Electronegative Nanochannels Accelerating Lithium‐Ion Transport for Enabling Highly Stable and High‐Rate Lithium Metal Anodes

Lithium (Li) metal is regarded as the most desirable anode candidates for high-energy-density batteries by virtue of its lowest redox potential and ultrahigh theoretical specific capacity. However, uncontrollable Li dendritic growth, infinite volume variation and unstable solid electrolyte interface (SEI) ineluctably plague its commercialization process. Herein, the three-dimensional (3D) nanofiber functional layers with synergistic soft-rigid feature, consisting of tin oxide (SnO2)-anchored polyvinylidene fluoride (PVDF) nanofibers, are directly electrospun on copper current collector. This strategy can effectively regulate uniform Li deposition and strengthen SEI stability through the dual effect of physical accommodation and chemical ionic intervention. On the one hand, the nanofiber interlayers with excellent electrolyte affinity and well-distributed Li+ transport pathways can promote uniform Li+ flux distribution and large-size Li deposition. On the other hand, the rigid SnO2 contributes to reducing Li nucleation overpotential and stabilizing SEI layer assisted by its spontaneous reaction with Li. As a result, the smooth and dense Li deposition is achieved by such soft-rigid nanofiber interlayers, thereby extending the cycling life and improving the safety application of Li metal batteries. This work offers a new route for efficient protection of Li metal anodes and brings a new inspiration for developing high-energy-density Li metal batteries. 

Realizing dendrite-free lithium deposition with three-dimensional soft-rigid nanofiber interlayers

At present, the dominating electron transport material (ETL) and hole transport material (HTL) used in the state-of-the-art perovskite solar cells (PSCs) are tin oxide and 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9′-spirobifluorene (Spiro-OMeTAD). However, the surface hydroxyl groups of the SnO2 layer and the Li+ ions within the Spiro-OMeTAD HTL layer generally cause surface charge recombination and Li+ migration, significantly reducing the devices' performance and stability. Here, a molecule bridging layer of 3,5-bis(fluorosulfonyl)benzoic acid (FBA) is introduced onto the SnO2 surface, which provides appropriate surface energy, reduces interfacial traps, forms a better energy level alignment, and, most importantly, anchors (immobilizes) Li+ ions in the ETL, and consequently improves the device power conversion efficiency (PCE) up to 24.26% without hysteresis. Moreover, the device with the FBA passivation layer shows excellent moisture and operational stability, maintaining over 80% of the initial PCE after 1000 h under both aging conditions. The current work provides a comprehensive understanding of the influence of the extrinsic Li+ ion migration within the cell on the device's performance and stability, which helps design and fabricate high-performance and hysteresis-free PSCs. 

A Multifunctional Molecular Bridging Layer for High Efficiency, Hysteresis‐Free, and Stable Perovskite Solar Cells

The various forms of cellulose-based materials possess high mechanical and thermal stabilities, as well as three-dimensional open network structures with high aspect ratios capable of incorporating other materials to produce composites for a wide range of applications. Being the most prevalent natural biopolymer on the Earth, cellulose has been used as a renewable replacement for many plastic and metal substrates, in order to diminish pollutant residues in the environment. As a result, the design and development of green technological applications of cellulose and its derivatives has become a key principle of ecological sustainability. Recently, cellulose-based mesoporous structures, flexible thin films, fibers, and three-dimensional networks have been developed for use as substrates in which conductive materials can be loaded for a wide range of energy conversion and energy conservation applications. The present article provides an overview of the recent advancements in the preparation of cellulose-based composites synthesized by combining metal/semiconductor nanoparticles, organic polymers, and metal-organic frameworks with cellulose. To begin, a brief review of cellulosic materials is given, with emphasis on their properties and processing methods. Further sections focus on the integration of cellulose-based flexible substrates or three-dimensional structures into energy conversion devices, such as photovoltaic solar cells, triboelectric generators, piezoelectric generators, thermoelectric generators, as well as sensors. The review also highlights the uses of cellulose-based composites in the separators, electrolytes, binders, and electrodes of energy conservation devices such as lithium-ion batteries. Moreover, the use of cellulose-based electrodes in water splitting for hydrogen generation is discussed. In the final section, we propose the underlying challenges and outlook for the field of cellulose-based composite materials.

/pdf/advances-in-cellulose-based-composites-for-energy-1htos3h1.pdf

Advances in Cellulose-Based Composites for Energy Applications

Cellulose filter papers derived separator featuring effective ion transferring channels for sodium-ion batteries

We design highly-active porous Co-doped carbon nitride (CN) rod by a facile thermal condensation of melem supramolecular assembly incorporated with Co species. The highly thermal-stable H-bonded melem supramolecule enables less and slow sublimation during the thermal condensation process, ensuring good microstructural integrality of the CN skeleton for the migration of photogenerated carriers. And the Co doping can further modulate the electronic, optical, and catalytic properties of the catalyst. The best-performing Co-doped CN catalyst demonstrates desirable performance toward the photocatalytic degradation of tetracycline hydrochloride (10.3 times higher than that of bulk CN) and good cycling stability maintaining 80.0 % after 5 reuses. 

Design of Co-doped carbon nitride based on melem supramolecular assembly with enhanced photocatalytic activity toward tetracycline hydrochloride degradation

The uncontrollable growth of lithium (Li) dendrites impedes the development of practical applications for the long-awaited lithium metal batteries. In this work, a strategy is proposed to protect the Li anode with a composite separator of in situ formed SnO2 and hydroxypropyl methyl cellulose (HPMC) on the polyethylene (PE) substrate. Based on the use of SnO2/HPMC@PE separator, the Li||Li cell has an ultralong cycle life of more than 2000 h and ultralow-voltage hysteresis of 11.1 mV, whereas the cell with PE separator only has the cycle life of 800 h and the voltage hysteresis of up to 222.9 mV. Moreover, Li||LiNi0.6Co0.2Mn0.2O2 (NCM622) has an initial discharge capacity of 142.3 mAh g–1 and a capacity retention of 77.9% after 250 cycles at 1 C, which are higher than those of PE (140.6 mAh g–1 with retention of 59.5%). All of the enhanced performance can be ascribed to a regulable SEI film that can be formed on the Li foil in direct contact with the SnO2 layer, which decreases the Li nucleation overpotential and facilitates ultimately uniform Li deposition. This work demonstrates the feasibility of using a modified separator to achieve stable Li metal batteries. 

Uniform Lithium Deposition Achieved by SnO2/Hydroxypropyl Methyl Cellulose Composite Separator toward Ultrastable Lithium Metal Batteries

Tailoring hydrogen-halogen bond networks in heptazine architectures for controlled fabrication of a high-performance C-doped porous carbon nitride photocatalyst.

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Design of Co-doped carbon nitride based on melem supramolecular assembly with enhanced photocatalytic activity toward tetracycline hydrochloride degradation

Uniform Lithium Deposition Achieved by SnO2/Hydroxypropyl Methyl Cellulose Composite Separator toward Ultrastable Lithium Metal Batteries

Tailoring hydrogen-halogen bond networks in heptazine architectures for controlled fabrication of a high-performance C-doped porous carbon nitride photocatalyst.