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The revival of ternary halides Li-M-X (M = Y, In, Zr, etc.; X = F, Cl, Br) as solid-state electrolytes (SSEs) shows promise in realizing practical solid-state batteries due to their direct compatibility toward high-voltage cathodes and favorable room-temperature ionic conductivities. Most of the reported superionic halide SSEs have a structural pattern of [MCl

Most information used to evaluate diabetic statuses is collected at a special time-point, such as taking fasting plasma glucose test and providing a limited view of individual's health and disease risk. As a new parameter for continuously evaluating personal clinical statuses, the newly developed technique "continuous glucose monitoring" (CGM) can characterize glucose dynamics. By calculating the complexity of glucose time series index (CGI) with refined composite multi-scale entropy analysis of the CGM data, the study showed for the first time that the complexity of glucose time series in subjects decreased gradually from normal glucose tolerance to impaired glucose regulation and then to type 2 diabetes (P for trend0.01). Furthermore, CGI was significantly associated with various parameters such as insulin sensitivity/secretion (all P0.01), and multiple linear stepwise regression showed that the disposition index, which reflects β-cell function after adjusting for insulin sensitivity, was the only independent factor correlated with CGI (P0.01). Our findings indicate that the CGI derived from the CGM data may serve as a novel marker to evaluate glucose homeostasis.

Lithium ion conducting argyrodites are among the most studied solid electrolytes due to their high ionic conductivities. A major concern in a solid-state battery is the solid electrolyte stability. Here we present a systematic study on the influence of cationic and anionic substitution on the electrochemical stability of Li6PS5X, using step-wise cyclic voltammetry, optical band gap measurements, hard X-ray photoelectron spectroscopy along with first-principles calculations. We observe that going from Li6PS5Cl to Li6+xP1-xMxS5I (M = Si4+, Ge4+), the oxidative degradation does not change. Considering the chemical bonding shows that the valence band edges are mostly populated by non-bonding orbitals of the PS43- units or unbound sulfide anions and that simple substitutions in these sulfide-based solid electrolytes cannot improve oxidative stabilities. This work provides insights on the role of chemical bonding on the stability of superionic conductors and shows that alternative strategies are needed for long-term stable solid-state batteries.

This study aimed to evaluate the influence of Jinlida granules on glycemic variability with or without metformin treatment in patients with newly diagnosed type 2 diabetes. This study was a 16-week, double-blinded, randomized, controlled clinical trial. The enrolled patients with newly diagnosed type 2 diabetes were randomly divided into four groups: control, Jinlida, metformin, and combination treatment groups. A retrospective continuous glucose monitoring (CGM) system was used for subcutaneous interstitial glucose monitoring for 3 days consecutively. Hemoglobin A1c (HbA1c), traditional Chinese medicine symptom score, and CGM parameters, including glucose coefficient of variation, standard deviation of blood glucose values, and time in range of glucose 3.9–10.0 mmol/L, were assessed pre-test and post-test. A total of 138 participants completed the entire procedure. Compared with the pre-test, fasting plasma glucose, 2 hour postprandial plasma glucose, HbA1c, and traditional Chinese medicine symptom score all decreased in the four groups at the end of the test, and the combination treatment group showed the most significant decrease. In terms of CGM parameters, time in range of the Jinlida and metformin groups improved after intervention compared with the baseline (Jinlida group: 78.68 ± 26.15 versus 55.47 ± 33.29; metformin group: 87.29 ± 12.21 vs. 75.44 ± 25.42; P < 0.01). Additionally, only the Jinlida group showed decreased glucose standard deviation after intervention (1.57 ± 0.61 vs. 1.96 ± 0.95; P < 0.01). Jinlida granules can improve glycemic control and glycemic variability in patients with newly diagnosed type 2 diabetes. Clinical trial registration number: ChiCTR-IOR-16009296.

