Dynamically Tunable All-Weather Daytime Cellulose Aerogel Radiative Supercooler for Energy-Saving Building.

A passive cooling strategy without any electricity input has shown a significant impact on overall energy consumption globally. However, designing tunable daytime radiative cooler to meet requirement of different weather conditions is still a big challenge, especially in hot, humid regions. Here, a novel type of tunable, thermally insulating and compressible cellulose nanocrystal (CNC) aerogel coolers is prepared via chemical cross-linking and unidirectional freeze casting process. Such aerogel coolers can achieve a subambient temperature drop of 9.2 °C under direct sunlight and promisingly reached the reduction of ∼7.4 °C even in hot, moist, and fickle extreme surroundings. The tunable cooling performance can be realized via controlling the compression ratio of shape-malleable aerogel coolers. Furthermore, energy consumption modeling of using such aerogel coolers in buildings in China shows 35.4% reduction of cooling energy. This work can pave the way toward designing high-performance, thermal-regulating materials for energy consumption savings.

Cellulose binary coatings with spherical envelope structure via structure rearrangement in ball milling for integrated radiative cooling-electricity generation.

Passive daytime radiative cooling is a zero-energy consumption cooling technology, which can dissipate heat to outer space via infrared radiation. Recently, coupling radiative cooling technology and thermoelectric devices to generate electricity has attracted much attention. However, existing radiative cooling integrated thermoelectric devices still suffer from low-temperature gradient and output voltage. Here, based on the Mie scattering and internal reflection enhancing principle, an impact-inducing geometry reconstruction approach was proposed to fabricate hierarchical nanostructured cellulosic coatings with good daytime cooling performance to achieve stable electricity generation function, which can be realized by using a scalable and facile wet ball milling technology. Guided by the theoretical simulations of the finite difference time domain method (FDTD), the cellulose and TiO2 nanoparticles can assemble into spherical envelope structured coatings drying by the shear, impact, and friction interaction in the ball milling process, dramatically enhancing the Mie scattering and internal reflection of coatings. The cellulosic coatings exhibit sunlight reflectivity of 0.962 and infrared emissivity of 0.94, resulting in a daytime radiative cooling efficiency of 5.9 °C under direct sunlight. Energy Plus stimulation demonstrated 35 % cooling energy and 468.9 kWh of cooling energy can be saved annually in China. Meanwhile, this cellulosic coating-based thermoelectric device can deliver a high voltage output of 150 mV under 1 Sun due to the strong bonding and high-temperature gradient formation (30 °C), which is higher than previous reports. This study will facilitate the development of sustainable power generation device for the goal of green future.

Cellulose-based evaporator with dual boost of water transportation and photothermal conversion for highly solar-driven evaporation.

Two-dimensional (2D) evaporation systems could significantly reduce the heat conduction loss compared with the photothermal conversion materials particles during the evaporation process. But the normal layer-by-layer self-assembly method of 2D evaporator would reduce the water transportation performance due to the highly compact channel structures. Herein, in our work, the 2D evaporator with cellulose nanofiber (CNF), Ti3C2Tx (MXene) and polydopamine modified lignin (PL) by layer-by-layer self-assembly and freeze-drying methods. The addition of PL also enhanced the light absorption and photothermal conversion performance of the evaporator due to the strong conjugation and π-π molecular interactions. After the combination process of layer-by-layer self-assembly and freeze-drying process, the as-prepared freeze-dried CNF/MXene/PL (f-CMPL) aerogel film exhibited highly interconnected porous structure with promoted hydrophilicity (enhanced water transportation performance). Benefiting these favorable properties, the f-CMPL aerogel film showed enhanced light absorption performance (surface temperature could be reached to 39 °C under 1 sun irradiation) and higher evaporation rate (1.60 kg m-2 h-1). This work opens new way to fabricate cellulose-based evaporator with highly evaporation performance for the solar steam generation and provides a new idea for improving the evaporation performance of 2D cellulose-based evaporator.

3D-cellulose acetate-derived hierarchical network with controllable nanopores for superior Li+ transference number, mechanical strength and dendrites hindrance.

