Additional Molecules Research Articles

Risk factors for radial artery calcification in patients with and without uremia

BackgroundCalcification of the radial artery is one of the main causes of anastomotic stenosis in autogenous arteriovenous fistulas in uremic patients. However, the pathogenesis of calcification is still unknown. This study attempted to screen and validate the risk factors for vascular calcification in patients with uremia.MethodsSerum of blood were collected and tissue samples from radial artery were obtained from 60 uremia patients with or without hemodialysis. General biochemical indicators and calcification-related molecules were collected and detected via ELISA or correlation analysis. In addition, pathological changes and calcification-related molecules in the radial artery were evaluated by HE or immunohistochemical staining.ResultsThere were differences in total calcium, calcium-phosphorus products, allograft inflammatory factor 1 (AIF-1), intact parathyroid hormone (iPTH), vitamin D (VD), fibroblast growth factor 23 (FGF23) and soluble klotho (sKlotho) in the blood of uremic patients with or without hemodialysis. Furthermore, these factors are related to calcification of the radial artery. The expression of AIF-1, PTHR1, VDR, FGF23 and sKlotho was also increased in the calcified radial artery.ConclusionsThe levels of AIF-1, PTH, VDR, FGF23 and sKlotho in serum were associated with calcification of the radial artery in patients with uremia. Furthermore, calcification of the radial artery was further aggravated by abnormalities in calcium and phosphorus in maintenance hemodialysis patients.

Machine Learning-Assisted High-Donor-Number Electrolyte Additive Screening toward Construction of Dendrite-Free Aqueous Zinc-Ion Batteries.

The utilization of electrolyte additives has been regarded as an efficient strategy to construct dendrite-free aqueous zinc-ion batteries (AZIBs). However, the blurry screening criteria and time-consuming experimental tests inevitably restrict the application prospect of the electrolyte additive strategy. With the rise of artificial intelligence technology, machine learning (ML) provides an avenue to promote upgrading of energy storage devices. Herein, we proposed an intriguing ML-assisted method to accelerate the development efficiency of electrolyte additives on dendrite-free AZIBs. Concretely, we selected the Gutmann donor number (DN value) as a screen parameter, which can reflect the interaction between solvent molecules and ions, and proposed an integrated ML model that can predict the DN values of organic molecules via molecular fingerprints, thereby achieving the screening of electrolyte additives. Then, combined with experimental tests and theoretical calculations, the influence law of three additive molecules with different DN values on the thermodynamic stability of the Zn anode and its corresponding optimization mechanisms were revealed; the DN values of the additives are in positive correlation with the electrochemical performance of the Zn anode. Especially, an isopropyl alcohol (IPA) additive with a high DN value (36) integrated with various Zn-based cells presented a superior electrochemical performance, including a high calendar life (1500 h), a stable Coulombic efficiency (99% within 450 cycles), and a favorable cycling retention. This work pioneers ML techniques for predicting DN values for electrolyte additives, offering a compelling investigation method for the investigation of AZIBs.

Preparation and Structural Properties of Gel Coating Films Containing Lipophilized Nanocarbon Particles Functionalized with Thixotropic Chains.

Gel coating films comprising nanodiamonds organo-modified with 12-hydroxystearic (12-OHC18 ) and stearic acids were prepared and characterized. Because molecules with 12-OHC18 groups can convert solvents into thixotropic gels, Gemini-type diamide derivatives with two 12-OHC18 chains were also introduced as thixotropic additives into the gel coating films. Although the 12-OHC18 -modified nanodiamonds did not lead to solvent gelation on their own, they displayed an affinity for the thixotropic additive molecules. The 12-OHC18 -modified nanodiamonds were localized near the surface of the nanofibers formed by the Gemini-type diamide derivative in the solvent, and the thixotropic properties of the supramolecular gel were confirmed. Nanoparticle aggregation and nanofiber crystallinity were found to be suppressed by the effect of 12-OHC18 modification in the gel coating films, making them suitable for cosmetic coating applications.