All-solid-state batteries with a lithium metal anode, enabled by lithium garnet solid electrolytes such as Li7La3Zr2O12 (LLZO), are a promising next-generation energy-storage technology. The further development of all-solid-state battery requires the integration of high-energy cathodes such as LiNi1-x-yMnxCoyO2 (NMC) with the garnet solid electrolyte with stable and low-resistance interfaces, which requires a coating layer to stabilize the interface during high-temperature sintering and electrochemical cycling. In order to guide the future development of interfacial coatings, we perform high-throughput thermodynamic analyses based on first-principles computation to investigate the stability of LLZO garnet and high-energy NMC cathodes with a wide range of materials chemistries. Our study reveals the factors governing the materials stability with LLZO garnet and NMC cathodes, and identifies the mechanisms of good coating layers stable with LLZO and NMC. In addition to classifying known coating layers, our study provides detailed guiding charts and multiple new materials systems as promising coatings for stabilizing LLZO NMC interfaces to enable high-energy-density garnet-based all-solid-state batteries. Our demonstrated computation scheme and high-throughput analyses are generally applicable to investigate and screen coating materials for stabilizing interfaces in energy-related applications.

All-solid-state battery with Li metal anode is a promising rechargeable battery technology with high energy density and improved safety. Currently, the application of Li metal anode is plagued by the failure at the interfaces between lithium metal and solid electrolyte (SE). However, little is known about the defects at Li-SE interfaces and their effects on Li cycling, impeding further improvement of Li metal anodes. Herein, by performing large-scale atomistic modeling of Li metal interfaces with common SEs, we discover that lithium metal forms an interfacial defect layer of nanometer-thin disordered lithium at the Li-SE interfaces. This interfacial defect Li layer is highly detrimental, leading to interfacial failure such as pore formation and contact loss during Li stripping. By systematically studying and comparing incoherent, coherent, and semi-coherent Li-SE interfaces, we find that the interface with good lattice coherence has reduced Li defects at the interface and has suppressed interfacial failure during Li cycling. Our finding discovered the critical roles of atomistic lithium defects at interfaces for the interfacial failure of Li metal anode, and motivates future atomistic-level interfacial engineering for Li metal anode in solid-state batteries.

The adsorption of AlCl$_{3}$ on Si(100) and the effect of annealing the AlCl$_{3}$-dosed substrate was studied to reveal key surface processes for the development of atomic-precision acceptor-doping techniques. This investigation was performed via scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. At room temperature, AlCl$_{3}$ readily adsorbed to the Si substrate dimers and dissociated to form a variety of species. Annealing of the AlCl$_{3}$-dosed substrate at temperatures below 450 $^{\circ}$C produced unique chlorinated aluminum chains (CACs) elongated along the Si(100) dimer row direction. An atomic model for the chains is proposed with supporting DFT calculations. Al was incorporated into the Si substrate upon annealing at 450 $^{\circ}$C and above, and Cl desorption was observed for temperatures beyond 450 $^{\circ}$C. Al-incorporated samples were encapsulated in Si and characterized by secondary ion mass spectrometry (SIMS) depth profiling to quantify the Al atom concentration, which was found to be in excess of 10$^{20}$ cm$^{-3}$ across a $\sim$2.7 nm thick $\delta$-doped region. The Al concentration achieved here and the processing parameters utilized promote AlCl$_{3}$ as a viable gaseous precursor for novel acceptor-doped Si materials and devices for quantum computing., Comment: 35 pages, 8 figures

