Deciphering the Roles of Extracellular Polymeric Substances (EPS) in Shaping Disinfection Kinetics through Permanent Removal via Genetic Disruption.

Extracellular polymeric substances (EPS) ubiquitously encapsulate microbes and play crucial roles in various environmental processes. However, understanding their complex interactions with dynamic bacterial behaviors, especially during the disinfection process, remains very limited. In this work, we investigated the impact of EPS on bacterial disinfection kinetics by developing a permanent EPS removal strategy. We genetically disrupted the synthesis of exopolysaccharides, the structural components of EPS, in Pseudomonas aeruginosa, a well-known EPS-producing opportunistic pathogen found in diverse environments, creating an EPS-deficient strain. This method ensured a lasting absence of EPS while maintaining bacterial integrity and viability, allowing for real-time in situ investigations of the roles of EPS in disinfection. Our findings indicate that removing EPS from bacteria substantially lowered their susceptibility threshold to disinfectants such as ozone, chloramine B, and free chlorine. This removal also substantially accelerated disinfection kinetics, shortened the resistance time, and increased disinfection efficiency, thereby enhancing the overall bactericidal effect. The absence of EPS was found to enhance bacterial motility and increase bacterial cell vulnerability to disinfectants, resulting in greater membrane damage and intensified reactive oxygen species (ROS) production upon exposure to disinfectants. These insights highlight the central role of EPS in bacterial defenses and offer promising implications for developing more effective disinfection strategies.

Laccase-induced decontamination and humification mechanisms of estrogen in water-crop matrices.

Enzymatic humification plays a crucial biogeochemical role in eliminating steroidal estrogens and expanding organic carbon stocks. Estrogenic contaminants in agroecosystems can be taken up and acropetally translocated by crops, but the roles of laccase-triggered rhizospheric humification (L-TRH) in pollutant dissipation and plant uptake remain poorly understood. In this study, the laccase-induced decontamination and humification mechanisms of 17ß-estradiol (E2) in water-crop media were investigated by performing greenhouse pot experiments with maize seedlings (Zea mays L.). The results demonstrated that L-TRH effectively dissipated E2 in the rhizosphere solution and achieved the kinetic constants of E2 dissipation at 10 and 50 µM by 8.05 and 2.75 times as much as the treatments without laccase addition, respectively. The copolymerization of E2 and root exudates (i.e. phenols and amino acids) consolidated by L-TRH produced a larger amount of humified precipitates with the richly functional carbon architectures. The growth parameters and photosynthetic pigment levels of maize seedlings were greatly impeded after a 120-h exposure to 50 µM E2, but L-TRH motivated the detoxication process and thus mitigated the phytotoxicity and bioavailability of E2. The tested E2 contents in the maize tissues initially increased sharply with the cultivation time but decreased steadily. Compared with the treatment without laccase addition, the uptake and accumulation of E2 in the maize tissues were obviously diminished by L-TRH. E2 oligomers such as dimer, trimer, and tetramer recognized in the rhizosphere solution were also detected in the root tissues but not in the shoots, demonstrating that the acropetal translocation of E2 oligomers was interrupted. These results highlight a promising strategy for decontaminating estrogenic pollutants, boosting rhizospheric humification, and realizing low-carbon emissions, which would be beneficial for agroenvironmental bioremediation and sustainability.

Tailoring d-band center of high-valent metal-oxo species for pollutant removal via complete polymerization.

Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d-band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding strength for peroxymonosulfate through d-band center modulation. A 100% polymerization transfer ratio is achieved by lowering the d-band center. This work presents a paradigm to dynamically modulate the electronic structure of high-valent metal-oxo species and optimize pollutant removal from wastewater via polymerization.

Age- and Gender-Specific Reference Intervals for the Fasting Serum Lipid Levels in a Pediatric Population Aged 0-＜15 Years in Nanjing, China.

