20 μm-Thick Li6.4La3Zr1.4Ta0.6O12-Based Flexible Solid Electrolytes for All-Solid-State Lithium Batteries

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The Open Access journal Energy Material Advances, published in association with BIT, is an interdisciplinary platform for research in multiple fields from cutting-edge material to energy science.

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Energy Material Advances’ editorial board is led by Feng Wu (Beijing Institute of Technology) and Jun Liu (University of Washington) and is comprised of experts who have made significant and well recognized contributions to the field.

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Special Issue Multiscale Simulations for Energy Materials is open for submissions now!

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Research Article

Sodium-Ion Storage Properties of Thermally Stable Anatase

Anatase titanium dioxide (TiO2) is a potential anode material for sodium-ion batteries (NIBs). However, the low electronic conductivity and sluggish ion diffusion kinetics at high rate hamper its practical applications. Herein, we demonstrate a sol-gel approach to the synthesis of thermally stable anatase nanoparticles with a carbon shell as anode materials for NIBs. A sample calcined at 750 °C (designated as H-750TiO2@C) exhibits high-rate capability and excellent stability against cycling with no capacity loss after 2000 cycles at 1 A g-1. In situ X-ray diffraction and Raman spectroscopy characterization results reveal a nearly zero-strain characteristic of the anatase phase during charge/discharge processes. In situ transmission electron microscopy, ex situ X-ray photoelectron spectroscopy, and scanning electron microscope characterization results of samples collected at different charged and discharged states suggest that the anatase phase undergoes an irreversible sodiation-activation during the initial discharge process to form a sodiated-TiO2 phase. A full cell assembled with H-750TiO2@C as the anode and Na3V2(PO4)3 as the cathode delivers an energy density of 220 Wh kg-1, demonstrating H-750TiO2@C is a potential anode material for NIBs.

Research Article

Regulating Uniform Zn Deposition via Hybrid Artificial Layer for Stable Aqueous Zn-Ion Batteries

Aqueous Zn-ion batteries (ZIBs) have great potential as promising candidates for next-generation energy conversion and storage devices, benefiting from competitive theoretical capacity, low cost, and high security. However, further applications of ZIBs are impeded by dendrite generation and side reactions. Herein, considering that Zn dendrites are caused by nonuniform metal deposition, involving uneven electric field and Zn2+ ion flux, a dual-functional carbon-coated NaTi2(PO4)3 (NTP-C) artificial protective layer with large surface area is constructed onto the surface of metallic Zn to stabilize Zn anode and regulate uniform Zn deposition. Benefiting from a synergistic strategy, NTP-C coating not only takes advantages of carbon to provide abundant Zn deposition sites to homogenize nucleation, adjust electric field distribution, and reduce local current density but also utilizes the ionic channel in NTP structure to modulate the distribution of Zn2+ flux at the same time. Consequently, the NTP-C@Zn symmetrical cell exhibits a stable cycling for more than 600 h with a low polarization (18.6 mV) at 1 mA cm−2/1 mAh cm−2. Especially, the NTP-C@Zn symmetrical cell even enables a steady plating/stripping process at a harsh condition (100 mA cm−2) without short circuit, indicating a potential application of high-load electrodes or supercapacitors. Furthermore, the NTP-C@Zn//α-MnO2 full cell also displays enhanced electrochemical performance for 1200 cycles with a capacity retention of 76.6% under 5 C (~1.5 A g−1). This work provides a synergistic strategy combining two protective mechanisms and delivers new inspirations for the improvement of stable Zn anode in aqueous ZIBs.

Review Article

Layered Double Hydroxides for Oxygen Evolution Reaction towards Efficient Hydrogen Generation

Electrochemical water splitting is one of the effective ways to obtain highly pure hydrogen. However, as one of the two half reactions, oxygen evolution reaction (OER) has a high overpotential, resulting in the low-energy utilization efficiency. Therefore, numerous electrocatalysts have been developed to reduce the energy barrier of OER. Among them, layered double hydroxides (LDHs) are excellent OER electrocatalysts with flexible composition and structure, which have been widely investigated in the past decade. Recent studies have been focusing on the identification of active sites for LDHs during OER process, trying to reveal clear reaction mechanism for designing more efficient LDHs electrocatalysts. Hence, this review tries to discuss the advances in identifying active site of LDHs based OER electrocatalysts for efficient hydrogen generation. We first introduce the effect of structure, composition, and defects to the OER performance of LDHs. Furthermore, main attention is paid on the active sites and mechanisms during OER, especially the coordination structures and catalytic mechanisms of active sites. At the end of this review, we put forward the existing problems and shortcomings in this fields, and propose the corresponding solutions, aiming to further promote the development of outstanding OER electrocatalysts towards efficient hydrogen production.