Phonon-based (vibrational) theories of ion transport are likely key to developing new design strategies for solid-state ionic conductors. However, they are not often utilized because it is difficult to ascertain which vibrational frequencies are important, even in describing fundamental parameters such as the activation barrier. This is perpetuated by the fact that it is difficult to tune vibrational frequencies directly, without changing the chemical structure, in order to study underlying phonon relations. Using isotopic substitution of 6Li for 7Li, we are able to change the mobile ion vibrations in the two exemplary ion conductors Li10SnP2S12 and Li6PS5Cl without altering their structure. Using a combination of nuclear magnetic resonance spectroscopy and ab initio molecular dynamics simulations to characterize temperature-dependent ion transport, it is demonstrated that the isotopic substitution of 6Li for 7Li increases the activation barrier for Li-ion transport. The magnitude of this isotope effect cannot be explained by changes in the zero-point vibrational energy alone. Therefore, we propose that the observed change in the activation barrier is related to the differences in the average critical phonon occupation needed to overcome the activation barrier. Our hypothesis is supported by an analytical model, based on the physics of quantum harmonic oscillators, that gives good agreement with the experimental results. Thus, isotopic substitution provides unique insights into the vibrational perspective and frequency dependence of the activation barrier in fast Li-ion conductors.

Lingli Cai,* Cheng Li,* Yufei Wang, Yifei Mo, Jun Yin, Xiaojing Ma Department of Endocrinology and Metabolism, Shanghai Jiao Tong University Affiliated Sixth People’s Hospital; Shanghai Clinical Center for Diabetes; Shanghai Diabetes Institute; Shanghai Key Laboratory of Diabetes Mellitus, Shanghai, People’s Republic of China*These authors contributed equally to this workCorrespondence: Jun Yin; Xiaojing MaDepartment of Endocrinology and Metabolism, Shanghai Jiao Tong University Affiliated Sixth People’s Hospital, 600 Yishan Road, Shanghai, 200233, People’s Republic of ChinaTel +86-21-64369181Fax +86-21-64368031Email yinjun@sjtu.edu.cn; maxiaojing@sjtu.edu.cnAim: Growth differentiation factor 15 (GDF15) is closely related to obesity. This study aimed to explore the influence of weight loss intervention on serum GDF15 levels and the relationship between GDF15 and metabolism.Materials and Methods: Forty-four overweight and obese adults either adopted a low-carbohydrate diet or performed moderate-to-vigorous exercise for 3 weeks. Weekly follow-ups were conducted to measure body composition, glucose and lipid metabolism and serum GDF15 levels.Results: After 3 weeks of intervention, body weight, fat mass and waist circumference in both groups decreased (P < 0.05). No significant change in GDF15 levels was observed in the two groups. Among all the subjects, 10 of them (22.7%, group of Down) showed a decrease in GDF15 and 34 (77.3%, group of Up) showed an increase in GDF15 after the intervention. We found that GDF15 increased significantly with the follow-up time in the UP group and waist circumference, fasting serum insulin (FINS), homeostasis model assessment of insulin resistance (HOMA-IR) and triglycerides (TG) decreased (P for trend < 0.05). However, no significant differences in all parameters were detected in Down group. In addition, GDF15 was elevated between 30 mins and 120 mins in a 75-g oral glucose tolerance test. Its trend was negatively correlated with plasma glucose and serum insulin.Conclusion: Increased serum GDF15 was associated with improvement in metabolism by lifestyle intervention among young overweight and obese adults. The increase of GDF15 could be an indicator to evaluate metabolic improvements in overweight and obese people.Clinical Trial Registration: www.chictr.org.cn, registration number ChiCTR1800016786.Keywords: growth differentiation factor 15, obesity, metabolism, low-carbohydrate diet, exercise

Oxide nanoparticles with elemental and structural diversity are widely studied for catalysis and energy applications. While compositional control holds great promise for materials discovery, current oxide nanoparticles are typically limited to a few cations due to the intrinsic complexity in nanoscale multi-element mixing. Here we report the rational design and synthesis of single-phase multi-element oxide nanoparticles with tunable composition, size and structure. We have identified temperature-, oxidation- and entropy-driven synthesis strategies to mix a range of elements with largely dissimilar oxidation potentials (including palladium), thus greatly expanding the compositional space. Through rapid synthesis and screening, we obtained a denary multi-element oxide catalyst showing high performance and superior stability for catalytic methane combustion over 100 hours due to the high-entropy design and stabilization. Our work therefore provides a viable synthesis route with clear guidelines for multi-element oxide nanoparticles and enables materials design in the multi-element space towards highly stable catalysts. Multi-element oxide catalysts can feature superior properties compared with their single-element analogues but obtaining such complex structures remains a challenge. Here, a method is reported to access single-phase denary nanoparticles as stable and efficient catalysts for the combustion of methane.