AIMS: The lipid reference intervals (RIs) that are currently used for children in China are not based on studies of the local population and normally do not consider age or gender differences. This study aimed to establish age- and sex-specific RIs for the fasting serum lipid levels in the pediatric population aged 0 - 15 years in Nanjing, China. METHODS: 5,866 children aged 3 days to ＜15 years were recruited to establish serum lipid RIs, and the triglyceride (TG), total cholesterol (TC), and high-density lipoprotein cholesterol (HDL-C) levels were analyzed using the Roche cobas702 automatic biochemical analyzer. Low-density lipoprotein cholesterol (LDL-C) and non-high-density lipoprotein cholesterol (nHDL-C) levels were calculated (LDL-C=TC-HDL-C-TG/5, and nHDL-C=TC-HDL-C). Smoothed percentile curves for the boys and girls were generated using the LMS method. Age- and sex-specific RIs were the determined according to the methods recommended by the Clinical and Laboratory Standards Institute EP28-A3c guidelines. RESULTS: This study showed that the serum lipid levels varied considerably throughout childhood and adolescence, with sex differences, especially in infants aged less than 2 years and puberty. Based on the Harris-Boyd method, sex partitions were required for ages ＜6 months in the TC indicator and for ages ≤ 28 days in LDL-C and nHDL-C. Age partitions were also required for all serum lipid parameters. CONCLUSIONS: We established age- and sex-specific RIs for TG, TC, HDL-C, LDL-C, and nHDL-C parameters in children aged 0 days to ＜15 years in Nanjing, China. These data are thus considered to be useful for the screening of dyslipidemia in children and adolescents.

Unexpected side reactions dominate the oxidative transformation of aromatic amines in the Co(II)/peracetic acid system.

Aromatic amines (AAs), ubiquitous in industrial applications, pose significant environmental hazards due to their resistance to conventional wastewater treatments. Peracetic acid (PAA)-based advanced oxidation processes (AOPs) have been proposed as effective strategies for addressing persistent AA contaminants. While the organic radicals generated in these systems are believed to be selective and highly oxidative, acetate residue complicates the evaluation of AA removal efficiency. In this work, we explored transformation pathways of AAs in a representative Co(II)-catalyzed PAA system, revealing five side reactions (i.e. nitrosation, nitration, coupling, dimerization, and acetylation) that yield 17 predominantly stable and toxic by-products. The dominant reactive species was demonstrated as Co-OOC(O)CH3, which hardly facilitated ring-opening reactions. Our findings highlight the potential risks associated with PAA-based AOPs for AA degradation and provide insights into selecting suitable catalytic systems aimed at efficient and by-product-free degradation of pollutants containing aromatic -NH2.

Land management policy shift influenced seasonal variation of erosion-induced nitrogen and phosphorus outputs from intensive agricultural catchment.

A shift in policy to intensive agricultural production and land management often leads to excessive fertilizer application and accelerated erosion with consequent detrimental effects to water bodies. We investigated the impact of that shift by quantifying the spatial and temporal change in sediment sources and associated total nitrogen (TN) and total phosphorus (TP) pollutants output loads in an intensive agricultural catchment in North China across one year (November 2021-November 2022). We describe the implications of this work for intensive agriculture elsewhere in China and other countries. Seasonal sediment source apportionment was estimated at the catchment outlet using Berillium-7 (7Be) combined with compound-specific stable isotope (CSSI) signatures from sources and sediments. Diagnostic 'fingerprints' in MixSIAR were used to discriminate sediment sources between forest and crop farmland converted from forest (F + C(F)), crop farmland (C), and vegetable farmland (V). Our study identified F + C(F) as the dominant sediment source (mean 55.24 ± 2.91 %), intermediate on V (mean 30.06 ± 2.20 %), and least on C (mean 14.70 ± 2.13 %). Sedimentation ranged from 37.98 ± 3.02 to 89.60 ± 12.68 t·ha-1·event-1 and coincided with shifted land use policy and rainfall distribution. The TN and TP in sediment were both mainly derived from F + C(F) (averaged 22.27 ± 4.26 t·event-1 and 11.62 ± 2.28 t·event-1) and least from V (averaged 1.63 ± 0.29 and 2.09 ± 0.33 t·event-1). Despite being a significant sediment source, V contributed little sediment TN and TP input for eutrophication. Our findings imply that F + C(F) are diffuse sources of catchment pollution over the short term. These results describe the successful use of CSSI and 7Be to cost-effectively quantify the seasonal variation of sediment TN and TP loads from land-use-specific sources in the catchment under shifting land management policy in China with potential for use elsewhere. These findings enable soil conservation strategies and land management practices optimized for implementing targeted pollutant abatement initiatives in intensive agriculture in China and elsewhere.

