Approach to hyperuniformity in a metallic glass-forming material exhibiting a fragile to strong glass transition.

We investigate a metallic glass-forming (GF) material (Al90Sm10) exhibiting a fragile-strong (FS) glass-formation by molecular dynamics simulation to better understand this highly distinctive pattern of glass-formation in which many of the usual phenomenological relations describing relaxation times and diffusion of ordinary GF liquids no longer apply, and where instead genuine thermodynamic features are observed in response functions and little thermodynamic signature is exhibited at the glass transition temperature, Tg. Given the many unexpected similarities between the thermodynamics and dynamics of this metallic GF material with water, we first focus on the anomalous static scattering in this liquid, following recent studies on water, silicon and other FS GF liquids. We quantify the "hyperuniformity index" H of our liquid, which provides a quantitative measure of molecular "jamming". To gain insight into the T-dependence and magnitude of H, we also estimate another more familiar measure of particle localization, the Debye-Waller parameter 〈u2〉 describing the mean-square particle displacement on a timescale on the order of the fast relaxation time, and we also calculate H and 〈u2〉 for heated crystalline Cu. This comparative analysis between H and 〈u2〉 for crystalline and metallic glass materials allows us to understand the critical value of H on the order of 10-3 as being analogous to the Lindemann criterion for both the melting of crystals and the "softening" of glasses. We further interpret the emergence of FS GF and liquid-liquid phase separation in this class of liquids to arise from a cooperative self-assembly process in the GF liquid.

Validity of Actigraph for Measuring Energy Expenditure in Healthy Adults: A Systematic Review and Meta-Analysis.

PURPOSE: The objective of this systematic review and meta-analysis was to assess the validity of the Actigraph triaxial accelerometer device in measuring physical activity energy expenditure (PAEE) in healthy adults, with indirect calorimetry (IC) serving as the validity criterion. METHODS: A comprehensive search was conducted using the PubMed, Web of Science, and sportdiscuss databases, in addition to manual searches for supplementary sources. Search strategies were employed that involved conducting single keyword searches using the terms "gt3x" and "Actigraph gt3x". The literature search encompassed the timeframe spanning from 1 January 2010 to 1 March 2023. The methodological quality of the studies included in the analysis was evaluated using both the Downs and Black checklist and the Consensus-Based Criteria for Selection of Measurement Instruments (COSMIN) checklist. The meta-analysis was conducted using the Review Manager 5.4 software. The standardized mean difference (SMD) was calculated and expressed as a 95% confidence interval (CI). The significance level was set at α = 0.05. A systematic assessment of the Actigraph's performance was conducted through the descriptive analysis of computed effect sizes. RESULTS: A total of 4738 articles were retrieved from the initial search. After eliminating duplicate articles and excluding those deemed irrelevant, a comprehensive analysis was conducted on a total of 20 studies, encompassing a combined sample size of 1247 participants. The scores on the Downs and Black checklist ranged from 10 to 14, with a mean score of 11.35. The scores on the COSMIN checklist varied from 50% to 100%, with an average score of 65.83%. The meta-analysis findings revealed a small effect size (SMD = 0.01, 95% CI = 0.50-0.52, p = 0.97), indicating no statistically significant difference (p > 0.05). CONCLUSIONS: The meta-analysis revealed a small effect size when comparing the Actigraph and IC, suggesting that the Actigraph can be utilized for assessing total PAEE. Descriptive analyses have indicated that the Actigraph device has limited validity in accurately measuring energy expenditure during specific physical activities, such as high-intensity and low-intensity activities. Therefore, caution should be exercised when utilizing this device for such purposes. Furthermore, there was a significant correlation between the activity counts measured by the Actigraph and the PAEE, indicating that activity counts can be utilized as a predictive variable for PAEE.

Synergistic Stimulation of Metal-Organic Frameworks for Stable Super-cooled Liquid and Quenched Glass.

Metal-organic framework (MOF) glasses are a fascinating new class of materials, yet their prosperity has been impeded by the scarcity of known examples and limited vitrification methods. In the work described in this report, we applied synergistic stimuli of vapor hydration and thermal dehydration to introduce structural disorders in interpenetrated dia-net MOF, which facilitate the formation of stable super-cooled liquid and quenched glass. The material after stimulus has a glass transition temperature (Tg) of 560 K, far below the decomposition temperature of 695 K. When heated, the perturbed MOF enters a super-cooled liquid phase that is stable for a long period of time (>104 s), across a broad temperature range (26 K), and has a large fragility index of 83. Quenching the super-cooled liquid gives rise to porous MOF glass with maintained framework connectivity, confirmed by EXAFS and PDF analysis. This method provides a fundamentally new route to obtain glassy materials from MOFs that cannot be melted without causing decomposition.