Li phosphorus oxynitride (LiPON) is one of a very few solid electrolytes that have demonstrated high stability against Li metal and extended cyclability with high Coulombic efficiency for all solid-state batteries (ASSBs). However, theoretical calculations show that LiPON reacts with Li metal. Here, we utilize in situ electron microscopy to observe the dynamic evolutions at the LiPON-Li interface upon contacting and under biasing. We reveal that a thin interface layer (∼60 nm) develops at the LiPON-Li interface upon contact. This layer is composed of conductive binary compounds that show a unique spatial distribution that warrants an electrochemical stability of the interface, serving as an effective passivation layer. Our results explicate the excellent cyclability of LiPON and reconcile the existing debates regarding the stability of the LiPON-Li interface, demonstrating that, though glassy solid electrolytes may not have a perfect initial electrochemical window with Li metal, they may excel in future applications for ASSBs.

Aims/Introduction To define the target value for the percentage coefficient of variation for glucose (%CV) as a measure of glycemic variability (GV) in Chinese diabetes patients. Materials and Methods This retrospective study included 3,007 diabetes patients who underwent continuous glucose monitoring for 3 days. Type 2 diabetes was divided into groups according to the received treatment: group 1, non‐insulinotropic agent (n = 138); group 2, insulinotropic agent (n = 761); group 3, basal insulin therapy (n = 100); group 4, premixed insulin (n = 784); and group 5, intensive insulin therapy (n = 612). Type 1 diabetes patients were included as group 6 (n = 612). %CV and percentage of time per day within, below (3.9mmol/L; TBR3.9) and above (10.0 mmol/L) the target glucose range (3.9–10.0 mmol/L) were computed. TBR3.9 ≥4% was defined as excessive hypoglycemia. Results Type 2 diabetes with a premixed or intensive insulin regimen had an increased %CV compared with those receiving oral therapy or basal insulin. The upper limit of %CV in group 1 was 33%, which was adopted as the threshold to define excessive GV. For each treatment group, the percentage of people with TBR3.9 ≥4% was significantly greater in the subgroup with %CV >33% than ≤33% (P 70% and time per day above 10.0 mmol/L

Nanoscale multi-principal element intermetallics (MPEIs) may provide a broad and tunable compositional space of active, high–surface area materials with potential applications such as catalysis and magnetics. However, MPEI nanoparticles are challenging to fabricate because of the tendency of the particles to grow/agglomerate or phase-separated during annealing. Here, we demonstrate a disorder-to-order phase transition approach that enables the synthesis of ultrasmall (4 to 5 nm) and stable MPEI nanoparticles (up to eight elements). We apply just 5 min of Joule heating to promote the phase transition of the nanoparticles into L1 0 intermetallic structure, which is then preserved by rapidly cooling. This disorder-to-order transition results in phase-stable nanoscale MPEIs with compositions (e.g., PtPdAuFeCoNiCuSn), which have not been previously attained by traditional synthetic methods. This synthesis strategy offers a new paradigm for developing previously unexplored MPEI nanoparticles by accessing a nanoscale-size regime and novel compositions with potentially broad applications.

