Interface Engineering on Cellulose-Based Flexible Electrode Enables High Mass Loading Wearable Supercapacitor with Ultrahigh Capacitance and Energy Density.

For practical energy storage devices, a bottleneck is to retain decent integrated performances while increasing the mass loading of active materials to the commercial level, which highlights an urgent need for novel electrode structure design strategies. Here, an active nitrogen-doped carbon interface with "high conductivity, high porosity, and high electrolyte affinity" on a flexible cellulose electrode surface is engineered to accommodate 1D active materials. The high conductivity of interface favors fast electron transport, while its high porosity and high electrolyte affinity properties benefit ion migration. As a result, the flexible anode accommodated by carbon nanotubes achieves an ultrahigh capacitance of 9501 mF cm-2 (315.6 F g-1 ) at a high mass loading of 30.1 mg cm-2 , and the flexible cathode accommodated by polypyrrole nanotubes realizes a remarkably high capacitance of 6212 mF cm-2 (248 F g-1 , 25 mg cm-2 ). The assembled flexible quasi-solid-state asymmetric supercapacitor delivers a maximum energy density of 1.42 mWh cm-2 (2.2 V, 2105 mF cm-2 ), representing the highest value among all reported flexible supercapacitors. This versatile design concept provides a new way to prepare high performance flexible energy storage devices.

Green Fabrication of Highly Conductive Paper Electrodes via Interface Engineering with Aminocellulose.

Herein, a novel, facile, and versatile approach to fabricate highly flexible and conductive paper is proposed by electroless deposition (ELD) with the assistance of aminocellulose as the interface layer. The obtained Cu nanoparticles (NPs)-coated cellulose paper is highly conductive with a significant low resistance of 0.38 Ω sq-1 after only 10 min of ELD treatment. This conductive cellulose paper shows excellent stability when it suffers from bending, folding, and tape adhesion cycles. With the same method, the Cu NPs can also be successfully deposited on the polypropylene (PP)-filled hybrid paper. The conductive paper exhibits very smooth and hydrophobic surface with high reflection, which can be used for special electronic devices. In a word, the fabrication of aminocellulose interface permits a controlled ELD of metal nanoparticles on paper substrate, and this mild and low-cost method opens up new opportunities for large-scale production of flexible and wearable electronics.

Enhancing Cross-Linking Network for Superior Wet Strength of Paper by Sustainable Hyperbranched Polyimines.

The paper industry has long been a crucial part of our lives, providing printing materials, tissue paper, and packaging products. However, the low wet strength of commercially available paper limits its application in packaging, particularly when it comes into contact with liquids. To address this issue, researchers have explored various strategies, including the use of wet strength agents. The most widely used agent, polyamide-epichlorohydrin resin (PAE), has limitations, such as poor dimensional stability and limited recyclability. Additionally, PAE can release harmful chlorinated organics. To overcome these challenges, we report a novel approach using a hyperbranched wet strength agent (referred to as "OA-PI") based on the cross-linking of oxidized amylopectin from waxy corn and polyamines through the Schiff base reaction. The hyperbranched structure of OA-PI provides multiple binding sites, enhancing the cross-linking strength of cellulosic paper under wet conditions. The paper treated with OA-PI exhibited exceptional wet strength, significantly higher than that of PAE-treated paper and paper with traditional starch-based additives. Moreover, the biomass-based OA-PI showed improved recyclability and reduced harm from chlorinated organic compounds. This study not only enhances the wet strength of paper but also opens sustainable avenues for the design of functional adhesives.

Antimicrobial cellulose paper tuned with chitosan fibers for high-flux oil/water separation.

Separating films with both high efficiency and large flux are desperately needed to meet the rising demand for the treatment of oily wastewater, while traditional oil/water separation papers with high separation efficiency usually suffered from low flux due to the unsuitable size of filtration pores. Herein, we report a bio-based porous, superhydrophobic, and antimicrobial hybrid cellulose paper with tunable porous structures for high flux oil/water separation. The size of pores in the hybrid paper can be tuned by both physical supports provided by the chitosan fibers and the chemical shielding supplied by the hydrophobic modification. The hybrid paper with increased porosity (20.73 µm; 35.15 %) and excellent antibacterial properties can efficiently separate a wide range of oil/water mixtures, solely by gravity, with outstanding flux (maximum of 23,692.69 L m-2 h-1), tiny oil interception, and high efficiency of over 99 %. This work provides new sights in the development of durable and low-cost functional papers for rapid and efficient oil/water separation.

Rapid transesterification of cellulose in a novel DBU-derived ionic liquid: Efficient synthesis of highly substituted cellulose acetate.