Vibration assisted glass-formation in zeolitic imidazolate framework.

A new glass forming method is essential for broadening the scope of liquid and glassy metal-organic frameworks due to the limitations of the conventional melt-quenching method. Herein, we show that in situ mechanical vibration can facilitate the framework melting at a lower temperature and produce glassy metal-organic frameworks (MOFs) with unique properties. Using zeolitic imidazolate framework (ZIF)-62 as a concept-proofing material, in situ mechanical vibration enables low-temperature melting at 653 K, far below its melting point (713 K). The resultant vibrated ZIF-62 glass exhibited a lower glass transition temperature of 545 K, improved gas accessible porosity, and pronounced short-to-medium range structures compared to the corresponding melt-quenched glass. We propose that vibration-facilitated surface reconstruction facilitates pre-melting, which could be the cause of the lowered melting temperature. The vibration assisted method represents a new general method to produce MOF glasses without thermal decomposition.

Structural length-scale of ß relaxation in metallic glass.

Establishing the structure-property relationship is an important goal of glassy materials, but it is usually impeded by their disordered structure and non-equilibrium nature. Recent studies have illustrated that secondary (ß) relaxation is closely correlated with several properties in a range of glassy materials. However, it has been challenging to identify the pertinent structural features that govern it. In this work, we show that the so-called polyamorphous transition in metallic glasses offers an opportunity to distinguish the structural length scale of ß relaxation. We find that, while the glass transition temperature and medium-range orders (MROs) change rapidly across the polyamorphous transition, the intensity of ß relaxation and the short-range orders (SROs) evolve in a way similar to those in an ordinary reference glass without polyamorphous transition. Our findings suggest that the MRO accounts mainly for the global stiffening of the materials and the glass transition, while the SRO contributes more to ß relaxation per se.

Metallic Nanoglasses with Promoted ß-Relaxation and Tensile Plasticity.

The secondary (ß) relaxation is an intrinsic feature of glassy systems and is crucial for the mechanical properties of metallic glasses. However, it remains puzzling what structural features control the ß-relaxation fundamentally. Here, we use the recently developed nanoglasses exhibiting well-defined structural features at the nanometer scale to interrogate such structure-dynamics relations. We show that an electrodeposited Ni77.5P22.5 nanoglass exhibits promoted ß-relaxation and enhanced microscale tensile plasticity over the most rapidly melt-quenched metallic glass with the same composition. Structurally, the ß-relaxation is sensitive to the interfacial regions among grains in the nanoglasses. Our results reveal a clear correlation between the amorphous nanostructures and the ß-relaxation. It seems that the nanostructuring represents a novel route to obtain high-energy glassy states, that is, the inverse problem of the ultrastable glass.

Immune responses and pathogenesis in persistently PCR-positive patients with SARS-CoV-2 infection.

Coronavirus disease 2019 (COVID-19) caused by severe acute respiratory syndrome coronavirus 2 emerged in China in December 2019 and then rapidly spread worldwide. Why COVID-19 patients with the same clinical condition have different outcomes remains unclear. This study aimed to examine the differences in the phenotype and functions of major populations of immune cells between COVID-19 patients with same severity but different outcomes. Four common type adult inpatients with laboratory confirmed COVID-19 from Beijing YouAn Hospital, Capital Medical University were included in this study. The patients were divided into two groups based on whether or not COVID-19 polymerase chain reaction (PCR)-negative conversion occurred within 3 weeks. Peripheral blood samples were collected to compare the differences in the phenotype and functions of major populations of immune cells between the two groups of patients. The result shows that the proportions of CD3+ CD8+ CD38+ HLA-DR+ CD27- effector T killer cells generally declined, whereas that of CD3+ CD4+ CD8+ double-positive T cells (DPTs) increased in the persistently PCR-positive patients. In summary, considering the imbalance between effector T killer cells/CD3+CD4+CD8+ DPTs was a possible key factor for PCR-negative conversion in patients with COVID-19.

Association of HSD17B13 rs72613567: TA allelic variant with liver disease: review and meta-analysis.