To investigate the association between short-term glycemic variability (GV) and all-cause mortality in type 2 diabetes with well-controlled glucose profile by continuous glucose monitoring (CGM).In this prospective study, 1839 diabetes patients who reached percentage of time in the target glucose range of 3.9-10 mmol/L 70%, percentage of time above range of 10 mmol/L 25% and percentage of time below range of 3.9 mmol/L 4% on CGM were enrolled and were classified into five groups by coefficient of variation for glucose (%CV) level: ≤20%, 20-25%, 25-30%, 30-35%, and 35%. Cox proportional hazard models were used to estimate hazard ratios (HRs) of all-cause mortality risk associated with the different %CV categories.At baseline, participants had mean age of 60.9 years and mean HbAGreater %CV was associated with increased risk for all-cause mortality even among patients with seemingly well-controlled glucose status.

Solid oxide proton conductor materials are crucial for enabling hydrogen-based energy applications such as solid oxide fuel cells and solid oxide membranes. The improvement in the performance and e...

Ion transport in crystalline fast ionic conductors is a complex physical phenomenon. Certain ionic species (e.g., Ag+, Cu+, Li+, F–, O2–, H+) in a solid crystalline framework can move as fast as in...

Solid-state batteries with desirable advantages, including high-energy density, wide temperature tolerance, and fewer safety-concerns, have been considered as a promising energy storage technology to replace organic liquid electrolyte-dominated Li-ion batteries. Solid-state electrolytes (SSEs) as the most critical component in solid-state batteries largely lead the future battery development. Among different types of solid-state electrolytes, garnet-type Li7La3Zr2O12 (LLZO) solid-state electrolytes have particularly high ionic conductivity (10-3 to 10-4 S/cm) and good chemical stability against Li metal, offering a great opportunity for solid-state Li-metal batteries. Since the discovery of garnet-type LLZO in 2007, there has been an increasing interest in the development of garnet-type solid-state electrolytes and all solid-state batteries. Garnet-type electrolyte has been considered one of the most promising and important solid-state electrolytes for batteries with potential benefits in energy density, electrochemical stability, high temperature stability, and safety. In this Review, we will survey recent development of garnet-type LLZO electrolytes with discussions of experimental studies and theoretical results in parallel, LLZO electrolyte synthesis strategies and modifications, stability of garnet solid electrolytes/electrodes, emerging nanostructure designs, degradation mechanisms and mitigations, and battery architectures and integrations. We will also provide a target-oriented research overview of garnet-type LLZO electrolyte and its application in various types of solid-state battery concepts (e.g., Li-ion, Li-S, and Li-air), and we will show opportunities and perspectives as guides for future development of solid electrolytes and solid-state batteries.

Summary All-solid-state lithium-metal batteries are regarded as promising next-generation battery systems. While thermal runaway in conventional Li-ion batteries is known to cause safety hazards, the thermal issues posed by highly reactive metallic lithium (Li) with non-flammable ceramic solid electrolytes (SEs) have been less studied but are critical for the safety of all-solid-state Li-metal batteries. Here, we quantify the thermal stability of four prevalent oxide SEs with metallic Li using the accelerating rate calorimeter (ARC). Thermal runaway is observed during ARC tests for four widely used SEs when contacting with Li, while no obvious heat releases from garnet with Li. The oxygen generation from SEs at elevated temperatures is found to be responsible for the thermal runaway with Li. Our results indicate potential safety issues in all solid-state batteries (ASSBs) brought by highly reactive metallic Li and oxygen from SEs at increased temperatures, emphasizing the need for investigating thermal safety issues in ASSBs.