A Comprehensive Metabolomic and Microbial Analysis Following Dietary Amino Acid Reduction in Mice.

Introduction: Nutritional metabolomics provides a comprehensive overview of the biochemical processes that are induced by dietary intake through the measurement of metabolite profiles in biological samples. However, there is a lack of deep phenotypic analysis that shows how dietary interventions influence the metabolic state across multiple physiologic sites. Dietary amino acids have emerged as important nutrients for physiology and pathophysiology given their ability to impact cell metabolism. Methods: The aim of the current study is to evaluate the effect of modulating amino acids in diet on the metabolome and microbiome of mice. Here, we report a comprehensive metabolite profiling across serum, liver, and feces, in addition to gut microbial analyses, following a reduction in either total dietary protein or diet-derived non-essential amino acids in mice. Results: We observed both distinct and overlapping patterns in the metabolic profile changes across the three sample types, with the strongest signals observed in liver and serum. Although amino acids and related molecules were the most commonly and strongly altered group of metabolites, additional small molecule changes included those related to glycolysis and the tricarboxylic acid cycle. Microbial profiling of feces showed significant differences in the abundance of select species across groups of mice. Conclusions: Our results demonstrate how changes in dietary amino acids influence the metabolic profiles across organ systems and the utility of metabolomic profiling for assessing diet-induced alterations in metabolism.

Human-in-the-loop active learning for goal-oriented molecule generation

Machine learning (ML) systems have enabled the modelling of quantitative structure–property relationships (QSPR) and structure-activity relationships (QSAR) using existing experimental data to predict target properties for new molecules. These property predictors hold significant potential in accelerating drug discovery by guiding generative artificial intelligence (AI) agents to explore desired chemical spaces. However, they often struggle to generalize due to the limited scope of the training data. When optimized by generative agents, this limitation can result in the generation of molecules with artificially high predicted probabilities of satisfying target properties, which subsequently fail experimental validation. To address this challenge, we propose an adaptive approach that integrates active learning (AL) and iterative feedback to refine property predictors, thereby improving the outcomes of their optimization by generative AI agents. Our method leverages the Expected Predictive Information Gain (EPIG) criterion to select additional molecules for evaluation by an oracle. This process aims to provide the greatest reduction in predictive uncertainty, enabling more accurate model evaluations of subsequently generated molecules. Recognizing the impracticality of immediate wet-lab or physics-based experiments due to time and logistical constraints, we propose leveraging human experts for their cost-effectiveness and domain knowledge to effectively augment property predictors, bridging gaps in the limited training data. Empirical evaluations through both simulated and real human-in-the-loop experiments demonstrate that our approach refines property predictors to better align with oracle assessments. Additionally, we observe improved accuracy of predicted properties as well as improved drug-likeness among the top-ranking generated molecules.Scientific contributionWe present an adaptable framework that integrates AL and human expertise to refine property predictors for goal-oriented molecule generation. This approach is robust to noise in human feedback and ensures that navigating chemical space with human-refined predictors leverages human insights to identify molecules that not only satisfy predicted property profiles but also score highly on oracle models. Additionally, it prioritizes practical characteristics such as drug-likeness, synthetic accessibility, and a favorable balance between exploring diverse chemical space and exploiting similarity to existing training data.

Efferocytosis: the resolution of inflammation in cardiovascular and cerebrovascular disease.