The dendrites is deemed to be one of the most crucial problems for lithium-ion batteries because it hampers their safety and cycling performance severely. Herein, a cellulose acetate-based separator with uniformly distributed nanopores was engineered and successfully prepared through a simple one-step process. The controlled nanopores promoted uniform transmission of ions and the cellulose acetate backbone inhibited the transference of anions, and prevented large-scale accumulation of lithium ions, thereby restricting the nucleation and growth of dendrites. The 3D-networked separator exhibited capacity retention of 78.6% after 900 cycles at 1C, with the breaking elongation and the strength increased by 620% and 28.4%, respectively, which originated from the porosity controlling of the nanofiber inter-bridging. The nanopore-assembled structure of 3D-hierarchy with MOFs provided the channels for the lithium ions transference through the separator and hence tackled the major challenge of mechanical vulnerability and electrochemical instability, which have never been reported before. Therefore, the developed strategy may offer a powerful and effective alternative for conventional approach of occurring dendrites post-treatments for higher ionic conductivity.

Strong biodegradable cellulose materials with improved crystallinity via hydrogen bonding tailoring strategy for UV blocking and antioxidant activity.

It has been a huge challenge to obtain simultaneously excellent mechanical strength and desirable multifunctionality from the cellulose nanocrystals (CNC) based food packing materials. In this work, we demonstrated a hydrogen bonding tailoring strategy that can produce CNC/lignin films with UV blocking and antioxidant activity, while bypassing the loss of mechanical strength. Using a hyperbranched polyester, lignin was first functionalized to increase the amount of hydroxyl groups, thereby increasing the intermolecular interactions. By assembling the polyester modified lignin (H-lignin) into CNC matrix, the hydrogen bonding crosslinks between the H-lignin and CNC chains were successfully promoted, resulting in the CNC composites with the significantly improved mechanical strength, UV blocking and antioxidant activity. The phenolic structure and the hydrogen donation of H-lignin also endowed the resulting CNC composites with excellent UV blocking and antioxidant activity. The experimental results indicated that the H-lignin could bring about 34% and 63% increase in tensile strength and Young's modulus, respectively, higher than the reported ones. The CNC-based composites showed better thermal stability and improved crystallinity property. The H-lignin provides a new insight into the multifunctional exploration of CNC-based composite. This work opens a new avenue for the next generation's biodegradable food packing materials from cellulose-sourced composites.

Ultralight Programmable Bioinspired Aerogels with an Integrated Multifunctional Surface for Self-Cleaning, Oil Absorption, and Thermal Insulation via Coassembly.

Creating a configurable and controllable surface for structure-integrated multifunctionality of ultralight aerogels is of significance but remains a huge challenge because of the critical limitations of mechanical vulnerability and structural processability. Herein, inspired by Salvinia minima, the facile and one-step coassembly approach is developed to allow the structured aerogels to spontaneously replicate Salvinia-like textures for function-adaptable surfaces morphologically. The in situ superimposed construction of bioinspired topography and intrinsic topology is for the first time performed for programmable binary architectures with multifunctionality without engendering structural vulnerability and functional disruption. By introducing the binding groups for hydrophobicity tailoring, functionalized nanocellulose (f-NC) is prepared via mechanochemistry as a structural, functional, and topographical modifier for a multitasking role. The self-generated bioinspired surface with f-NC greatly maintains the structural unity and mechanical robustness, which enable self-adaptability and self-supporting of surface configurations. With fine-tuning of nucleation-driving, the binary microstructures can be controllably diversified for structure-adaptable multifunctionalities. The resulting ultralight S. minima-inspired aerogels (e.g., 0.054 g cm-3) presented outstanding temperature-endured elasticity (e.g., 90.7% high-temperature compress-recovery after multiple cycles), durable superhydrophobicity, anti-icing properties, oil absorbency efficiency (e.g., 60.2 g g-1), and thermal insulating (e.g., 0.075 W mK-1), which are superior to these reported on the overall performance. This coassembly strategy offers the opportunities for the design of ultralight materials with topography- and function-tailorable features to meet the increasing demands in many fields such as smart surfaces and self-cleaning coatings.