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Due to the extensive use of plastic products and unreasonable disposal, nanoplastics contamination has become one of the important environmental problems that mankind must face. The composition and structure of porous media can determine the complexity and diversity of the transport behavior of nanoplastics. In this study, the influence of diatomite (DIA) on the nanoplastics transport in porous media is investigated by column experiments combined with XDLVO interaction energy and transport model. Results suggest that the recovery rates of unmodified polystyrene nanoparticles (PSNPs) and carboxyl-modified polystyrene nanoparticles (PSNPs-COOH) in the porous media containing DIA decreases compared with that in the pure quartz sand (QS), and the BTCs showed a "blocking" pattern. The presence of DIA inhibits the transport of both PSNPs and PSNPs-COOH, but the inhibition is not significant. This may be because the presence of DIA provides more favorable deposition sites for PSNPs and PSNPs-COOH to some extent. However, since DIA itself carries a certain negative charge, this can only play a role in compressing the double electric layer for PSNPs and PSNPs-COOH with the same negative charge, and cannot destabilize them. The migration capacity of PSNPs and PSNPs-COOH is strongest in the DIA-QS porous media at pH = 7, and is weak at pH = 9 and pH = 5. The inhibition of migration at pH = 9 can be attributed to the dissolution of the DIA surface under alkaline conditions and the formation of pore and defect structures, which provide more deposition sites for PSNPs and PSNPs-COOH. The presence of humic acid (HA) leads to an increase in the mobility of PSNPs and PSNPs-COOH, and the mobility is enhanced with HA concentration. The mobility of PSNPs and PSNPs-COOH in DIA-QS decreases with ionic valence and ionic strength, and PSNPs-COOH is more significantly inhibited compared to PSNPs.
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Solution Gated Graphene Field-Effect Transistors (SGGT) are eagerly anticipated as an amplification platform for fabricating advanced ultra-sensitive sensors, allowing significant modulation of the drain current with minimal gate voltage. However, few studies have focused on light-matter interplay gating control for SGGT. Herein, this challenge is addressed by creating an innovative photoelectrochemical solution-gated graphene field-effect transistor (PEC-SGGT) functionalized with enzyme cascade reactions (ECR) for Organophosphorus (OPs) detection. The ECR system, consisting of acetylcholinesterase (AChE) and CuBTC nanomimetic enzymes, selectively recognizes OPs and forms o-phenylenediamine (oPD) oligomers sediment on the PEC electrode, with layer thickness related to the OPs concentration, demonstrating time-integrated amplification. Under light stimulation, the additional photovoltage generated on the PEC gate electrode is influenced by the oPD oligomers sediment layer, creating a differentiated voltage distribution along the gate path. PEC-SGGT, inherently equipped with built-in amplification circuits, sensitively captures gate voltage changes and delivers output with an impressive thousandfold current gain. The seamless integration of these three amplification modes in this advanced sensor allows a good linear range and highly sensitive detection of OPs, with a detection limit as low as 0.05 pm. This work provides a proof-of-concept for the feasibility of light-assisted functionalized gate-controlled PEC-SGGT for small molecule detection.
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In recent years, dysprosium macrocycle single-molecule magnets (SMMs) have received increasing attention due to their excellent air/thermal stability, strong magnetic anisotropy, and rigid molecular skeleton. However, they usually display fast zero-field quantum tunneling of the magnetization (QTM) rate, severely hindering their data storage applications. Herein, we report the design, synthesis, and characterization of an air-stable monodecker didysprosium macrocycle integrating strong single-ion anisotropy, near-perfect local crystal field (CF) symmetry, and efficient exchange bias. These indispensable features enable clear-cut elucidation of the crucial role of very weak antiferromagnetic coupling on magnetization dynamics, creating a prominent SMM with a large effective energy barrier (Ueff) of 670 cm-1, open hysteresis loops at zero field up to 14.9 K, and a record relaxation time of QTM (τQTM), 24281 s, for all known nonradical-bridged lanthanide SMMs.