Cardiovascular and cerebrovascular diseases have surpassed cancer as significant global health challenges, which mainly include atherosclerosis, myocardial infarction, hemorrhagic stroke and ischemia stroke. The inflammatory response immediately following these diseases profoundly impacts patient prognosis and recovery. Efficient resolution of inflammation is crucial not only for halting the inflammatory process but also for restoring tissue homeostasis. Efferocytosis, the phagocytic clearance of dying cells by phagocytes, especially microglia and macrophages, plays a critical role in this resolution process. Upon tissue injury, phagocytes are recruited to the site of damage where they engulf and clear dying cells through efferocytosis. Efferocytosis suppresses the secretion of pro-inflammatory cytokines, stimulates the production of anti-inflammatory cytokines, modulates the phenotype of microglia and macrophages, accelerates the resolution of inflammation, and promotes tissue repair. It involves three main stages: recognition, engulfment, and degradation of dying cells. Optimal removal of apoptotic cargo by phagocytes requires finely tuned machinery and associated modifications. Key molecules in efferocytosis, such as 'Find-me signals', 'Eat-me signals', and 'Don't eat-me signals', have been shown to enhance efferocytosis following cardiovascular and cerebrovascular diseases. Moreover, various additional molecules, pathways, and mitochondrial metabolic processes have been identified to enhance prognosis and outcomes via efferocytosis in diverse experimental models. Impaired efferocytosis can lead to inflammation-associated pathologies and prolonged recovery periods. Therefore, this review consolidates current understanding of efferocytosis mechanisms and its application in cardiovascular and cerebrovascular diseases, proposing future research directions.

Ameliorative Potential of Ursolic Acid Isolated from Morina coulteriana Royle Targeting P53 Gene Mutation Induced by Cyclophosphamide

Objective: More than 50% of human cancers show mutated TP53 gene. Reactivation or restoration of p53 mutations is viewed as a potential approach for treating cancer. The objective of the present study was to determine whether ursolic acid (UA) could effectively restore the p53 mutations to their wild type or normal state and upregulate its expression. Methods: The animals were divided into 3 groups, each with 10 mice. Group I was the negative control which received normal saline with 1% dimethyl sulfoxide (DMSO). Group II was the positive control which received cyclophosphamide (CP) (50mg/kg bw) intrapritonealy for 4 days continuously after which the animals were kept on normal saline for the rest 10 days. The treatment group received cyclophosphamide (CP) initially for the first 4 successive days intraperitoneally (50mg/kg bw) and then ursolic acid (UA) (60 mg/kg bw) orally for the next 10 days (post-treatment). Isolated DNA was used in Sanger sequencing of the polymerase chain reaction (PCR) amplified product of the TP53 gene. Results: Our study demonstrated that UA treatment post CP injection had a restoration efficacy of 89.08%. The molecule, in this investigation, was able to restore the wild type (normal) conformation to the mutations induced by cyclophosphamide in the TP53 gene. 89.08 % mutations converted back to their normal or wild-type forms in the treatment group. Conclusion: Several investigations have been carried out on this molecule and have indicated UA as a promising chemopreventive agent. The most frequently mutated gene in any type of cancer is the tumor suppressor p53 and UA has shown a potential in functional restoration of the mutated p53 protein. p53 is known to play a vital role in apoptosis and the p53 dependent apoptotic pathway is of prime importance in cancer therapy. Though there has been pioneering work on PRIMA-1 and thiosemicarbazones, identification and development of additional molecules is required.

Self-Supported Transition Metal Based-Textile Electrodes through Interfacial Assembly for Overall Water Splitting in Alkaline Media

Water splitting holds significant promise for sustainable hydrogen production without carbon emissions. To develop electrodes suitable for large-scale hydrogen generation, characteristics such as large surface area, low electrical resistance, high electrocatalytic activity, and enduring operational stability are paramount. In our investigation, we've engineered high-performance water-splitting electrodes (WSEs) with exceptionally low overpotentials and robust stability through a process integrating carbonization and interfacial assembly-induced electrodeposition. These electrodes feature high-quality electrocatalytic structures based on transition metals (Ni, Fe, and Co), facilitated by strong electronic interactions. They exhibit low sheet resistance akin to bulk metals, a porous 3D architecture with ample specific surface area, and robust interfacial adhesion between the textile-based support and electrocatalysts. Our methodology begins with textiles, transformed into hydrophilic conductive substrates via carbonization and acid treatment, with additional amine molecule incorporation to enhance support-electrocatalyst interactions. Notably, our hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrodes demonstrate extremely low overpotentials (12 mV at 10 mA cm−2 for HER, 186 mV at 50 mA cm−2 for OER) under alkaline conditions. Furthermore, our full-cell electrodes exhibit sustained water-splitting activity at diverse current density from 10 to 2000 mA cm−2 for at least 2100 hours in 1 M KOH solution. We anticipate that our methodology lays a foundational framework for the development of commercially viable, high-performance WSEs.