Reduced Lattice Constant in Al-Doped LiMn2O4 Nanoparticles for Boosted Electrochemical Lithium Extraction.

Extracting lithium selectively and efficiently from brine sources is crucial for addressing energy and environmental challenges. The electrochemical system employing LiMn2O4 (LMO) electrodes has been recognized as an effective method for lithium recovery. However, the lithium selectivity and stability of LMO need further enhancement for its practical applications. Herein, the Al-doped LMO with reduced lattice constant is successfully fabricated through a facile one-step solid-state sintering method, leading to enhanced lithium selectivity. The reduced lattice constant in Al-doped LMO is proved through spectroscopic analyses and theoretic calculations. Compared to the original LMO, the Al-doped LMO (LiAl0.05Mn1.95O4, LMO-Al0.05) exhibits highercapacitance, lower resistance, and improved stability. Moreover, the LMO-Al0.05 with reduced lattice constant can offer higher Li+ diffusion coefficient and lower intercalation energy revealed by cyclic voltammetry and multiscale simulations. When employed in hybrid capacitive deionization (CDI), the LMO-Al0.05 obtains a Li+ intercalation capacity of 21.7 mg g-1 and low energy consumption of 2.6 Wh mol-1 Li+. Importantly, the LMO-Al0.05 achieves a high Li+ extraction percentage (≈86%) with Li+/Na+ and Li+/Mg2+ selectivity of 1653.8 and 434.9, respectively, in synthetic brine. The results demonstrate that the Al-doped LMO with reduced lattice constant could be a sustainable solution for electrochemical lithium extraction.

Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production.

Direct electrosynthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction presents a burgeoning alternative to the conventional energy-intensive anthraquinone process for on-site applications. Nevertheless, its adoption is currently hindered by inferior H2O2 selectivity and diminished H2O2 yield induced by consecutive H2O2 reduction or Fenton reactions. Herein, guided by theoretical calculations, we endeavor to overcome this challenge by activating a main-group Pb single-atom catalyst via a local micro-environment engineering strategy employing a sulfur and oxygen super-coordinated structure. The main-group catalyst, synthesized using a carbon dot-assisted pyrolysis technique, displays an industrial current density reaching 400 mA cm-2 and elevated accumulated H2O2 concentrations (1358 mM) with remarkable Faradaic efficiencies. Both experimental results and theoretical simulations elucidate that S and O super-coordination directs a fraction of electrons from the main-group Pb sites to the coordinated oxygen atoms, consequently optimizing the *OOH binding energy and augmenting the 2e- oxygen reduction activity. This work unveils novel avenues for mitigating the production-depletion challenge in H2O2 electrosynthesis through the rational design of main-group catalysts.

Embedding electronic perpetual motion into single-atom catalysts for persistent Fenton-like reactions.

In our quest to leverage the capabilities of the emerging single-atom catalysts (SACs) for wastewater purification, we confronted fundamental challenges related to electron scarcity and instability. Through meticulous theoretical calculations, we identified optimal placements for nitrogen vacancies (Nv) and iron (Fe) single-atom sites, uncovering a dual-site approach that significantly amplified visible-light absorption and charge transfer dynamics. Informed by these computational insights, we cleverly integrated Nv into the catalyst design to boost electron density around iron atoms, yielding a potent and flexible photoactivator for benign peracetic acid. This exceptional catalyst exhibited remarkable stability and effectively degraded various organic contaminants over 20 cycles with self-cleaning properties. Specifically, the Nv sites captured electrons, enabling their swift transfer to adjacent Fe sites under visible light irradiation. This mechanism accelerated the reduction of the formed "peracetic acid-catalyst" intermediate. Theoretical calculations were used to elucidate the synergistic interplay of dual mechanisms, illuminating increased adsorption and activation of reactive molecules. Furthermore, electron reduction pathways on the conduction band were elaborately explored, unveiling the production of reactive species that enhanced photocatalytic processes. A six-flux model and associated parameters were also applied to precisely optimize the photocatalytic process, providing invaluable insights for future photocatalyst design. Overall, this study offers a molecule-level insight into the rational design of robust SACs in a photo-Fenton-like system, with promising implications for wastewater treatment and other high-value applications.

