Berit H. Goodge, Danfeng Li, Motoki Osada, Bai Yang Wang, Yi Cui, Lena F. Kourkoutis, Harold Y. Hwang
Abstract
The recent observation of superconductivity in Nd0.8Sr0.2NiO2 calls for further investigation and optimization of the synthesis of this infinite-layer nickelate structure. Here, we present our current understanding of important aspects of the growth of the parent perovskite compound via pulsed laser deposition on SrTiO3 (001) substrates and the subsequent topotactic reduction. We find that to achieve single-crystalline, single-phase superconducting Nd0.8Sr0.2NiO2, it is essential that the precursor perovskite Nd0.8Sr0.2NiO3 thin film is stabilized with no visible impurity phases; in particular, a Ruddlesden–Popper-type secondary phase is often observed. We have further investigated the evolution of the soft-chemistry topotactic reduction conditions to realize full transformation to the infinite-layer structure with no film decomposition or formation of other phases. We find that capping the nickelate film with a subsequent SrTiO3 layer provides an epitaxial template to the top region of the nickelate film, much like the substrate. Thus, for currently optimized growth conditions, we can stabilize superconducting single-phase Nd0.8Sr0.2NiO2 (001) epitaxial thin films up to ∼10 nm.
Eilam Yalon, Connor J McClellan, Jinsong Zhang, Ozgur Burak Aslan, Aditya Sood, Jie Sun, Christopher M Andolina, Wissam A Saidi, Kenneth E Goodson, Tony F Heinz, Yi Cui and Eric Pop
Abstract
Layered two-dimensional (2D) materials such as MoS2 have attracted much attention for nano- and opto-electronics. Recently, intercalation (e.g. of ions, atoms, or molecules) has emerged as an effective technique to modulate material properties of such layered 2D films reversibly. We probe both the electrical and thermal properties of Li-intercalated bilayer MoS2 nanosheets by combining electrical measurements and Raman spectroscopy. We demonstrate reversible modulation of carrier density over more than two orders of magnitude (from 0.8 × 1012 to 1.5 × 1014 cm−2), and we simultaneously obtain the thermal boundary conductance between the bilayer and its supporting SiO2 substrate for an intercalated system for the first time. This thermal coupling can be reversibly modulated by nearly a factor of eight, from 14 ± 4.0 MW m−2 K−1 before intercalation to 1.8 ± 0.9 MW m−2 K−1 when the MoS2 is fully lithiated. These results reveal electrochemical intercalation as a reversible tool to modulate and control both electrical and thermal properties of 2D layers.
William Huang , Hansen Wang , Yuzhang Li, Hao Chen, Zhiao Yu, Wenbo Zhang, Zhenan Bao and Yi Cui
Abstract
Rechargeable lithium (Li) metal batteries must have long cycle life and calendar life (retention of capacity during storage at open circuit). Particular emphasis has been placed on prolonging the cycle life of Li metal anodes, but calendar ageing is less understood. Here, we show that Li metal loses at least 2–3% of its capacity after only 24 hours of ageing, regardless of the electrolyte chemistry. These losses of capacity during calendar ageing also shorten the cycle life of Li metal batteries. Cryogenic transmission electron microscopy shows that chemical corrosion of Li and the continuous growth of the solid electrolyte interphase—a passivation film on Li—cause the loss of capacity. Electrolytes with long cycle life do not necessarily form a solid electrolyte interphase with more resistance to chemical corrosion, so functional electrolytes must simultaneously minimize the rate of solid electrolyte interphase growth and the surface area of electrodeposited Li metal.