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Rubidium atomic clocks have been used extensively in various fields, with applications such as a core component of Global Navigation Satellite Systems (GNSS). However, they exhibit inherently poor long-term stability. This paper presents the development of a control system for rubidium atomic clocks. It introduces an adaptive Kalman filtering algorithm for the disciplining of a rubidium atomic clock, utilizing autocovariance least squares (ALS) to estimate the clock's noise parameters. The experimental results demonstrate that the proposed algorithm achieves a high estimation accuracy. The standard deviation of the clock error between the steered rubidium atomic clock 1 Pulse Per Second (1PPS) and Coordinated Universal Time (UTC) provided by the National Time Service Center (NTSC) is better than 2.568 nanoseconds(ns), with peak-to-peak values improving to within 11.358 ns. Notably, its frequency stability is reduced to 3.06 × 10-13 @100,000 s. The results for the rubidium atomic clock demonstrate that the adaptive Kalman filtering algorithm proposed herein constitutes an accurate and effective control strategy for the rubidium atomic clock discipline.
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Heterotopic ossification (HO), defined as the formation of extraskeletal bone in muscle and soft tissues, is a diverse pathological process caused by either genetic mutations or inciting trauma. Fibrodysplasia ossificans progressiva (FOP) is a genetic form of HO caused by mutations in the bone morphogenetic protein (BMP) type I receptor gene activin A receptor type 1 (ACVR1). These mutations make ACVR1 hypersensitive to BMP and responsive to activin A. Hedgehog (Hh) signaling also contributes to HO development. However, the exact pathophysiology of how skeletogenic cells contribute to endochondral ossification in FOP remains unknown. Here, we showed that the wild-type or FOP-mutant ACVR1 localized in the cilia of stem cells from human exfoliated deciduous teeth with key FOP signaling components, including activin A receptor type 2A/2B, SMAD family member 1/5, and FK506-binding protein 12kD. Cilia suppression by deletion of intraflagellar transport 88 or ADP ribosylation factor like GTPase 3 effectively inhibited pathological BMP and Hh signaling, subdued aberrant chondro-osteogenic differentiation in primary mouse or human FOP cells, and diminished in vivo extraskeletal ossification in Acvr1Q207D, Sox2-Cre; Acvr1R206H/+ FOP mice and in burn tenotomy-treated wild-type mice. Our results provide a rationale for early and localized suppression of cilia in affected tissues after injury as a therapeutic strategy against either genetic or acquired HO.
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Receptores de Activinas Tipo I , Proteínas Morfogenéticas Óseas , Cilios , Proteínas Hedgehog , Miositis Osificante , Osificación Heterotópica , Transducción de Señal , Osificación Heterotópica/metabolismo , Osificación Heterotópica/patología , Cilios/metabolismo , Cilios/patología , Proteínas Hedgehog/metabolismo , Animales , Humanos , Proteínas Morfogenéticas Óseas/metabolismo , Receptores de Activinas Tipo I/metabolismo , Ratones , Miositis Osificante/metabolismo , Miositis Osificante/patología , Osteogénesis , Células Madre/metabolismoRESUMEN
It is important to differentiate milk with different thermostabilities for diverse applications in food products and for the appropriate selection of processing and maintenance of manufacturing facilities. In this review, an overview of the chemical changes in milk subjected to high-temperature heating is given. An emphasis is given to the studies of traditional and state-of-the-art strategies for assessing the milk thermostability, as well as their influencing factors. Traditional subjective and objective techniques have been used extensively in many studies for evaluating thermostability, whereas recent research has been focused on novel approaches with greater objectivity and accuracy, including innovative physical, spectroscopic, and predictive tools.
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This study presents the utilization of a novel, highly lipophilic nitric oxide (NO) donor molecule, S-nitroso-1-adamantanethiol (SNAT), for developing an NO-emitting polymer surface aimed at preventing thrombus formation and bacterial infection in extracorporeal circuits (ECCs). S-nitroso-1-adamantanethiol, a tertiary nitrosothiol-bearing adamantane species, was synthesized, characterized, and used to impregnate polyvinyl chloride (PVC) tubing for subsequent in vivo evaluation. The impregnation process with SNAT preserved the original mechanical strength of the PVC. In vitro assessments revealed sustained NO release from the SNAT-impregnated PVC tubing (iSNAT), surpassing or matching endothelial NO release levels for up to 42 days. The initial NO release remained stable even after 1 year of storage at -20°C. The compatibility of iSNAT with various sterilization techniques (OPA Plus, hydrogen peroxide, EtO) was tested. Acute in vivo experiments in a rabbit model demonstrated significantly reduced thrombus formation in iSNAT ECCs compared with controls, indicating the feasibility of iSNAT to mitigate coagulation system activation and potentially eliminate the need for systemic anticoagulation. Moreover, iSNAT showed substantial inhibition of microbial biofilm formation, highlighting its dual functionality. These findings underscore the promising utility of iSNAT for long-term ECC applications, offering a multifaceted approach to enhancing biocompatibility and minimizing complications.