Serum uric acid levels and health outcomes in CKD: a prospective cohort study.

BACKGROUND: Hyperuricemia is prevalent in individuals with chronic kidney disease (CKD). Elevated serum uric acid (SUA) concentrations have been considered an independent risk factor for the onset of CKD. However, the relationship between SUA concentrations and long-term health outcomes among patients with CKD remains unclear. METHODS: We performed a prospective cohort study with nationally representative sample to investigate the relationship between SUA concentrations and mortality risk including all-cause, cardiovascular disease (CVD) and cancer mortality, among patients with CKD. The weighted restricted cubic spline analyses combined with the multivariate-adjusted Cox proportional hazard models were used to test the nonlinearity of relationship. RESULTS: The 6642 patients participating in National Health and Nutrition Examination Survey 1999-2018 were enrolled. During 656 885 person-months of follow-up time, 2619 all-cause deaths were recorded, including 1030 CVD deaths and 458 cancer deaths. Our study presented J-shaped non-linear relationships between SUA concentrations and all-cause and CVD mortality with inflection points at 311.65 µmol/L and 392.34 µmol/L, respectively. When SUA concentration was higher than those inflection points, every increase of 50 µmol/L SUA was associated with 11.7% and 17.0% greater multivariable-adjusted hazard ratio of all-cause and CVD mortality, respectively. In addition, a negative linear correlation with cancer mortality was detected. CONCLUSION: These findings suggested that maintaining appropriate SUA concentrations may improve long-term health outcomes among CKD patients. The corresponding inflection points of J-shaped non-linear relationships were 311.65 and 392.34 µmol/L for all-cause and CVD mortality. Further clinical trials are required to investigate uric acid-lowering targets.

Single-cell transcriptomics reveals variations in monocytes and Tregs between gout flare and remission.

Gout commonly manifests as a painful, self-limiting inflammatory arthritis. Nevertheless, the understanding of the inflammatory and immune responses underlying gout flares and remission remains ambiguous. Here, based on single-cell RNA-Seq and an independent validation cohort, we identified the potential mechanism of gout flare, which likely involves the upregulation of HLA-DQA1+ nonclassical monocytes and is related to antigen processing and presentation. Furthermore, Tregs also play an essential role in the suppressive capacity during gout remission. Cell communication analysis suggested the existence of altered crosstalk between monocytes and other T cell types, such as Tregs. Moreover, we observed the systemic upregulation of inflammatory and cytokine genes, primarily in classical monocytes, during gout flares. All monocyte subtypes showed increased arachidonic acid metabolic activity along with upregulation of prostaglandin-endoperoxide synthase 2 (PTGS2). We also detected a decrease in blood arachidonic acid and an increase in leukotriene B4 levels during gout flares. In summary, our study illustrates the distinctive immune cell responses and systemic inflammation patterns that characterize the transition from gout flares to remission, and it suggests that blood monocyte subtypes and Tregs are potential intervention targets for preventing recurrent gout attacks and progression.

The neglected ammonia leaching calcium in anaerobic granular sludge.

Previous researches have primarily emphasized the deleterious impacts of NH4+ on anaerobic granular sludge due to its biotoxicity. Despite this, the role of NH4+ as a monovalent cation in leaching multivalent Ca2+, thereby hindering granule formation and undermining its stability, remains underappreciated. This study investigated the potential of NH4+ to leach Ca2+ from anaerobic granular sludges. The results indicated that a shock loading of NH4+ at a concentration of 900 mg/L caused a Ca2+ leaching of 57.1 mg/L at pH 7.0. In an acidified environment (pH 5.0), the shock loading resulted in a Ca2+ release of 127.3 mg/L, a magnitude 5.24 times greater than the control group. The leaching process modestly affected granular sludge activity and size but markedly compromised granular strength due to calcium loss. Subsequent to the NH4+ shock, the granular strength manifested a significant reduction, as evidenced by a 15-fold increase in protein release from the granules compared to the intact ones. Additionally, NH4+ shock altered the calcium partitioning within the granular sludge, resulting in a decrease in residual calcium and a concomitant increase in bound calcium, further affecting granular strength. This study underscores the overlooked significant phenomenon of NH4+ shock-leaching Ca2+ in anaerobic granular sludge, which warrants significant attention given to its rapid and deleterious effects on granular strength and the shift in calcium state.