Wei-Sheng Lee, Harold Y. Hwang, Yi Cui, Jan Zaanen, Thomas Devereaux, Brian Moritz, and Chunjing Jia
Abstract
The recent discovery of superconductivity in oxygen-reduced monovalent nickelates has raised a new platform for the study of unconventional superconductivity, with similarities to and differences from the cuprate high-temperature superconductors. In this paper, we investigate the family of infinite-layer nickelates RNiO2 with rare-earth R spanning across the lanthanide series, introducing a new and nontrivial “knob” with which to tune nickelate superconductivity. When traversing from La to Lu, the out-of-plane lattice constant decreases dramatically with an accompanying increase of Ni d x2−y2 bandwidth; however, surprisingly, the role of oxygen charge transfer diminishes. In contrast, the magnetic exchange grows across the lanthanides, which may be favorable to superconductivity. Moreover, compensation effects from the itinerant 5d electrons present a closer analogy to Kondo lattices, indicating a stronger interplay between charge transfer, bandwidth renormalization, compensation, and magnetic exchange. We also obtain the microscopic Hamiltonian using the Wannier downfolding technique, which will provide the starting point for further many-body theoretical studies.
Yusheng Ye, Lee Hiang Kwee, Wenxiao Huang, Rong Xu, Xin Gao, Renjie Chen, Feng Wu, Tsung Chia-Kuang, Yi Cui
Abstract
Safety issues associated with lithium-ion batteries are of major concern, especially with the ever-growing demand for higher-energy-density storage devices. Although flame retardants (FRs) added to electrolytes can reduce fire hazards, large amounts of FRs are required and they severely deteriorate battery performance. Here, we report a feasible method to balance flame retardancy and electrochemical performance by coating an electrolyte-insoluble FR on commercial battery separators. By integrating dual materials via a two-pronged mechanism, the quantity of FR required could be limited to an ultrathin coating layer (4 μm) that rarely influences electrochemical performance. The developed composite separator has a four-times better flame retardancy than conventional polyolefin separators in full pouch cells. Additionally, this separator can be fabricated easily on a large scale for industrial applications. High-energy-density batteries (2 Ah) were assembled to demonstrate the scaling of the composite separator and to confirm its enhanced safety through nail penetration tests.
Yangtao Ou, Bao Zhang, Jindi Wang, Lin Fu, Mintao Wan, Guocheng Li, Wenyu Wang, Li Wang, Jianjun Jiang, Zhi Wei Seh, Enyuan Hu, Xiao-Qing Yang, Yi Cui, and Yongming Sun
Abstract
Metal anodes represent as a prime choice for the coming generation rechargeable batteries with high energy density. However, daunting challenges including electrode volume variation and inevitable side reactions preclude them from becoming a viable technology. Here, a facile replacement reaction was employed to fabricate a three-dimensional (3D) interdigitated metal/solid electrolyte composite electrode, which not only provides a stable host structure for buffering the volume change within the composite but also prevents side reactions by avoiding the direct contact between active metal and liquid electrolyte. As a proof-of-concept demonstration, a 3D interdigitated zinc (Zn) metal/solid electrolyte architecture was fabricated via a galvanic replacement reaction between Zn metal foil and indium (In) chloride solution followed by electrochemical activation, featuring the interdigitation between metallic Zn and amorphous indium hydroxide sulfate (IHS) with high Zn2+ conductivity (56.9 ± 1.8 mS cm–1), large Zn2+ transference number (0.55), and high electronic resistivity [(2.08 ± 0.01) × 103 Ω cm]. The as-designed Zn/IHS electrode sustained stable electrochemical Zn plating/stripping over 700 cycles with a record-low overpotential of 8 mV at 1 mA cm–2 and 0.5 mAh cm–2. More impressively, it displayed cycle-stable performance with low overpotential of 10 mV under ultrahigh current density and areal capacity (20 mA cm–2, 20 mAh cm–2), which outperformed all the reported Zn metal electrodes in mild aqueous electrolyte. The fabrication of interdigitated metal/solid electrolyte was generalized to other metal pairs, including Zn/Sn and Zn/Co, which provide inspiration for next-generation Zn metal batteries with high energy density and reversibility.
