High-Entropy Energy Materials in the Age of Big Data: A Critical Guide to Next-Generation Synthesis and Applications

High-entropy materials (HEMs) with promising energy storage and conversion properties have recently attracted worldwide increasing research interest. Nevertheless, most research on the synthesis of HEMs focuses on a “trial and error” method without any guidance, which is very laborious and time-consuming. This review aims to provide an instructive approach to searching and developing new high-entropy energy materials in a much more efficient way. Toward materials design for future technologies, a fundamental understanding of the process/structure/property/performance linkage on an atomistic level will promote prescreening and selection of material candidates. With the help of computational material science, in which the fast development of computational capabilities that have a rapidly growing impact on new materials design, this fundamental understanding can be approached. Furthermore, high-throughput experimental methods, enabled by the advances in instrumentation and electronics, will accelerate the production of large quantities of results and stimulate the identification of the target products, adding knowledge in computational design. This review shows that combining computational preselection and verification by high-throughput can be an efficient approach to unveil the complexities of HEMs and design novel HEMs with enhanced properties for energy-related applications

High‐Entropy Energy Materials in the Age of Big Data: A Critical Guide to Next‐Generation Synthesis and Applications

High-entropy materials (HEMs) with promising energy storage and conversion properties have recently attracted worldwide increasing research interest. Nevertheless, most research on the synthesis of HEMs focuses on a “trial and error” method without any guidance, which is very laborious and time-consuming. This review aims to provide an instructive approach to searching and developing new high-entropy energy materials in a much more efficient way. Toward materials design for future technologies, a fundamental understanding of the process/structure/property/performance linkage on an atomistic level will promote prescreening and selection of material candidates. With the help of computational material science, in which the fast development of computational capabilities that have a rapidly growing impact on new materials design, this fundamental understanding can be approached. Furthermore, high-throughput experimental methods, enabled by the advances in instrumentation and electronics, will accelerate the production of large quantities of results and stimulate the identification of the target products, adding knowledge in computational design. This review shows that combining computational preselection and verification by high-throughput can be an efficient approach to unveil the complexities of HEMs and design novel HEMs with enhanced properties for energy-related applications

Operando acoustic emission monitoring of degradation processes in lithium-ion batteries with a high-entropy oxide anode

In recent years, high-entropy oxides are receiving increasing attention for electrochemical energy-storage applications. Among them, the rocksalt (Co$_{0.2}$Cu$_{0.2}$Mg$_{0.2}$Ni$_{0.2}$Zn$_{0.2}$)O (HEO) has been shown to be a promising high-capacity anode material. Because high-entropy oxides constitute a new class of electrode materials, systematic understanding of their behavior during ion insertion and extraction is yet to be established. Here, we probe the conversion-type HEO material in lithium half-cells by acoustic emission (AE) monitoring. Especially the clustering of AE signals allows for correlations of acoustic events with various processes. The initial cycle was found to be the most acoustically active because of solid-electrolyte interphase formation and chemo-mechanical degradation. In the subsequent cycles, AE was mainly detected during delithiation, a finding we attribute to the progressive crack formation and propagation. Overall, the data confirm that the AE technology as a non-destructive operando technique holds promise for gaining insight into the degradation processes occurring in battery cells during cycling

Fully Printed Inverters using Metal‐Oxide Semiconductor and Graphene Passives on Flexible Substrates

Printed and flexible metal‐oxide transistor technology has recently demonstrated great promise due to its high performance and robust mechanical stability. Herein, fully printed inverter structures using electrolyte‐gated oxide transistors on a flexible polyimide (PI) substrate are discussed in detail. Conductive graphene ink is printed as the passive structures and interconnects. The additive printed transistors on PI substrates show an $_{on}$/$_{off}$ ratio of 10$^{6}$ and show mobilities similar to the state‐of‐the‐art printed transistors on rigid substrates. Printed meander structures of graphene are used as pull‐up resistances in a transistor–resistor logic to create fully printed inverters. The printed and flexible inverters show a signal gain of 3.5 and a propagation delay of 30 ms. These printed inverters are able to withstand a tensile strain of 1.5% following more than 200 cycles of mechanical bending. The stability of the electrical direct current (DC) properties has been observed over a period of 5 weeks. These oxide transistor‐based fully printed inverters are relevant for digital printing methods which could be implemented into roll‐to‐roll processes

Fully Printed Electrolyte‐Gated Transistor Formed in a 3D Polymer Reservoir with Laser Printed Drain/Source Electrodes

In solution processed electronic devices it is crucial that the deposited inks are properly aligned and that all post-processing steps are compliant with each other. Moreover, shorter channel lengths are highly beneficial to increase the device performance. Herein, laser printing of metals and polymer reservoirs allows to print sub-micrometer sized channel lengths while confining functional inks into these small gaps. Therefore, a manufacturing concept and optimized material stack, suitable for combined inkjet and laser printing are proposed. A nanoparticulate indium oxide (In$_2$O$_3$) semiconductor is inkjet printed into and constrained by a 3D laser written polymer (pentaerythritol triacrylate, PETA) reservoir. Inside the 3D printed polymer reservoir, platinum (Pt) electrodes, that are further routed over the reservoir walls, are laser printed by a metal reduction process. The transistor fabrication is completed by a second inkjet printed layer of composite solid polymer electrolyte and an organic top-gate layer (PEDOT:PSS). This concept does not exceed annealing temperatures higher than 100°C, and is compatible with a range of substrates. The characterized electrolyte-gated field-effect transistor show a reasonable on/off-ratio in the range of 10$^4$ with negligible leakage currents. This materials and hybrid device manufacturing scheme has believed great potential for bioelectronics, lab-on-a-chip applications and others

High-entropy energy materials: Challenges and new opportunities

The essential demand for functional materials enabling the realization of new energy technologies has triggered tremendous efforts in scientific and industrial research in recent years. Recently, high-entropy materials, with their unique structural characteristics, tailorable chemical composition and correspondingly tunable functional properties, have drawn increasing interest in the fields of environmental science and renewable energy technology. Herein, we provide a comprehensive review of this new class of materials in the energy field. We begin with discussions on the latest reports on the applications of high-entropy materials, including alloys, oxides and other entropy-stabilized compounds and composites, in various energy storage and conversion systems. In addition, we describe effective strategies for rationally designing high-entropy materials from computational techniques and experimental aspects. Based on this overview, we subsequently present the fundamental insights and give a summary of their potential advantages and remaining challenges, which will ideally provide researchers with some general guides and principles for the investigation and development of advanced high-entropy materials