Fluoroalcohol Additives That Modify the Nature of Solid Electrolyte Interphase and Cathode Electrolyte Interphase Selected By Machine Learning Approach

Inclusion of silicon materials to the negative electrode is seen as a promising approach to realize high-capacity lithium-ion batteries. However, the cycle life of such batteries including silicon materials is limited. The importance of controlling the solid-electrolyte interphase (SEI) has been pointed out for the extended battery life. It has been reported that fluoroethylene carbonate (FEC) and vinylene carbonate (VC) extend the battery life by modifying the nature of SEI. Still, it is difficult to satisfy multiple requirements for commercial batteries (like storage stability and low resistance) with a single additive. Therefore, it is important to expand the options of additive species and to optimize the combination of additives.In this study, a cell consisting of a Si/graphite composite negative electrode is considered, and we explored potential additive candidates that extend the battery life. Candidate additive molecules were selected by machine learning approach, where machine leant models was used for a screening withing a framework of Bayesian optimization that predict a capacity retention rate at a particular cycle be means of the molecular descriptors. In particular, we report a fluoroalcohol material, hexafluoroisopropanol (HFIP) as an additive that improves the cycle performance. Conventionally, the introduction of an alcohol material into the electrolyte has been regarded to promote the generation of hydrogen fluoride (HF) and result in the degradation of cell components such as electrolytes. However, our work found out that such degradation is suppressed when HFIP is included (Figure 1). To study electrochemical and chemical properties of the cell with HFIP, NCA||Si/graphite composite cells were fabricated, and cycle tests were carried out. Afterwards, the cells were dismantled, then the surface of positive and negative electrodes were investigated by XPS. Further characterization was conducted by NMR on the extracted electrolyte and the SEI rinsed individually from positive and negative electrodes. In this presentation, we report the relationship between (1) the chemical aspects of the electrolyte and SEI, and (2) the battery performance, and discuss the key factors that contribute to the improved cycle performance. Figure 1

Enhancing the Interfacial Stability of Li6PS5Cl through Adsorption of Trimethylsilyl Compound-Based Solid Electrolyte Additives