BACKGROUND: To assess the association of HSD17B13 rs72613567:TA allelic variant with liver disease, we performed the current review and meta-analysis. METHODS: Seven studies were identified by a search of CNKI,CBM,MEDLINE, PubMed, EMBASE, and CENTRAL databases from inception to November 2021. Odds ratios (ORs) with 95% confidence interval (CI) were calculated using random effects model or fixed effects model based on the between-study heterogeneity. The Stata 14.0 software was employed for data analysis. RESULTS: Statistical analysis showed that the HSD17B13 rs72613567:TA allelic variant can decrease the risk of hepatocellular carcinoma(HCC) in nonalcoholic fatty liver disease (NAFLD) patients, alcoholic fatty liver disease (ALD) patients and viral hepatitis patients (TA vs T OR = 0.766, 95% CI = 0.682-0.860, P = 0.000; TATA + TAT vs TT OR = 0.755, 95% CI = 0.645-0.885, P = 0.001) or healthy controls(TA vs T OR = 0.649, 95% CI = 0.431-0.977, P = 0.038). Besides, the HSD17B13 rs72613567:TA allelic variant can also provide protection from nonalcoholic fatty liver disease (NAFLD) not only in entire population (TA vs T OR = 0.669, 95% CI = 0.524-0.856, P = 0.001) but also in healthy people (TA vs T OR = 0.600, 95% CI = 0.464-0.777, P = 0.000). No significant publication bias found in this airticle. CONCLUSION: The present findings suggest HSD17B13 rs72613567:TA allelic variant can reduce the risk of HCC and NAFLD in the entire population studied.

Dynamic heterogeneity, cooperative motion, and Johari-Goldstein [Formula: see text]-relaxation in a metallic glass-forming material exhibiting a fragile-to-strong transition.

We investigate the Johari-Goldstein (JG) [Formula: see text]-relaxation process in a model metallic glass-forming (GF) material ([Formula: see text]), previously studied extensively by both frequency-dependent mechanical measurements and simulation studies devoted to equilibrium properties, by molecular dynamics simulations based on validated and optimized interatomic potentials with the primary aim of better understanding the nature of this universal relaxation process from a dynamic heterogeneity (DH) perspective. The present relatively low temperature and long-time simulations reveal a direct correspondence between the JG [Formula: see text]-relaxation time [Formula: see text] and the lifetime of the mobile particle clusters [Formula: see text], defined as in previous DH studies, a relationship dual to the corresponding previously observed relationship between the [Formula: see text]-relaxation time [Formula: see text] and the lifetime of immobile particle clusters [Formula: see text]. Moreover, we find that the average diffusion coefficient D nearly coincides with [Formula: see text] of the smaller atomic species (Al) and that the 'hopping time' associated with D coincides with [Formula: see text] to within numerical uncertainty, both trends being in accord with experimental studies. This indicates that the JG [Formula: see text]-relaxation is dominated by the smaller atomic species and the observation of a direct relation between this relaxation process and rate of molecular diffusion in GF materials at low temperatures where the JG [Formula: see text]-relaxation becomes the prevalent mode of structural relaxation. As an unanticipated aspect of our study, we find that [Formula: see text] exhibits fragile-to-strong (FS) glass formation, as found in many other metallic GF liquids, but this fact does not greatly alter the geometrical nature of DH in this material and the relation of DH to dynamical properties. On the other hand, the temperature dependence of the DH and dynamical properties, such as the structural relaxation time, can be significantly altered from 'ordinary' GF liquids.

Fast dynamics in a model metallic glass-forming material.

We investigate the fast ß- and Johari-Goldstein (JG) ß-relaxation processes, along with the elastic scattering response of glass-forming (GF) liquids and the boson peak, in a simulated Al-Sm GF material exhibiting a fragile-strong (FS) transition. These dynamical processes are universal in "ordinary" GF fluids and collectively describe their "fast dynamics," and we find these relaxation processes also arise in a GF liquid exhibiting a FS transition. String-like particle motion, having both an irreversible and a reversible nature (stringlets) component, occurs in the fast-dynamics regime, corresponding to a ps timescale. String-like collective motion associated with localized unstable modes facilitates irreversible and intermittent particle "jumping" events at long times associated with the JG ß-relaxation process, while stringlets associated with localized stable modes and corresponding perfectly reversible atomic motion give rise to the boson peak. To further clarify the origin of the boson peak, we calculate the density of states for both the stringlet particles and the "normal" particles and find that the stringlet particles give rise to a boson peak, while the normal atoms do not. The growth of stringlets upon heating ultimately also leads to the "softening" of these excitations, and the boson peak frequency and shear modulus drop in concert with this softening. The growth of string-like collective motion upon heating in the fast-dynamics regime is further shown to be responsible for the growth in the intensity of the fast relaxation process. Relaxation in cooled liquids clearly involves a hierarchy of relaxation processes acting on rather different timescales and spatial scales.