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In this study, the antibacterial mechanism of metabolites of Lactobacillus plantarum SCB2505 (MLp SCB2505) against Pseudomonas lundensis (P. lundensis) SCB2605 was investigated, along with evaluation of their preservative effects on dry-aged beef. The results demonstrated the effective inhibition of MLp SCB2505 on the growth and biofilm synthesis of P. lundensis. The treatment with MLp SCB2505 led to the compromised membrane integrity, as evidenced by reduced intracellular ATP content, increased extracellular AKPase, K+ and protein content, as well as disrupted cell morphology. Further metabolomics analysis revealed that MLp SCB2505 interfered amino acid metabolism, nucleotide metabolism, cofactor and vitamin metabolism, lipid metabolism and respiratory chain in P. lundensis, ultimately leading to the interrupted life activities and even death of the bacteria. Besides, MLp SCB2505 could effectively inhibit the growth of Pseudomonas in dry-aged beef and delay spoilage. These findings propose the potential application of MLp SCB2505 as an antibacterial agent in meat products.
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In this study, we developed a solar ceramic kiln to address the problem of CO2 emissions caused by traditional ceramic ware firing processes. Ceramic specimens were fired using the proposed setup, and their properties were compared with those of an electric-fired ceramic cup (ECC). The solar-fired ceramic cup (SCC) exhibited no cracks on its surface. Its water absorption was 4.25%, open porosity was 9.93%, bulk density was 2.210 g/cm3, bending strength was 88.96 MPa, and ovalization was 1.46%. These findings suggested that the physical performance of the SCC was comparable to that of the ECC, which had water absorption of 4.03%, an open porosity of 8.79%, a bulk density of 2.180 g/cm3, an ovalization of 1.45%, and a bending strength of 72.4 MPa. The SCC achieved these results in 120 min, which was seven times faster than that of the ECC (firing time of 869 min).
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Differences in electrical properties of media are the basis for determining the type and extent of contamination using geophysical methods. However, differences in heavy metals and organic matter complicate the electrical properties of compound-contaminated media, and existing geophysical methods cannot independently identify compound contamination. Therefore, this study proposes a geophysical detection system that combines electrical resistance tomography (ERT) and induced polarization methods and establishes a solid theory as the basis for the system application through laboratory experiments, model analysis, and site applications. The study reveals that as the organics volume proportion increases, the resistivity and normalized chargeability of contaminated media increased slowly, followed by a rapid increase, and finally reached a stable state. The specific type of compound significantly influences the electrical properties, while the resistivity of different kinds of compound-contaminated media reaches the same maximum value as the organics volume proportion increases. The medium type determines the contaminated media's lower resistivity limit and upper normalized chargeability limit. Additionally, the interplay between heavy metal type, content, and medium complicates the electrical properties of the media, with the compound type exerting a significant impact on resistivity. Archie's law and random forest modeling reveal that the inflection point for resistivity change occurs at 40 % and 80 % organics volume proportions, while the inflection point for normalized chargeability change occurs at 30 % and 70 % organics volume proportions in compound-contaminated media. These inflection points depend on the types of compounds, compositions, proportions, and media, and their importance for the electrical properties of the media changes with the increasing organics volume proportion. Based on the changing patterns of resistivity and normalized chargeability in heavy metal-organic compound contaminated media, the modified geophysical detection system can effectively identify the pollution type and intensity, which provides accurate pollution information to develop effective treatment strategies.