Research Article

Magnesium/Lithium Hybrid Batteries Based on SnS2-MoS2 with Reversible Conversion Reactions

The magnesium/lithium hybrid batteries (MLHBs) featuring dendrite-less deposition with Mg anode and Li-storage cathode are a promising alternative to Li-ion batteries for large-scale energy storage. However, their limited energy density limits their practical implementation. To improve this, beyond the commonly proposed intercalation compounds, high-capacity conversion-type cathodes based on heterostructures of tin sulphide-molybdenum disulphide (SnS2-MoS2) are proposed in this work. Individual SnS2 is already a promising high-capacity electrode material for multivalent batteries and undergoes conversion reactions during the ion storage process. The introduction of S-deficient MoS2 enhances the reversibility of SnS2 in the conversion reaction via strong polysulfide anchoring and catalytic effect. Our results show that the SnS2-MoS2 electrode achieves a high charge capacity of ~600 mAh g-1 at 50 mA g-1 and an excellent rate capability of 240 mAh g-1 at 1000 mAh g-1 with a negligible capacity fading rate of 0.063% per cycle across 1000 cycles. The results highlight a new direction toward designing 2D heterostructures as high-capacity cathodes beyond intercalation-type cathodes for multivalent-ion batteries.

Research Article

Unraveling the Effect of Cation Types on Electrochromic Properties of Titanium Dioxide Nanocrystals

Electrochromic (EC) devices have been regarded as promising candidates for energy-saving smart windows, next-generation displays, and wearable electronics. Monovalent ions such as H+- and Li+-based electrolytes are the benchmark insertion ions for EC devices but have serious limitations such as high cost, instability, and difficulty to handle. Seeking multivalent electrolytes is an effective alternative way to prepare high-performance EC devices; unfortunately, the related reports are currently limited to tungsten oxide EC materials. Herein, for the first time, we investigate the EC properties driven by different valence cationic (i.e., Li+, Zn2+, and Al3+) electrolytes in the titanium dioxide system. It is found that the initial optical modulation ranges of TiO2 nanocrystal (NC) films in Li+, Zn2+, and Al3+ electrolytes are 76.8%, 77.4%, and 77.3%, respectively. After 250 cycles, the optical contrast of these films in Zn2+ electrolyte decreased by only 2.3%, much lower than that in benchmark Li+ electrolyte of 10.1% and Al3+ electrolyte of 59.1%. Density functional theory calculation indicates that the potential barriers of Li+, Zn2+, and Al3+ in TiO2 are 0.59, 0.55, and 0.74 eV, respectively, which makes TiO2 NCs show good EC properties in Zn2+ electrolytes. This work unravels the effect of different valence cations on the electrochromic properties of titanium dioxide NCs, which may provide some new directions for the development of excellent EC devices with long-term stability and durability.

Review Article

Recent Development of Integrated Systems of Microsupercapacitors

Development of wearable and portable electronics promotes the miniaturization of energy storage devices. Microsupercapacitor (MSC) featuring in fast charging and discharging rates, long cycle life, and high-power density stands out from miniaturized energy storage devices, particularly for its small size and adjustable structure which is easily processed to integrate with other on-chip electronics. In this review, we systematically analyzed the MSC integration with other electronics from the perspective of structures and functions. At the beginning, we briefly introduced typical MSCs with unique properties. Subsequently, applications and integrations of MSCs with energy-consuming or energy-generating electronics were highlighted. Furthermore, compatible materials and designed structure of the all-in-one device were also depicted. Finally, challenges and future development of MSC-integrated systems were put forward.