Association of PNPLA3 rs738409 G/C gene polymorphism with nonalcoholic fatty liver disease in children: a meta-analysis.

BACKGROUND: Nonalcoholic fatty liver disease (NAFLD) is one of the most common causes of chronic liver disease worldwide. Current studies have shown that PNPLA3 (Patatin-like phospholipase domain containing 3) rs738409 G/C gene polymorphism is associated with adult nonalcoholic fatty liver disease [1, 2].But there is no consensus on the relationship between PNPLA3 rs738409 G/C gene polymorphism and children NAFLD due to differences in population samples. To this end, a meta-analysis of published research is conducted to comprehensively assess the relationship between PNPLA3 gene polymorphism and NAFLD in children. METHODS: We searched MEDLINE, PubMed, EMBASE, and CENTRAL databases from inception to May 2019. Case-control studies assessing the relationship between PNPLA3 rs738409 G/C gene polymorphism with non-alcoholic fatty liver disease in children were selected according to inclusion and exclusion criteria. Random effects model was used to quantify the association between the PNPLA3 rs738409 G/C gene polymorphism and the susceptibility of children's NAFLD. Fixed effects model was used to quantify the relationship between the PNPLA3 rs738409 G/C gene polymorphism and the severity of NAFLD in children. The Stata 12.0 software was employed for data analysis. RESULTS: A total of nine case-control studies were included in this meta-analysis containing data of 1173 children with NAFLD and 1792 healthy controls. Five studies compared NAFLD children and non-NAFLD healthy populations. Statistical analysis showed that PNPLA3 gene polymorphism was significantly associated with children's NAFLD in the allele contrast, dominant, recessive and over dominant models (G vs C,OR = 3.343, 95% CI = 1.524-7.334; GG + GC vs CC,OR = 3.157, 95% CI = 1.446-6.892;GG vs GC + CC,OR = 5.692, 95% CI = 1.941-16.689; GG + CC vs GC,OR = 2.756, 95% CI = 1.729-4.392). Four case-control studies compared Children with nonalcoholic fatty liver (NAFL) and children with nonalcoholic steatohepatitis (NASH). The results showed that the PNPLA3 gene polymorphism was also significantly associated with the severity of NAFLD in children in recessive gene model (GG vs GC + CC,OR = 14.43, 95% CI = 5.985-34.997); The Egger's test revealed no significant publication bias. CONCLUSIONS: Meta-analysis showed that PNPLA3 gene polymorphism was significantly associated with susceptibility and severity of NAFLD in children.

Predicting Complex Relaxation Processes in Metallic Glass.

Relaxation processes significantly influence the properties of glass materials. However, understanding their specific origins is difficult; even more challenging is to forecast them theoretically. In this study, using microseconds molecular dynamics simulations together with an accurate many-body interaction potential, we predict that an Al_{90}Sm_{10} metallic glass would have complex relaxation behaviors: In addition to the main (α) relaxation, the glass (i) shows a pronounced secondary (ß) relaxation at cryogenic temperatures and (ii) exhibits an anomalous relaxation process (α_{2}) accompanying α relaxation. Both of the predictions are verified by experiments. Computational simulations reveal the microscopic origins of relaxation processes: while the pronounced ß relaxation is attributed to the abundance of stringlike cooperative atomic rearrangements, the anomalous α_{2} process is found to correlate with the decoupling of the faster motions of Al with slower Sm atoms. The combination of simulations and experiments represents a first glimpse of what may become a predictive routine and integral step for glass physics.

Association of TM6SF2 rs58542926 T/C gene polymorphism with hepatocellular carcinoma: a meta-analysis.