Cellulose acetate (CA) is one of the most important cellulose plastics that has demonstrated extensive applications in many areas. In search of a more sustainable and efficient way to prepare CA, we synthesized a novel ionic liquid, [DBUC8]Cl, based on the commonly used catalyst DBU (1,8-diazabicyclo[5.4.0]undecyquin-7-ene) in a simple manner. [DBUC8]Cl can dissolve cellulose more efficiently than the same type of imidazolyl ionic liquid, owing to the stronger alkalinity of DBU. It is noteworthy that highly substituted CA (DS = 2.82) was successfully synthesized via transesterification with alkenyl ester under mild conditions (80 °C, 40 min) without the addition of a catalyst in this solvent, which is superior to most of the reported work. Furthermore, we confirmed that the synthesized CA had good thermoplasticity, and a transparent cellulose acetate film (CAF) was obtained by hot pressing with a small amount of glycerol. Therefore, we propose a new DBU-derived ionic liquid, which may serve as a versatile platform system for producing cellulose-derived bioplastics more sustainably and efficiently.

Trace Amounts of Triple-Functional Additives Enable Reversible Aqueous Zinc-Ion Batteries from a Comprehensive Perspective.

Although their cost-effectiveness and intrinsic safety, aqueous zinc-ion batteries suffer from notorious side reactions including hydrogen evolution reaction, Zn corrosion and passivation, and Zn dendrite formation on the anode. Despite numerous strategies to alleviate these side reactions have been demonstrated, they can only provide limited performance improvement from a single aspect. Herein, a triple-functional additive with trace amounts, ammonium hydroxide, was demonstrated to comprehensively protect zinc anodes. The results show that the shift of electrolyte pH from 4.1 to 5.2 lowers the HER potential and encourages the in situ formation of a uniform ZHS-based solid electrolyte interphase on Zn anodes. Moreover, cationic NH4+ can preferentially adsorb on the Zn anode surface to shield the "tip effect" and homogenize the electric field. Benefitting from this comprehensive protection, dendrite-free Zn deposition and highly reversible Zn plating/stripping behaviors were realized. Besides, improved electrochemical performances can also be achieved in Zn//MnO2 full cells by taking the advantages of this triple-functional additive. This work provides a new strategy for stabilizing Zn anodes from a comprehensive perspective.

A highly conductive, pliable and foldable Cu/cellulose paper electrode enabled by controlled deposition of copper nanoparticles.

There is great interest in extending cellulosic platforms to applications in flexible, lightweight, low-cost and sustainable electronics. The critical need is the development of methods to confer electronic properties to these materials platforms (i.e., paper and fabrics). Here we report a highly conductive, pliable and foldable Cu/cellulose paper electrode enabled by a simple low-cost and scalable wet-processing method to coat a Cu nanoparticle (NP) layer on common cellulose paper, where polydopamine adhesion and electroless deposition were used to yield highly conductive paper with a sheet resistance as low as 0.01 Ω sq-1. This Cu/cellulose paper has excellent stability because of the strong adhesion between Cu NPs and cellulose, and because the methods are sufficiently mild to prevent damage to the paper substrate. This fabrication method results in the controlled deposition of Cu NPs and yields Cu/cellulose paper with highly hydrophobic and self-cleaning properties, high photothermal conversion efficiency, and excellent electromagnetic interface (EMI) shielding effectiveness. This high-performance Cu/cellulose paper could have promising application potential for a range of emerging applications in flexible electronics and packaging.

MnO2@Corncob Carbon Composite Electrode and All-Solid-State Supercapacitor with Improved Electrochemical Performance.

Two corncob-derived carbon electrode materials mainly composed of micropores (activated carbon, AC) and mesopores/macropores (corncob carbon, CC) were prepared and studied after the anodic electrodeposition of MnO2. The capacity of the MnO2/activated carbon composite (MnO2@AC) electrode did not noticeably increase after MnO2 electrodeposition, while that of the MnO2/corncob carbon composite (MnO2@CC) electrode increased up to 9 times reaching 4475 mF cm-2. An asymmetric all-solid-state supercapacitor (ASC) was fabricated using AC as the anode, MnO2@CC as the cathode, and polyvinyl alcohol (PVA)/LiCl gel as the electrolyte. An ultrahigh specific capacitance of 3455.6 mF cm-2 at 1 mA cm-2, a maximum energy density of 1.56 mW h cm-2, and a long lifetime of 10,000 cycles can be achieved. This work provides insights in understanding the function of MnO2 in biomass-derived electrode materials, and a green path to prepare an ASC from waste biomass with excellent electrochemical performance.