Zheng Jia

Tin Anode for Sodium-Ion Batteries Using Natural Wood Fiber as a Mechanical Buffer and Electrolyte Reservoir

Sodium (Na)-ion batteries offer an attractive option for low cost grid scale storage due to the abundance of Na. Tin (Sn) is touted as a high capacity anode for Na-ion batteries with a high theoretical capacity of 847 mAh/g, but it has several limitations such as large volume expansion with cycling, slow kinetics, and unstable solid electrolyte interphase (SEI) formation. In this article, we demonstrate that an anode consisting of a Sn thin film deposited on a hierarchical wood fiber substrate simultaneously addresses all the challenges associated with Sn anodes. The soft nature of wood fibers effectively releases the mechanical stresses associated with the sodiation process, and the mesoporous structure functions as an electrolyte reservoir that allows for ion transport through the outer and inner surface of the fiber. These properties are confirmed experimentally and computationally. A stable cycling performance of 400 cycles with an initial capacity of 339 mAh/g is demonstrated; a significant improvement over other reported Sn nanostructures. The soft and mesoporous wood fiber substrate can be utilized as a new platform for low cost Na-ion batteries.

Atomic-Layer-Deposition Oxide Nanoglue for Sodium Ion Batteries

Atomic-layer-deposition (ALD) coatings have been increasingly used to improve battery performance. However, the electrochemical and mechanistic roles remain largely unclear, especially for ALD coatings on electrodes that undergo significant volume changes (up to 100%) during charging/discharging. Here we investigate an anode consisting of tin nanoparticles (SnNPs) with an ALD-Al2O3 coating. For the first time, in situ transmission electron microscopy unveiled the dynamic mechanical protection of the ALD-Al2O3 coating by coherently deforming with the SnNPs under the huge volume changes during charging/discharging. Battery tests in coin-cells further showed the ALD-Al2O3 coating remarkably boosts the cycling performance of the Sn anodes, comparing with those made of bare SnNPs. Chemomechanical simulations clearly revealed that a bare SnNP debonds and falls off the underlying substrate upon charging, and by contrast the ALD-Al2O3 coating, like ion-conductive nanoglue, robustly anchors the SnNP anode to the substrate during charging/discharging, a key to improving battery cycle performance.

Lithium-Assisted Electrochemical Welding in Silicon Nanowire Battery Electrodes

From in situ transmission electron microscopy (TEM) observations, we present direct evidence of lithium-assisted welding between physically contacted silicon nanowires (SiNWs) induced by electrochemical lithiation and delithiation. This electrochemical weld between two SiNWs demonstrates facile transport of lithium ions and electrons across the interface. From our in situ observations, we estimate the shear strength of the welded region after delithiation to be approximately 200 MPa, indicating that a strong bond is formed at the junction of two SiNWs. This welding phenomenon could help address the issue of capacity fade in nanostructured silicon battery electrodes, which is typically caused by fracture and detachment of active materials from the current collector. The process could provide for more robust battery performance either through self-healing of fractured components that remain in contact or through the formation of a multiconnected network architecture.

Anomalous scaling law of strength and toughness of cellulose nanopaper

Significance A long-standing challenge in material design is to overcome the conflict between strength and toughness, because they are generally mutually exclusive. To address this challenge, we rationally design cellulose-based nanopaper and investigate the dependence of their mechanical properties on constituent cellulose fiber size. Surprisingly, we find that both the strength and toughness of the nanopaper increase simultaneously (40 and 130 times, respectively) as the average diameter of constituent cellulose fibers decreases from 27 μm to 11 nm, suggesting the promising potential toward an anomalous but highly desirable scaling law: the smaller, the stronger and the tougher. There are abundant opportunities to use the fundamental bottom-up strategy to design a novel class of functional materials that are both strong and tough. The quest for both strength and toughness is perpetual in advanced material design; unfortunately, these two mechanical properties are generally mutually exclusive. So far there exists only limited success of attaining both strength and toughness, which often needs material-specific, complicated, or expensive synthesis processes and thus can hardly be applicable to other materials. A general mechanism to address the conflict between strength and toughness still remains elusive. Here we report a first-of-its-kind study of the dependence of strength and toughness of cellulose nanopaper on the size of the constituent cellulose fibers. Surprisingly, we find that both the strength and toughness of cellulose nanopaper increase simultaneously (40 and 130 times, respectively) as the size of the constituent cellulose fibers decreases (from a mean diameter of 27 μm to 11 nm), revealing an anomalous but highly desirable scaling law of the mechanical properties of cellulose nanopaper: the smaller, the stronger and the tougher. Further fundamental mechanistic studies reveal that reduced intrinsic defect size and facile (re)formation of strong hydrogen bonding among cellulose molecular chains is the underlying key to this new scaling law of mechanical properties. These mechanistic findings are generally applicable to other material building blocks, and therefore open up abundant opportunities to use the fundamental bottom-up strategy to design a new class of functional materials that are both strong and tough.

In situ electro-mechanical experiments and mechanics modeling of tensile cracking in indium tin oxide thin films on polyimide substrates

Indium tin oxide (ITO) thin films supported by polymer substrates have been widely used as transparent electrodes/interconnects in flexible electronics. Understanding the electro-mechanical behaviors of such material system is crucial for reliable operation of flexible devices under large deformation. In this paper, we performed in situ mechanical and electrical tests of ITO thin films with two different thicknesses (200 and 80 nm) deposited on polyimide substrates inside a scanning electron microscope. The crack initiation and propagation, crack density evolution and the corresponding electrical resistance variation were systematically investigated. It was found that cracks initiated at a higher tensile strain level and saturated with a higher density in thinner ITO films. Integrated with a coherently formulated mechanics model, the cohesive toughness and fracture strength of ITO thin films and the ITO/polyimide interfacial toughness were quantitatively determined. The experimentally observed thickness d...

Processing bulk natural wood into a high-performance structural material

Synthetic structural materials with exceptional mechanical performance suffer from either large weight and adverse environmental impact (for example, steels and alloys) or complex manufacturing processes and thus high cost (for example, polymer-based and biomimetic composites). Natural wood is a low-cost and abundant material and has been used for millennia as a structural material for building and furniture construction. However, the mechanical performance of natural wood (its strength and toughness) is unsatisfactory for many advanced engineering structures and applications. Pre-treatment with steam, heat, ammonia or cold rolling followed by densification has led to the enhanced mechanical performance of natural wood. However, the existing methods result in incomplete densification and lack dimensional stability, particularly in response to humid environments, and wood treated in these ways can expand and weaken. Here we report a simple and effective strategy to transform bulk natural wood directly into a high-performance structural material with a more than tenfold increase in strength, toughness and ballistic resistance and with greater dimensional stability. Our two-step process involves the partial removal of lignin and hemicellulose from the natural wood via a boiling process in an aqueous mixture of NaOH and Na2SO3 followed by hot-pressing, leading to the total collapse of cell walls and the complete densification of the natural wood with highly aligned cellulose nanofibres. This strategy is shown to be universally effective for various species of wood. Our processed wood has a specific strength higher than that of most structural metals and alloys, making it a low-cost, high-performance, lightweight alternative.

Reprogrammable ultra-fast shape-transformation of macroporous composite hydrogel sheets

In this communication, we report a composite macroporous hydrogel sheet that can rapidly transform into multiple 3D shapes in response to near-infrared (NIR) light on demand. The transformation relies on the photo-thermal-induced asymmetric shrinking of the hydrogel material, which is further verified by finite element modeling.