BACKGROUND: Hepatocellular carcinoma (HCC) is the sixth-most common malignancy worldwide. Multiple previous studies have assessed the relationship between TM6SF2 gene polymorphism and the risk of developing HCC, with discrepant conclusions reached. To assess the association of TM6SF2 rs58542926 T/C gene polymorphism with liver cancer, we performed the current meta-analysis. METHODS: This study queried the MEDLINE, PubMed, EMBASE, and CENTRAL databases from inception to April 2019. Case-control studies assessing the relationship between TM6SF2 rs5854292 locus polymorphism and liver cancer were selected according to inclusion and exclusion criteria. The Stata 12.0 software was employed for data analysis. RESULTS: A total of 5 articles, encompassing 6873 patients, met inclusion criteria and were included in the meta-analysis. Statistical analysis showed that the TM6SF2 gene polymorphism was significantly associated with liver cancer in the allele contrast, dominant, recessive and over dominant models (T vs C, OR = 1.621, 95%CI 1.379-1.905; CT + TT vs CC. OR = 1.541, 95%CI 1.351-1.758; TT vs CT + CC, OR = 2.897, 95%CI 1.690-4.966; CC + TT vs TC, OR = 0.693, 95%CI 0.576-0.834). The Egger's test revealed no significant publication bias. CONCLUSION: The present findings suggest a significant association of TM6SF2 gene polymorphism with HCC risk in the entire population studied.

Structural origin for vibration-induced accelerated aging and rejuvenation in metallic glasses.

Glassy materials are nonequilibrium and their energy states have crucial influences on properties. Recent studies have shown that oscillating deformations (vibrations) can cause either accelerated aging (lowering energy) or rejuvenation (elevating energy); however, the underlying atomic mechanisms remain elusive. Using metallic glasses (MGs) as model systems, we show that the vibration-induced accelerated aging is correlated with the strain field of the stringlike atomic motions stemming from the Johari-Goldstein (ß) relaxation, whereas the rejuvenation is associated with nonlinear response and the formation of nanoscale shear bands attributing to the activation of α relaxation. Both processes are affected by thermal fluctuations, which result in an optimal temperature for accelerated aging. These results suggest intrinsic correlations among relaxation dynamics, mechanical properties, and the vibration induced structural rearrangements in MGs.

Anomalous nonlinear damping in metallic glasses: Signature of elasticity breakdown.

Solid materials, whether crystalline or glasses, are characterized by their elasticity. Generally, elasticity is independent of the probing strain if it is not exceeding the yielding point. Here, by contrast, we experimentally capture a pronounced strain-dependent elasticity in metallic glasses, as manifested by nonlinear mechanical damping in the apparent elastic deformation regime (∼1/100 of the yielding strain). Normal damping behaviors recover at higher temperatures but still below the glass transition. Atomistic simulations reproduce these features and reveal that they could be related to avalanche-like local structural instabilities. Our findings demonstrate that the standard elasticity is not held for metallic glasses at low temperatures and plastic events can be triggered at small perturbations. These results are consistent with previous simulations of model glasses and a scenario of hierarchical free-energy landscape of mean-field theory.

[Inhibitory effect of Panax notoginseng saponins on alveolar epithelial to mesenchymal transition].

In the study, the effects of Panax notoginseng saponins (PNS) on alveolar epithelial to mesenchymal transition (EMT) and extracellular matrix degradation were observed in a type of human alveolar epithelial cell, A549 cells, stimulated by TGF-beta1. Firstly, MTT method was applied to evaluation of cellular proliferation and found that PNS from 12.5 mg x L(-1) to 200 mg x L(-1) dosage could not inhibit significantly cellular proliferation. Then, cells were divided into five groups, normal group, TGF-beta1 group, TGF-beta1 + 50 mg x L(-1) PNS group, TGF-beta1 + 100 mg x L(-1) PNS group and TGF-beta1 + 200 mg x L(-1) PNS group. Normal cells were not stimulatec by TGF-beta1; TGF-beta1 cells were only stimulated by TGF-beta1 and the other cells were stimulated by TGF-beta1 with different doses of PNS, respectively. After stimulation, cells and supernatants were collected for assays. Cellular roundness was applied to quantitative evaluation of morphological change. Immunocytochemistry was applied to examine E-cadherion, a-SMA and FN proteins expression in the cells. Enzyme linked-immunosorbent assay was applied to MMP-9 and TIMP-1 levels. The results showed that EMT of A549 cells was induced by TGF-beta1, showing significant change of roundness, E-cadherion, alpha-SMA and FN (P < 0.05, P < 0.01). Compared to TGF-beta1, PNS significantly inhibited the changes of roundness (P < 0.05), FN and alpha-SMA (P < 0.05, P < 0.01) and not significantly inhibited the change of E-cadherion. Furthermore, MMP-9 levels were significantly increased by TGFbeta1 stimulation (P < 0.05), without significant change of TIMP-1. Compared with TGF-beta1, PNS could significantly increase MMP-9 level (P < 0.05) and decrease TIMP-1 levels (P < 0.05, P < 0.01). In conclusion, PNS could inhibit alveolar epithelial cell EMT induced by TGF-beta1, with increase of extracellular matrix degradation ability, which showed anti-fibrosis of lung ability.

