR), compared to TaON@Gr, due to the optimized O adsorption and favored *OOH binding in the Janus TaO/TaN heterojunction. This provides a new approach for the structural design of high-performance 2e ORR catalysts.
Compartmentalised single-chain nanoparticles and their function
Single-chain nanoparticles (SCNPs) are generated by intramolecular collapse and crosslinking of single polymer chains, thus conceptually resembling the structures of folded proteins. Their chemical flexibility and ability to form compartmentalised nanostructures sized ∼1 nm make them perfect candidates for numerous applications, such as in catalysis and drug delivery. In this review we discuss principles for the design, synthesis and analysis of SCNPs, with a focus on their compartmentalised structures, highlighting our own previous work. As such compartments offer the potential to generate a specific nanoenvironment for the covalent and non-covalent encapsulation of catalysts or drugs, they represent a novel, exciting, and expanding research area. Starting from the architectural and chemical design of the starting copolymers by controlling their amphiphilic profile, the embedding of blocks-, or secondary-structure-mimetic arrangements, we discuss design principles to form internal compartments inside the SCNPs. While the generation of compartments inside SCNPs is straightforward, their analysis is still challenging and often demands special techniques. We finally discuss applications of SCNPs, also linked to the compartment formation, predicting a bright future for these special nanoobjects.
Lipidic biomass as a renewable chemical building block for polymeric materials
Polymers are intrinsically connected to modern society and are found and used in a variety of technologies. Although polymers are valuable, concerns about synthetic polymers derived from non-renewable sources have emerged. Therefore, there is a need to develop new polymeric materials from renewable sources, especially those that are cost-effective, non-toxic, widely available, not derived from depleting sources and are designed to be biodegradable after disposal. In this regard, a perfect class of renewable resources are the lipids (not soluble in water), among which, we can find useful compounds such as triacylglycerols/triglycerides (vegetable oil), terpenes/terpenoids (essential oils), and abietic acid (rosin resin). These are liable to modification to new monomers that can be used in adhesives, 3D-printing, self-healing and so on. However, these materials still suffer from some limitations when compared to non-renewable polymers. Therefore, in this feature article, we will present a description/review of these renewable sources together with related polymeric materials and their mechanical/chemical/physical properties and applications.
Super-resolution imaging with a cucurbituril-encapsulated fluorophore
Red-emitting oxazine fluorophores are shown to bind to cucurbit[7]uril (CB[7]) with high affinity. Their fluorescence quantum yield and lifetime are thereby enhanced owing to shielding of the dyes from water. Using CB[7] as an imaging additive leads to a larger number of photons detected per molecule in super-resolution experiments with the dye ATTO655.
Nickel-catalyzed silylation of aryl thianthrenium salts with silylzinc pivalates
A nickel-catalyzed C-S silylation of aryl thianthrenium salts with salt-stabilized silylzinc pivalates is disclosed, thus allowing us to rapidly incorporate silyl motifs into aromatics in a site- and chemoselective fashion. This method is distinguished by its ample scope and facile derivatizations of the aryl silanes for increasing functional molecular complexity. Moreover, modular installation of silyl groups into pharmaceutically active molecules provides a new platform for the synthesis of sila-drugs.
Recent advances in nanomaterial-enabled chemiresistive hydrogen sensors
With the growing adoption of hydrogen energy and the rapid advancement of Internet of Things (IoT) technologies, there is an increasing demand for high-performance hydrogen gas (H) sensors. Among various sensor types, chemiresistive H sensors have emerged as particularly promising due to their excellent sensitivity, fast response times, cost-effectiveness, and portability. This review comprehensively examines the recent progress in chemiresistive H sensors, focusing on developments over the past five years in nanostructured materials such as metals, metal oxide semiconductors, and emerging alternatives. This review delves into the underlying sensing mechanisms, highlighting the enhancement strategies that have been employed to improve sensing performance. Finally, current challenges are identified, and future research directions are proposed to address the limitations of existing chemiresistive H sensor technologies. This work provides a critical synthesis of the most recent advancements, offering valuable insights into both current challenges and future directions. Its emphasis on innovative material designs and sensing strategies will significantly contribute to the ongoing development of next-generation H sensors, fostering safer and more efficient energy applications.
Visible-light-induced hydroalkylation of alkenes with aromatic β-ketoesters
A mild and environmentally friendly photocatalytic method for C-C bond formation between 1,3-dicarbonyls and styrene derivatives has been developed in a green solvent - ethanol. A series of α-functionalized β-diketones were obtained in moderate to good yields. Based on the results of control experimental and theoretical calculations, the photocatalytic transformation might be accomplished by generating reactive radicals a single electron transfer process. Moreover, the matching of reduced-state photocatalyst with the radical intermediate is considered to be critical for this conversion.
Acid-induced fluorescence enhancement of piperazinylphenyl-substituted nanographene
A dibenzo[,]ovalene (DBOV) derivative bay-substituted with two piperazinylphenyl (PZP) groups (DBOV-PZP) was synthesized. Comprehensive investigations of its photophysical properties revealed acid-induced fluorescence enhancement through the protonation of PZP units, leading to the suppression of the photoinduced electron transfer. These results pave the way towards "turn-on" type nanographenes for biosensing and optical imaging.
Interstitial and substitutional doping of Mn in 2D PEAPbBr and BAPbBr perovskites
Mn doping imposes intriguing optoelectronic properties on lead-halide perovskites; however, its impact on their crystal structure remains unclear. This study investigates the consequences of interstitial and substitutional Mn doping on the lattice-strain and interplanar spacings of 2D perovskites and correlates the structural changes to their optical properties.