The demand for lithium-ion batteries (LIBs) is increasing due to the rapid expansion of energy storage systems (ESS) and electric vehicles (EVs). However, conventional LIBs raise safety concerns due to the presence of flammable organic solvents in their electrolytes. All-solid-state batteries (ASSBs) are considered state-of-the-art solutions capable of achieving high-energy density while mitigating safety risks. Among these, sulfide-based ASSBs have garnered significant attention owing to exceptional ionic conductivity and mechanical flexibility of sulfide-based solid electrolyte.[1] Nonetheless, the paradigm shift to solid-state battery technology introduces complex solid-solid interfacial side reaction that must be addressed to facilitate the commercialization of sulfide-based ASSBs. This challenge arises from the narrow electrochemical stability window of the sulfide-based solid electrolytes compared to oxide cathode materials, leading to chemical and electrochemical decomposition at the interface.[2] To overcome these inherent obstacles, the development of a chemically and electrochemically stable passivation layer at the interface is imperative.[3] For LIBs containing liquid electrolytes, various electrolyte additives have been commonly utilized to form stable interphases, such as cathode-electrolyte interphase (CEI) on the cathode surface.[4] In particular, electrolyte additives composed of trimethylsilyl functional groups are known to significantly enhance the electrochemical performance of high-voltage cathode materials. Drawing inspiration from this, we have introduced solid electrolyte additives based on trimethylsilyl compounds to improve the interfacial stability between Li6PS5Cl (LPSCl) and LiCoO2. Since solid electrolyte additives cannot dissolve in solid electrolytes, achieving a uniform and thin distribution of the additives is crucial. Additionally, LPSCl undergoes electrochemical decomposition at the surface of carbon additives, underscoring the necessity for a stable passivation layer at the interface between LPSCl and carbon additives.[5] To address these challenges, we aimed to achieve uniform adsorption of a trimethylsilyl-based additive molecule with a thiol functional group, such as 2-(trimethylsilyl)ethanethiol, onto the LPSCl surface through hydrogen bonding and chalcogen-chalcogen interactions.A straightforward solution-based additive adsorption process successfully yields a thin and uniformly coated layer of LPSCl with the additives. The amorphous 2-(trimethylsilyl)ethanethiol (TMS-SH) adsorption layer was approximately a few nanometers thick. TMS-SH underwent electrochemical decomposition at 4.2 V (vs. Li/Li+) during charging, forming a stable silicate-based CEI layer. This stable passivation layer enhanced the electrochemical and chemical stability of the LPSCl surface. Consequently, electrodes utilizing LPSCl adsorbed with TMS-SH demonstrated exceptional cycle life, exceeding 2000 cycles with 85.0% capacity retention after 2000 cycles, and exhibited superior rate capability compared to those utilizing bare LPSCl. This outstanding electrochemical performance stemmed from the stable passivation layer derived from the TMS-SH, which mitigated the interfacial side reactions and effectively suppressed the accumulation of the by-products, such as sulfate, phosphate, and cobalt sulfide. Additionally, TMS-SH enhanced the chemical stability of LPSCl in a dry oxygen atmosphere. Thus, the TMS-SH additive holds promise for sulfide-based solid electrolytes, offering not only in terms of electrochemical performance but also practicality in industry.

Transient transition from Stable to Dissipative Assemblies in Response to the Spatiotemporal Availability of a Chemical Fuel

AbstractThe transition from inactive to active matter implies a transition from thermodynamically stable to energy‐dissipating structures. Here, we show how the spatiotemporal availability of a chemical fuel causes a thermodynamically stable self‐assembled structure to transiently pass to an energy‐dissipating state. The system relies on the local injection of a weak affinity phosphodiester substrate into an agarose hydrogel containing surfactant‐based structures templated by ATP. Injection of substrate leads to the inclusion of additional surfactant molecules in the assemblies leading to the formation of catalytic hotspots for substrate conversion. After the local disappearance of the substrate as a result of chemical conversion and diffusion the assemblies spontaneously return to the stable state, which can be reactivated upon the injection of a new batch of fuel. The study illustrates how a dissipating self‐assembled system can cope with the intermittent availability of chemical energy without compromising long‐term structural stability.

Transient transition from Stable to Dissipative Assemblies in Response to the Spatiotemporal Availability of a Chemical Fuel.

The transition from inactive to active matter implies a transition from thermodynamically stable to energy-dissipating structures. Here, we show how the spatiotemporal availability of a chemical fuel causes a thermodynamically stable self-assembled structure to transiently pass to an energy-dissipating state. The system relies on the local injection of a weak affinity phosphodiester substrate into an agarose hydrogel containing surfactant-based structures templated by ATP. Injection of substrate leads to the inclusion of additional surfactant molecules in the assemblies leading to the formation of catalytic hotspots for substrate conversion. After the local disappearance of the substrate as a result of chemical conversion and diffusion the assemblies spontaneously return to the stable state, which can be reactivated upon the injection of a new batch of fuel. The study illustrates how a dissipating self-assembled system can cope with the intermittent availability of chemical energy without compromising long-term structural stability.