Recycling Coal Fly Ash for Super-Thermal-Insulating Aerogel Fiber Preparation with Simultaneous Al2O3 Extraction.

A large quantity of coal fly ash is generated worldwide from thermal power plants, causing a serious environmental threat owing to disposal and storage problems. In this work, for the first time, coal fly ash is converted into advanced and novel aerogel fibers and high-purity α-Al2O3. Silica-bacterial cellulose composite aerogel fibers (CAFs) were synthesized using an in situ sol-gel process under ambient pressure drying. Due to the unique "nanoscale interpenetrating network" (IPN) structure, the CAFs showed wonderful mechanical properties with an optimum tensile strength of 5.0 MPa at an ultimate elongation of 5.8%. Furthermore, CAFs with a high porosity (91.8%) and high specific surface area (588.75 m2/g) can inherit advanced features, including excellent thermal insulation, stability over a wide temperature range, and hydrophobicity (contact angle of approximately 144°). Additionally, Al2O3 was simultaneously extracted from the coal fly ash to ensure that the coal fly ash was fully exploited. Overall, low-cost woven CAFs fabrics are suitable for wearable applications and offer a great approach to comprehensively use coal fly ash to address environmental threats.

Unraveling heterogeneity of dissolved organic matter in highly connected natural water bodies at molecular level.

The exploring of molecular-level heterogeneity of dissolved organic matter (DOM) in highly connected water bodies is of great importance for pollution tracing and lake management, and provides new perspectives on the transformations and fate of DOM in aquatic systems. However, the inherent homogeneity of DOM in connected water bodies poses challenges for its heterogeneity analysis. In this work, an innovative method combining fluorescence spectroscopy, high-resolution mass spectrometry (HRMS), and cluster analysis was developed to reveal the heterogeneity of DOM in highly connected water bodies at the molecular level. We detected 4538 molecules across 36 sampling sites in Chaohu Lake using HRMS. Cluster analysis based on excitation-emission matrix (EEM) data effectively divided the sampling sites into four clusters, representing the water bodies from West Chaohu Lake, East Chaohu Lake, agricultural land, and urban areas. Analysis of DOM in the western and eastern parts of the lake revealed that aerobic degradation led to a decrease in CHOS and aliphatic compounds, alongside an increase in CHO and highly unsaturated and phenolic compounds. Furthermore, we unveiled the characteristics and sources of heterogeneity in DOM from agricultural land and urban areas. Our method accurately captured the heterogeneous distribution of DOM in the lake and revealed the heterogeneous composition of DOM at molecular level. This work underscores the importance of integrating complementary spectroscopic analyses with HRMS in DOM research with similar compositions.

Re-evaluation and modification of dehydrogenase activity tests in assessing microbial activity for wastewater treatment plant operation.

Reliable and cost-effective methods for monitoring microbial activity are critical for process control in wastewater treatment plants. The dehydrogenase activity (DHA) test has been recognized as an efficient measure of biological activity due to its simplicity and broad applicability. Nevertheless, the existing DHA test methods suffer from imperfections and are difficult to implement as routine monitoring techniques. In this work, an accurate and cost-effective modified DHA approach was developed and the procedure for the DHA test was critically evaluated with respect to the standard construction, sample pretreatment, incubation and extraction conditions. The feasibility of the modified DHA test was demonstrated by comparison with the oxygen uptake rate and adenosine triphosphate in a sequencing batch reactor. The sensitivities of the two typical tetrazolium salts to toxicant inhibition by heavy metals and antibiotics were compared, revealing that 2,3,5-triphenyltetrazolium chloride (TTC) exhibited a higher sensitivity. Furthermore, the sensitivity mechanism of the two DHA tests was elucidated through electrochemical experiments, theoretical analysis and molecular simulations. Both tetrazolium salts were found to be effective artificial electron acceptors due to their low redox potentials. Molecular docking simulations revealed that TTC could outperform other tetrazolium salts in accepting electrons and hydrogens from dehydrogenase. Overall, the modified DHA approach presents an accurate and cost-effective way to measure microbial activity, making it a practical tool for wastewater treatment plants.