William Huang, Zhiao Yu, Wenxiao Huang, Rong Xu, Zewen Zhang, Zhenan Bao, Yi Cui
Abstract
Advanced electrolytes were developed to improve the cyclability of lithium (Li) metal anodes, yet their working mechanisms remain unclear. Here, we study the Li cycling performance under different pressures in a 1 M Li bis(fluorosulfonyl)imide/fluorinated 1,4-dimethoxybutane electrolyte. A consistently long cycle life is achieved over a wide range of pressures (30–600 psi). This is due to a completely different Li plating mode with more favorable deposition morphologies compared to that in a conventional carbonate electrolyte, which exhibits increasing cycle stability with increased pressure. We show that this is enabled by the properties of an anion-derived residual solid-electrolyte interphase (rSEI) framework on the electrode surface, an undercharacterized structure with profound implications for Li metal cycling. This anion-derived rSEI chemistry is likely the key to a prolonged cycle life of Li metal batteries and should be vigorously addressed in future electrolyte designs.
Sang Cheol Kim, Tomás Rojas, Yangying Zhu, Yanbin Li, Lin Ma, Kang Xu, Anh T. Ngo, Yi Cui
Abstract
Temperature coefficients (TCs) for either electrochemical cell voltages or potentials of individual electrodes have been widely utilized to study the thermal safety and cathode/anode phase changes of lithium (Li)-ion batteries. However, the fundamental significance of single electrode potential TCs is little known. In this work, we discover that the Li-ion desolvation process during Li deposition/intercalation is accompanied by considerable entropy change, which significantly contributes to the measured Li/Li+ electrode potential TCs. To explore this phenomenon, we compare the Li/Li+ electrode potential TCs in a series of electrolyte formulations, where the interaction between Li-ion and solvent molecules occurs at varying strength as a function of both solvent and anion species as well as salt concentrations. As a result, we establish correlations between electrode potential TCs and Li-ion solvation structures and further verify them by ab initio molecular dynamics simulations. We show that measurements of Li/Li+ electrode potential TCs provide valuable knowledge regarding the Li-ion solvation environments and could serve as a screening tool when designing future electrolytes for Li-ion/Li metal batteries.
Aqueous Zn-based batteries are attractive because of the low cost and high theoretical capacity of the Zn metal anode. However, the Zn-based batteries developed so far utilize an excess amount of Zn (i.e., thick Zn metal anode), which decreases the energy density of the whole battery. Herein, we demonstrate an anode-free design (i.e., zero-excess Zn), which is enabled by employing a nanocarbon nucleation layer. Electrochemical studies show that this design allows for uniform Zn electrodeposition with high efficiency and stability over a range of current densities and plating capacities. Using this anode-free configuration, we showcase a Zn–MnO2 battery prototype, showing 68.2% capacity retention after 80 cycles. Our anode-free design opens a new direction for implementing aqueous Zn-based batteries in energy storage systems.
Lei Liao, Wang Xiao, Arturas Vailionis, Antonio J. Ricco, Robin White, Yoshio Nishi, Wah Chiu, Steven Chu, Yi Cui
Abstract
The global COVID-19 pandemic has changed many aspects of daily lives. Wearing personal protective equipment, especially respirators (face masks), has become common for both the public and medical professionals, proving to be effective in preventing spread of the virus. Nevertheless, a detailed understanding of respirator filtration-layer internal structures and their physical configurations is lacking. Here, we report three-dimensional (3D) internal analysis of N95 filtration layers via X-ray tomography. Using deep learning methods, we uncover how the distribution and diameters of fibers within these layers directly affect contaminant particle filtration. The average porosity of the filter layers is found to be 89.1%. Contaminants are more efficiently captured by denser fiber regions, with fibers <1.8 μm in diameter being particularly effective, presumably because of the stronger electric field gradient on smaller diameter fibers. This study provides critical information for further development of N95-type respirators that combine high efficiency with good breathability.