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High-energy Ni-rich layered oxide cathode materials such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) suffer from detrimental side reactions and interfacial structural instability when coupled with sulfide solid-state electrolytes in all-solid-state lithium-based batteries. To circumvent this issue, here we propose a gradient coating of the NMC811 particles with lithium oxy-thiophosphate (Li 3 P 1+x O 4 S 4x ). Via atomic layer deposition of Li 3 PO 4 and subsequent in situ formation of a gradient Li 3 P 1+x O 4 S 4x coating, a precise and conformal covering for NMC811 particles is obtained. The tailored surface structure and chemistry of NMC811 hinder the structural degradation associated with the layered-to-spinel transformation in the grain boundaries and effectively stabilize the cathode|solid electrolyte interface during cycling. Indeed, when tested in combination with an indium metal negative electrode and a Li 10 GeP 2 S 12 solid electrolyte, the gradient oxy-thiophosphate-coated NCM811-based positive electrode enables the delivery of a specific discharge capacity of 128 mAh/g after almost 250 cycles at 0.178 mA/cm 2 and 25 °C. Layered oxide cathode active materials suffer from interfacial structural instability when coupled with sulfide solid-state electrolytes. Here, the authors propose a gradient coating with a lithium oxythiophosphate layer that can stabilize the cathode|solid-state electrolyte interface.

Increasing the specific energy, energy density, specific power, energy efficiency and energy retention of electrochemical storage devices are major incentives for the development of all-solid-state batteries. However, a general evaluation of all-solid-state battery performance is often difficult to derive from published reports, mostly due to the interdependence of performance measures, but also due to the lack of a basic reference system. Here, we present all-solid-state batteries reduced to the bare minimum of compounds, containing only a lithium metal anode, β-Li 3 PS 4 solid electrolyte and Li(Ni 0.6 Co 0.2 Mn 0.2 )O 2 cathode active material. We use this minimalistic system to benchmark the performance of all-solid-state batteries. In a Ragone-type graph, we compare literature data for thiophosphate-, oxide-, phosphate- and polymer-based all-solid-state batteries with our minimalistic cell. Using fundamental equations for key performance parameters, we identify research targets towards high energy, high power and practical all-solid-state batteries. Considering the interdependence of performance measures and the lack of a basic reference system for all-solid-state batteries, Jürgen Janek and co-workers analyse literature performance data for major types of all-solid-state batteries and benchmark them against minimalistic reference cells.

Recent works into sulfide-type solid electrolyte materials have attracted much attention among the battery community. Specifically, the oxidative decomposition of phosphorus and sulfur based solid state electrolyte has been considered one of the main hurdles towards practical application. Here we demonstrate that this phenomenon can be leveraged when lithium thiophosphate is applied as an electrochemically “switched-on” functional redox mediator-generator for the activation of commercial bulk lithium sulfide at up to 70 wt.% lithium sulfide electrode content. X-ray adsorption near-edge spectroscopy coupled with electrochemical impedance spectroscopy and Raman indicate a catalytic effect of generated redox mediators on the first charge of lithium sulfide. In contrast to pre-solvated redox mediator species, this design decouples the lithium sulfide activation process from the constraints of low electrolyte content cell operation stemming from pre-solvated redox mediators. Reasonable performance is demonstrated at strict testing conditions. The decomposition of solid state electrolyte material has been well-known in the literature. Here the authors report that the same decomposition process can be leveraged to act as a source of redox mediator that is only activated at certain voltages for application in Li 2 S based cathodes.

While still premature as an energy storage technology, bulk solid-state batteries are attracting much attention in the academic and industrial communities lately. In particular, layered lithium metal oxides and lithium thiophosphates hold promise as cathode materials and superionic solid electrolytes, respectively. However, interfacial side reactions between the individual components during battery operation usually result in accelerated performance degradation. Hence, effective surface coatings are required to mitigate or ideally prevent detrimental reactions from occurring and having an impact on the cyclability. In the present work, we examine how surface carbonates incorporated into the sol–gel-derived LiNbO 3 protective coating on NCM622 [Li 1+ x (Ni 0.6 Co 0.2 Mn 0.2 ) 1– x O 2 ] cathode material affect the efficiency and rate capability of pellet-stack solid-state battery cells with β-Li 3 PS 4 or argyrodite Li 6 PS 5 Cl solid electrolyte and a Li 4 Ti 5 O 12 anode. Our research data indicate that a hybrid coating may in fact be beneficial to the kinetics and the cycling performance strongly depends on the solid electrolyte used.

Combining logical function and memory characteristics of transistors is an ideal strategy for enhancing computational efficiency of transistor devices. Here, we rationally design a tri-gate two-dimensional (2D) ferroelectric van der Waals heterostructures device based on copper indium thiophosphate (CuInP 2 S 6 ) and few layers tungsten disulfide (WS 2 ), and demonstrate its multi-functional applications in multi-valued state of data, non-volatile storage, and logic operation. By co-regulating the input signals across the tri-gate, we show that the device can switch functions flexibly at a low supply voltage of 6 V, giving rise to an ultra-high current switching ratio of 10 7 and a low subthreshold swing of 53.9 mV/dec. These findings offer perspectives in designing smart 2D devices with excellent functions based on ferroelectric van der Waals heterostructures.