Slow-release synthesis of Cu single-atom catalysts with the optimized geometric structure and density of state distribution for Fenton-like catalysis.

Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure-performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure-reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.

Molecular insights into complexation between protein and silica: Spectroscopic and simulation investigations.

The synergistic effect of protein-silica complexation leads to exacerbated membrane fouling in the membrane desalination process, exceeding the individual impacts of silica scaling or protein fouling. However, the molecular-level dynamics of silica binding to proteins and the resulting structural changes in both proteins and silica remain poorly understood. This study investigates the complexation process between silica and proteins-negatively charged bovine serum albumin (BSA) and positively charged lysozyme (LYZ) at neutral pH-using infrared spectroscopy (IR), in situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and multiple computational simulations. The findings reveal that both protein and silica structures undergo changes during the complexation process, with calcium ions in the solution significantly exacerbating these alterations. In particular, in situ ATR-FTIR combined with two-dimensional correlation spectroscopy analysis shows that BSA experiences more pronounced unfolding, providing additional binding sites for silica adsorption compared to LYZ. The adsorbed proteins promote silica polymerization from lower-polymerized to higher-polymerized species. Furthermore, molecular dynamics simulations demonstrate greater conformational variation in BSA through root-mean-square-deviation analysis and the bridging role of calcium ions via mean square displacement analysis. Molecular docking and density functional theory calculations identify the binding sites and energy of silica on proteins. In summary, this research offers a comprehensive understanding of the protein-silica complexation process, contributing to the knowledge of synergistic behaviors of inorganic scaling and organic fouling on membrane surfaces. The integrated approach used here may also be applicable for exploring other complex complexation processes in various environments.

MSU crystal deposition contributes to inflammation and immune responses in gout remission.

As a prominent feature of gout, monosodium urate (MSU) crystal deposition induces gout flares, but its impact on immune inflammation in gout remission remains unclear. Using single-cell RNA sequencing (scRNA-seq), we characterize the transcription profiling of peripheral blood mononuclear cells (PBMCs) among intercritical remission gout, advanced remission gout, and normal controls. We find systemic inflammation in gout remission with MSU crystal deposition at the intercritical and advanced stages, evidenced by activated inflammatory pathways, strengthened inflammatory cell-cell interactions, and elevated arachidonic acid metabolic activity. We also find increased HLA-DQA1high classic monocytes and PTGS2high monocytes in advanced gout and overactivated CD8+ T cell subtypes in intercritical and advanced gout. Additionally, the osteoclast differentiation pathway is significantly enriched in monocytes, T cells, and B cells from advanced gout. Overall, we demonstrate systemic inflammation and distinctive immune responses in gout remission with MSU crystal deposition, allowing further exploration of the underlying mechanism and clinical significance in conversion from intercritical to advanced stage.

Lithium-ion battery multi-scale modeling coupled with simplified electrochemical model and kinetic Monte Carlo model.

The multi-scale modeling of lithium-ion battery (LIB) is difficult and necessary due to its complexity. However, it is difficult to capture the aging behavior of batteries, and the coupling mechanism between multiple scales is still incomplete. In this paper, a simplified electrochemical model (SEM) and a kinetic Monte Carlo (KMC)-based solid electrolyte interphase (SEI) film growth model are used to study the multi-scale characteristics of LIBs. The single-particle SEM (SP-SEM) is described for macro scale, and a simple and self-consistent multi-particle SEM (MP-SEM) is developed. Then, the KMC-based SEI model is established for micro-scale molecular evolution. And, the two models are coupled to construct the full-cycle multi-scale model. After modeling, validation is performed by using a commercial 18650-type LIB. Finally, the effect of parameters on the SEI model is studied, including qualitative trend analysis and quantitative sensitivity analysis. The growth of SEI film with different particle sizes is studied by MP-SEM coupling simulation.