Water Sorption on Isoreticular CPO-27-Type MOFs: From Discrete Sorption Sites to Water-Bridge-Mediated Pore Condensation.

Pore engineering is commonly used to alter the properties of metal-organic frameworks. This is achieved by incorporating different linker molecules (L) into the structure, generating isoreticular frameworks. CPO-27, also named MOF-74, is a prototypical material for this approach, offering the potential to modify the size of its one-dimensional pore channels and the hydrophobicity of pore walls using various linker ligands during synthesis. Thermal activation of these materials yields accessible open metal sites (i.e., under-coordinated metal centers) at the pore walls, thus acting as strong primary binding sites for guest molecules, including water. We study the effect of the pore size and linker hydrophobicity within a series of Ni2+-based isoreticular frameworks (i.e., Ni2L, L = dhtp, dhip, dondc, bpp, bpm, tpp), analyzing their water sorption behavior and the water interactions in the confined pore space. For this purpose, we apply water vapor sorption analysis and Fourier transform infrared spectroscopy. In addition, defect degrees of all compounds are determined by thermogravimetric analysis and solution 1H nuclear magnetic resonance spectroscopy. We find that larger defect degrees affect the preferential sorption sites in Ni2dhtp, while no such indication is found for the other materials in our study. Instead, strong evidence is found for the formation of water bridges/chains between coordinating water molecules, as previously observed for hydrophobic porous carbons and mesoporous silica. This suggests similar sorption energies for additional water molecules in materials with larger pore sizes after saturation of the primary binding sites, resulting in more bulk-like water arrangements. Consequently, the sorption mechanism is driven by classical pore condensation through H-bonding anchor sites instead of sorption at discrete sites.

Molecular Synergistic Effects Mediate Efficient Interfacial Chemistry: Enabling Dendrite-Free Zinc Anode for Aqueous Zinc-Ion Batteries.

The primary cause of the accelerated battery failure in aqueous zinc-ion batteries (AZIBs) is the uncontrollable evolution of the zinc metal-electrolyte interface. In the present research on the development of multiadditives to ameliorate interfaces, it is challenging to elucidate the mechanisms of the various components. Additionally, the synergy among additive molecules is frequently disregarded, resulting in the combined efficacy of multiadditives that is unlikely to surpass the sum of each component. In this study, the "molecular synergistic effect" is employed, which is generated by two nonhomologous acid ester (NAE) additives in the double electrical layer microspace. Specifically, ethyl methyl carbonate (EMC) is more inclined to induce the oriented deposition of zinc metal by means of targeted adsorption with the zinc (002) crystal plane. Methyl acetate (MA) is more likely to enter the solvated shell of Zn2+ and will be profoundly reduced to produce SEI that is dominated by organic components under the "molecular synergistic effect" of EMC. Furthermore, MA persists in a spontaneous hydrolysis reaction, which serves to mitigate the pH increase caused by the hydrogen evolution reaction (HER) and further prevents the formation of byproducts. Consequently, the 1E1M electrolyte not only extends the cycle life of the zinc anode to 3140 cycles (1 mA h cm-2 and 1 mA cm-2) but also extends the life of the Zn//MnO2 full battery, with the capacity retention rate still at 89.9% after 700 cycles.