The family of layered thio- and seleno-phosphates has gained attention as potential control dielectrics for the rapidly growing family of two-dimensional and quasi-two-dimensional electronic materials. Here we report a combination of density functional theory calculations, quantum molecular dynamics simulations and variable-temperature, -pressure and -bias piezoresponse force microscopy data to predict and verify the existence of an unusual ferroelectric property—a uniaxial quadruple potential well for Cu displacements—enabled by the van der Waals gap in copper indium thiophosphate (CuInP 2 S 6 ). The calculated potential energy landscape for Cu displacements is strongly influenced by strain, accounting for the origin of the negative piezoelectric coefficient and rendering CuInP 2 S 6 a rare example of a uniaxial multi-well ferroelectric. Experimental data verify the coexistence of four polarization states and explore the temperature-, pressure- and bias-dependent piezoelectric and ferroelectric properties, which are supported by bias-dependent molecular dynamics simulations. These phenomena offer new opportunities for both fundamental studies and applications in data storage and electronics. The atomic displacements that generate ferroelectricity in materials commonly fit a double-well potential energy surface. Here, ferroelectricity in two-dimensional CuInP 2 S 6 is shown to fit a quadruple well due to the van der Waals gap between layers of this material.

ObjectiveAn aptamer specifically binding to diethyl thiophosphate (DETP) was constructed and incorporated in an optical sensor and electrochemical techniques to enable the specific measurement of DETP as a metabolite and a biomarker of organophosphate exposure.ResultsA DETP-bound aptamer was selected from the library using capillary electrophoresis-systematic evolution of ligands by exponential enrichment (CE-SELEX). A colorimetric method revealed that the aptamer had the highest affinity for DETP, with a mean Kd value (± SD) of 0.103 ± 0.014 µM. The docking results and changes in resistance showed that the selectivity of the aptamer for DETP was higher than that for the similar structures of dithiophosphate (DEDTP) and diethyl phosphate (DEP). The altered amplitude of cyclic voltammetry showed a linear range of DETP detection covering 0.0001–10 µg/ml with a limit of detection of 0.007 µg/ml. The recovery value of a real sample of pH 7 was 97.2%.ConclusionsThe current method showed great promise in using the DETP-specific aptamer to detect the exposure history to organophosphates by measuring their metabolites, although degradation of organophosphate parent compounds might occur.

All-perovskite tandem solar cells (PTSCs) demonstrate exceptional potential to surpass the Shockley-Queisser (SQ) theoretical limit. However, practical implementation faces critical challenges due to a self-reinforcing photothermal-mechanical degradation mechanism originating from multiscale physical couplings. In this study, a multifunctional polyamine ligand triphenyltriamine thiophosphate (TPTA) was introduced into the tin-lead (Sn-Pb) perovskite solution system to establish an I-Sn-N coordination-mediated lattice stabilization framework, and the photothermal-mechanical coupling path was cut off from multiple aspects such as suppressing periodic oscillations and regulating stress. Consequently, single-junction Sn-Pb perovskite solar cells (PSCs) achieve a power conversion efficiency (PCE) of 23.4% and retaining 94.9% of initial performance after 950 hours of maximum power point (MPP) tracking. When the device is integrated into the 2-terminal (2 T) tandem architecture, its PCE reaches a significant level of 29.6 % (certified PCE of 28.9%), and 93.4% of the initial efficiency can be maintained after 900 hours continuous operation. Practical implementation of all-perovskite tandem solar cells faces challenges due to the self-reinforcing photothermal-mechanical degradation mechanism. Here, authors employ a polyamine ligand to establish I-Sn-N coordination for stabilizing lattice framework, achieving device efficiency of 29.6%.

Over the past few years, evidence has accrued that demonstrates that terrestrial photochemical reactions could have provided numerous (proto)biomolecules with implications for the origin of life. This chemistry simply relies on UV light, inorganic sulfur species and hydrogen cyanide. Recently, we reported that, under the same conditions, reduced phosphorus species, such as those delivered by meteorites, can be oxidized to orthophosphate, generating thiophosphate in the process. Here we describe an investigation of the properties of thiophosphate as well as additional possible means for its formation on primitive Earth. We show that several reported prebiotic reactions, including the photoreduction of thioamides, carbonyl groups and cyanohydrins, can be markedly improved, and that tetroses and pentoses can be accessed from hydrogen cyanide through a Kiliani–Fischer-type process without progressing to higher sugars. We also demonstrate that thiophosphate allows photochemical reductive aminations, and that thiophosphate chemistry allows a plausible prebiotic synthesis of the C5 moieties used in extant terpene and terpenoid biosynthesis, namely dimethylallyl alcohol and isopentenyl alcohol.The streamlined synthesis of multiple (proto)biomolecules from common starting materials is a key goal of prebiotic chemistry. Now, a one-pot synthesis of ribo-aminooxazoline (a precursor for prebiotic nucleotide synthesis) from HCN has been achieved. Additionally, the two moieties used in extant terpenoid biosynthesis have been accessed, with all carbon atoms also originating from HCN.

The all-solid-state lithium batteries using solid electrolytes are considered to be the new generation of devices for energy storage, which might be a key solution for power electric and hybrid electric vehicles in the future. This review focuses on the crystal structures and electrochemical properties of sulfide solid electrolytes. They are classified to several subgroups according to their chemical compositions, namely thiophosphates, halide thiophosphates, sulfide without phosphorus, and glassy sulfides electrolytes, which might be potential solid electrolytes in lithium batteries and may replace the currently used polymeric electrolytes for LIBs. Through discussion, this review provides an insight into future promising sulfide electrolytes.