[Discussing the basic ecological relations of sand dune vegetation process]. / è®ºæ²™ä¸˜æ¤è¢«è¿‡ç¨‹çš„åŸºæœ¬ç”Ÿæ€å ³ç³».

Dune is often considered as a degraded ecosystem. Natural vegetation restoration and stable artificial vegetation construction are the basic means restoring dune ecosystem. Based on long-term study of dune ecosystem, by taking into consideration both the philosophical principles of unity of opposites and dynamic change, and related ecological theories, we put forward some ecological relations that should be paid attention to in the study of vegetation assembly from the perspective of the uniqueness of dune ecosystem. We discussed the necessity of coupling relationships of scale-pattern-process and the transformation of synergy-tradeoff relationships, interpreted the importance of distinguishing sand dune stabilized and shifting phases, disturbance and stress, wind erosion and sand burial in the study of vegetation process. We further explored the applied value of niche law or neutral law in the study of dune vegetation process. Finally, we discussed the issues that should be paid attention to in the study of dune vegetation process from the aspects of adaptability to aeolian activities and drought tolerance, physiological and reproductive process, sexual and asexual reproduction of plants. This study would provide theoretical supports for vegetation restoration and stable vegetation construction of dune ecosystem.

Universal origin of glassy relaxation as recognized by configuration pattern matching.

Relaxation processes are crucial for understanding the structural rearrangements of liquids and amorphous materials. However, the overarching principle that governs these processes across vastly different materials remains an open question. Substantial analysis has been carried out based on the motions of individual particles. Here, as an alternative, we propose viewing the global configuration as a single entity. We introduce a global order parameter, namely the inherent structure minimal displacement (IS Dmin), to quantify the variability of configurations by a pattern-matching technique. Through atomic simulations of seven model glass-forming liquids, we unify the influences of temperature, pressure and perturbation time on the relaxation dissipation, via a scaling law between the mechanical damping factor and IS Dmin. Fundamentally, this scaling reflects the curvature of the local potential energy landscape. Our findings uncover a universal origin of glassy relaxation and offer an alternative approach to studying disordered systems.

Predicting the pathways of string-like motions in metallic glasses via path-featurizing graph neural networks.

String-like motions (SLMs)-cooperative, "snake"-like movements of particles-are crucial for dynamics in diverse glass formers. Despite their ubiquity, questions persist: Do SLMs prefer specific paths? If so, can we predict these paths? Here, in Al-Sm glasses, our isoconfigurational ensemble simulations reveal that SLMs do follow certain paths. By designing a graph neural network (GNN) to featurize the environment around directional paths, we achieve a high-fidelity prediction of likely SLM pathways, solely based on the static structure. GNN gauges a structural measure to assess each path's propensity to engage in SLMs, akin to a "softness" metric, but for paths rather than for atoms. Our GNN interpretation reveals the critical role of the bottleneck zone along a path in steering SLMs. By monitoring "path softness," we elucidate that SLM-favored paths transit from fragmented to interconnected upon glass transition. Our findings reveal that, beyond atoms or clusters, glasses have another dimension of structural heterogeneity: "paths."

Amorphous conversion in pyrolytic symmetric trinuclear nickel clusters trigger trifunctional electrocatalysts.

The pursuit of multifunctional electrocatalysts holds significant importance due to their comprehension of material chemistry. Amorphous materials are particularly appealing, yet they pose challenges in terms of rational design due to their structural disorder and thermal instability. Herein, we propose a strategy that entails the tandem (low-temperature/250-350 °C) pyrolysis of molecular clusters, enabling preservation of the local short-range structures of the precursor Schiff base nickel (Ni3[2(C21H24N3Ni1.5O6)]). The temperature-dependent residuals demonstrate exceptional activity and stability for at least three distinct electrocatalytic processes, including the oxygen evolution reaction (η10 = 197 mV), urea oxidation reaction (η10 = 1.339 V), and methanol oxidation reaction (1358 mA cm-2 at 0.56 V). Three distinct nickel atom motifs are discovered for three efficient electrocatalytic reactions (Ni1 and Ni1' are preferred for UOR/MOR, while Ni2 is preferred for OER). Our discoveries pave the way for the potential development of multifunctional electrocatalysts through disordered engineering in molecular clusters under tandem pyrolysis.