The Dehydration of Serpentines and Extraction of Water

Some groups of carbonaceous chondrites are dominated by phyllosilicates, specifically the serpentine group, which are characterized as alternating layers of silicates, metal cations, and hydroxyl (OH). Both antigorite, an Mg-rich member, and cronstedtite, an Fe-rich member, can be found in hydrated carbonaceous chondrites. Cronstedtite is found in substantial amounts in CM chondrites. The hydroxyl can make up to a quarter of the molecular mass, and part of it can turn into molecular water through thermal-induced crystal structure breakup. Understanding how the water is released through thermal effects is important for describing the history of certain near-Earth asteroids, as well as for ascertaining the viability of in situ resource utilization (ISRU) for a given object. Here we investigate the temperature of dehydration of the main serpentine constituents of carbonaceous chondrites—antigorite, lizardite, and cronstedtite—under both atmospheric and vacuum conditions. Our results show that the mass loss for cronstedtite starts at about 150 °C lower temperature than for the Mg serpentines. Additionally, vacuum does not affect significantly the onset of the mass loss, but it affects its dynamics. Finally, our observations suggest that cronstedtite loses additional oxygen molecules besides the ones contained within the hydroxyl. These results provide an important new perspective on the orbital history of certain asteroids and the required proximity to the Sun in order for them to lose water. Additionally, it puts the CM-type asteroids on the center stage for ISRU.

Proton transfer driven by the fluctuation of water molecules in chitin film.

Proton-transfer mechanisms and hydration states were investigated in chitin films possessing the functionality of fuel-cell electrolytes. The absolute hydration number per chitin molecule (N) as a function of relative humidity (RH) was determined from the OH stretching bands of H2O molecules, and the proton conductivity was found to enhance above N = 2 (80%RH). The FIR spectrum at 500-900cm-1 for 20%RH (N < 1) together with first-principles calculations clearly shows that the w1 site has the same hydration strength as the w2 site. The molecular dynamics simulations for N = 2 demonstrate that H2O molecules with tiny fluctuations are localized on w1 and w2, and the hydrogen-bond (HB) network is formed via the CH2OH group of chitin molecules. Shrinkage of the O-O distance (dOO), which synchronizes with the barrier height, is required for proton transfer from H3O+ to adjacent CH2OH groups or H2O molecules. Nevertheless, dOO is hardly modulated for N = 2 because H2O molecules are strongly constrained on w1 and w2, and therefore, the transfer probability becomes small. For N = 3, novel HBs emerged between the additional H2O molecules broadly distributed on the w3 site and H2O molecules on w1 and w2. The transfer probability is enhanced because large fluctuations and diffusions in the whole H2O molecule yield large modulations of dOO. Consequently, long-range proton hopping is driven by the Zundel-type protonated hydrates in the water network.

Synthesis of Multifunctional Organic Molecules via Michael Addition Reaction to Manage Perovskite Crystallization and Defect

AbstractAdditive engineering plays a pivotal role in achieving high‐quality light‐absorbing layers for high‐performance and stable perovskite solar cells (PSCs). Various functional groups within the additives exert distinct regulatory effects on the perovskite layer. However, few additive molecules can synergistically fulfill the dual functions of regulating crystallization and passivating defects. Here, we custom‐synthesized 2‐ureido‐4‐pyrimidone (UPy) organic small molecules with diverse functional groups as additives to modulate crystallization and defects in perovskite films via the Michael addition reaction. Theoretical and experimental investigations demonstrate that the −OH groups in UPy exhibit significant effects in fixing uncoordinated Pb2+ ions, passivation of lead‐iodide antisite defects, alleviating hysteresis, and reducing non‐radiative recombination. Furthermore, the enhanced C=O and −NH2 motifs interact with the A‐site cation via hydrogen bonding, which relieves residual strain and adjusts crystal orientation. This strategy effectively controls perovskite crystallization and passivates defects, ultimately enhancing the quality of perovskite films. Consequently, the open‐circuit voltage of the UPy‐based p‐i‐n PSCs reaches 1.20 V, and the fill factor surpasses 84 %. The champion device delivers a power conversion efficiency of 25.75 %. Remarkably, the unencapsulated device maintained 96.9 % and 94.5 % of its initial efficiency following 3,360 hours of dark storage and 1,866 hours of 1‐sun illumination, respectively.

Synthesis of Multifunctional Organic Molecules via Michael Addition Reaction to Manage Perovskite Crystallization and Defect.