The enabling of high energy density of all-solid-state lithium batteries (ASSLBs) requires the development of highly Li+-conductive solid-state electrolytes (SSEs) with good chemical and electrochemical stability. Recently, halide SSEs based on different material design principles have opened new opportunities for ASSLBs. Here, we discovered a series of LixScCl3+x SSEs (x = 2.5, 3, 3.5, and 4) based on the cubic close-packed anion sublattice with room-temperature ionic conductivities up to 3 × 10-3 S cm-1. Owing to the low eutectic temperature between LiCl and ScCl3, LixScCl3+x SSEs can be synthesized by a simple co-melting strategy. Preferred orientation is observed for all the samples. The influence of the value of x in LixScCl3+x on the structure and Li+ diffusivity were systematically explored. With increasing x value, higher Li+, lower vacancy concentration, and less blocking effects from Sc ions are achieved, enabling the ability to tune the Li+ migration. The electrochemical performance shows that Li3ScCl6 possesses a wide electrochemical window of 0.9-4.3 V vs Li+/Li, stable electrochemical plating/stripping of Li for over 2500 h, as well as good compatibility with LiCoO2. LiCoO2/Li3ScCl6/In ASSLB exhibits a reversible capacity of 104.5 mAh g-1 with good cycle life retention for 160 cycles. The observed changes in the ionic conductivity and tuning of the site occupations provide an additional approach toward the design of better SSEs.

Background: Time in range (TIR) is an emerging metric of glycemic control and is reported to be associated with microvascular complications of diabetes. We sought to investigate the association of ...

The association between β-cell function and glycemic variability remains to be clarified in insulin-treated patients with type 2 diabetes. Therefore, the study sought to examine the association of various indices of β-cell function with glycemic variability in Chinese insulin-treated patients with type 2 diabetes. Glycemic variability was assessed by the coefficient of variation (CV) of glucose levels with the use of continuous glucose monitoring (CGM). Basal β-cell function was evaluated by fasting C-peptide (FCP) and the homeostasis model assessment 2 for β-cell function (HOMA2-%β). Postload β-cell function was measured by 2-hour C-peptide (2hCP) and the acute C-peptide response (ACPR) to arginine. When a cutoff value of CV ≥ 36% was used to define unstable glucose, the multivariable-adjusted odds ratios for labile glycemic control were 0.34 (95% CI 0.18–0.64) for each 1 ng/mL increase in ACPR, 0.47 (95% CI 0.27–0.81) for each 1 ng/mL increase in FCP, 0.77 (95% CI 0.61–0.97) for each 1 ng/mL increase in 2hCP, and 1.00 (95% CI 0.98–1.01) for each 1% increase in HOMA2-%β. When we further adjusted for 2hCP and HOMA2-%β in the ACPR and FCP analyses, and adjusted for ACPR or FCP in the 2hCP analyses, only ACPR but not FCP or 2hPC remained to be a significant and inverse predictor for labile glycemic control. ACPR evaluated by the arginine stimulation test may be superior to other commonly used β-cell function parameters to reflect glycemic fluctuation in insulin-treated patients with type 2 diabetes.

Tremendous efforts have been devoted to the design of solid Li+ electrolytes and the development of all-solid-state batteries. Compared with conventional Li-ion batteries, which use flammable liqui...

Solid electrolyte is the key component in all-solid-state-batteries that is currently limiting the commercialization of this technology. An ideal solid electrolyte should have high room temperature ionic conductivity, low electronic conductivity, good compatibility with both cathode and anode, good mechanical properties, high air and moisture stability and low manufacture cost. Among these requirements, the improvement of ionic conductivity is prioritized as the conductivity of most existing solid electrolyte is still much lower than that of conventional liquid electrolyte. The improvement of ionic conductivity and design and development of solid electrolyte materials are closely related to our understanding on the ionic diffusion mechanism in solids and the structure-property relationship. We believe that rational design of high-performance solid electrolyte should start from careful characterization and good understanding of the crystal structure. Here we report the crystal structure characterization on sulfides and halide solid electrolytes and the design and development of novel solid electrolytes based on our findings in structural characterizations. Ex situ high resolution synchrotron X-ray and neutron diffraction and pair distribution function analysis are used to understand the crystal structures in great details. In situ X-ray diffraction for different synthesis methods is coupled with variable temperature electrochemical impedance spectroscopy to understand the structure-property relationship in the solid electrolytes. The design, synthesis and electrochemical evaluation of several solid electrolytes will be presented and discussed.