Additive engineering plays a pivotal role in achieving high-quality light-absorbing layers for high-performance and stable perovskite solar cells (PSCs). Various functional groups within the additives exert distinct regulatory effects on the perovskite layer. However, few additive molecules can synergistically fulfill the dual functions of regulating crystallization and passivating defects. Here, we custom-synthesized 2-ureido-4-pyrimidone (UPy) organic small molecules with diverse functional groups as additives to modulate crystallization and defects in perovskite films via the Michael addition reaction. Theoretical and experimental investigations demonstrate that the -OH groups in UPy exhibit significant effects in fixing uncoordinated Pb2+ ions, passivation of lead-iodide antisite defects, alleviating hysteresis, and reducing non-radiative recombination. Furthermore, the enhanced C=O and -NH2 motifs interact with the A-site cation via hydrogen bonding, which relieves residual strain and adjusts crystal orientation. This strategy effectively controls perovskite crystallization and passivates defects, ultimately enhancing the quality of perovskite films. Consequently, the open-circuit voltage of the UPy-based p-i-n PSCs reaches 1.20 V, and the fill factor surpasses 84 %. The champion device delivers a power conversion efficiency of 25.75 %. Remarkably, the unencapsulated device maintained 96.9 % and 94.5 % of its initial efficiency following 3,360 hours of dark storage and 1,866 hours of 1-sun illumination, respectively.

Polyelectrolyte Additive-Modulated Interfacial Microenvironment Boosting CO2 Electrolysis in Acid.

Acidic CO2 electrolysis offers a promising strategy to achieve high carbon utilization and high energy efficiency. However, challenges still remain in suppressing the competitive hydrogen evolution reaction (HER) and improving product selectivity. Although high concentrations of potassium ions (K+) can suppress HER and accelerate CO2 reduction, they still inevitably suffer from salt precipitation problems. In this study, we demonstrate that the sulfonate-based polyelectrolyte, polystyrene sulfonate (PSS), enables to reconstruct the electrode-electrolyte interface to significantly enhance the acidic CO2 electrolysis. Mechanistic studies reveal that PSS induces high local K+ concentrations through the electrostatic interaction between PSS anions and K+. In situ spectroscopy reveals that PSS reshapes the interfacial hydrogen-bond (H-bond) network, which is attributed to the H-bonds between PSS anions and hydrated proton, as well as the steric hindrance of the additive molecules. This greatly weakens proton transfer kinetics and leads to the suppression of undesirable HER. As a result, a Faradaic efficiency of 93.9 % for CO can be achieved at 250 mA cm-2, simultaneous with a high single-pass carbon efficiency of 72.2 % on commercial Ag catalysts in acid. This study highlights the important role of the electrode-electrolyte interface induced by polyelectrolyte additives in promoting electrocatalytic reactions.

AI-Driven Electrolyte Additive Selection to Boost Aqueous Zn-Ion Batteries Stability.

In tackling the stability challenge of aqueous Zn-ion batteries (AZIBs) for large-scale energy storage, the adoption of electrolyte additive emerges as a practical solution. Unlike current trial-and-error methods for selecting electrolyte additives, a data-driven strategy is proposed using theoretically computed surface free energy as a stability descriptor, benchmarked against experimental results. Numerous additives are calculated from existing literature, forming a database for machine learning (ML) training. Importantly, this ML model relies solely on experimental values, effectively addressing the challenge of large solvent molecule models that are difficult to handle with quantum chemistry computation. The interpretable linear regression algorithm identifies the number of heavy atoms in the additive molecule and the liquid surface tension as key factors. Artificial intelligence (AI) clustering categorizes additive molecules, identifying regions with the most significant impact on enhancing battery stability. Experimental verification successfully confirms the exceptional performance of 1,2,3-butanetriol and acetone in the optimal region. This integrated methodology, combining theoretical models, data-driven ML, and experimental validation, provides insights into the rational design of battery electrolyte additives.