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The shift of carbon utilization from primarily glucose to other nutrients is a fundamental metabolic adaptation to cope with decreased blood glucose levels and the consequent decline in glucose oxidation. AMP-activated protein kinase (AMPK) plays crucial roles in this metabolic adaptation. However, the underlying mechanism is not fully understood. Here, we show that PDZ domain containing 8 (PDZD8), which we identify as a new substrate of AMPK activated in low glucose, is required for the low glucose-promoted glutaminolysis. AMPK phosphorylates PDZD8 at threonine 527 (T527) and promotes the interaction of PDZD8 with and activation of glutaminase 1 (GLS1), a rate-limiting enzyme of glutaminolysis. In vivo, the AMPK-PDZD8-GLS1 axis is required for the enhancement of glutaminolysis as tested in the skeletal muscle tissues, which occurs earlier than the increase in fatty acid utilization during fasting. The enhanced glutaminolysis is also observed in macrophages in low glucose or under acute lipopolysaccharide (LPS) treatment. Consistent with a requirement of heightened glutaminolysis, the PDZD8-T527A mutation dampens the secretion of pro-inflammatory cytokines in macrophages in mice treated with LPS. Together, we have revealed an AMPK-PDZD8-GLS1 axis that promotes glutaminolysis ahead of increased fatty acid utilization under glucose shortage.
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OBJECTIVES: This study aims to investigate the diagnostic value of heparin-binding protein (HBP) in sepsis and develop a sepsis diagnostic model incorporating HBP with key biomarkers and disease-related scores for rapid, and accurate diagnosis of sepsis in the intensive care unit (ICU). DESIGN: Clinical retrospective cross-sectional study. SETTING: A comprehensive teaching tertiary hospital in China. PARTICIPANTS: Adult patients (aged ≥18 years) who underwent HBP testing or whose blood samples were collected when admitted to the ICU. MAIN OUTCOME MEASURES: HBP, C reactive protein (CRP), procalcitonin (PCT), white blood cell count (WBC), interleukin-6 (IL-6), lactate (LAC), Acute Physiology and Chronic Health Evaluation II (APACHE II) and Sequential Organ Failure Assessment (SOFA) score were recorded. RESULTS: Between March 2019 and December 2021, 326 patients were enrolled in this study. The patients were categorised into a non-infection group (control group), infection group, sepsis group and septic shock group based on the final diagnosis. The HBP levels in the sepsis group and septic shock group were 45.7 and 69.0 ng/mL, respectively, which were significantly higher than those in the control group (18.0 ng/mL) and infection group (24.0 ng/mL) (p<0.001). The area under the curve (AUC) value of HBP for diagnosing sepsis was 0.733, which was lower than those corresponding to PCT, CRP and SOFA but higher than those of IL-6, LAC and APACHE II. Multivariate logistic regression analysis identified HBP, PCT, CRP, IL-6 and SOFA as valuable indicators for diagnosing sepsis. A sepsis diagnostic model was constructed based on these indicators, with an AUC of 0.901, a sensitivity of 79.7% and a specificity of 86.9%. CONCLUSIONS: HBP could serve as a biomarker for the diagnosis of sepsis in the ICU. Compared with single indicators, the sepsis diagnostic model constructed using HBP, PCT, CRP, IL-6 and SOFA further enhanced the diagnostic performance of sepsis.
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Péptidos Catiónicos Antimicrobianos , Biomarcadores , Proteínas Sanguíneas , Proteína C-Reactiva , Unidades de Cuidados Intensivos , Puntuaciones en la Disfunción de Órganos , Sepsis , Humanos , Estudios Retrospectivos , Estudios Transversales , Femenino , Masculino , Biomarcadores/sangre , Persona de Mediana Edad , Sepsis/diagnóstico , Sepsis/sangre , China , Anciano , Proteínas Sanguíneas/análisis , Proteína C-Reactiva/análisis , Proteína C-Reactiva/metabolismo , Péptidos Catiónicos Antimicrobianos/sangre , Polipéptido alfa Relacionado con Calcitonina/sangre , APACHE , Interleucina-6/sangre , Adulto , Curva ROC , Ácido Láctico/sangreRESUMEN
Optimizing the width of depletion region is a key consideration in designing high performance photovoltaic photodetectors, as the electron-hole pairs generated outside the depletion region cannot be effectively separated, leading to a negligible contribution to the overall photocurrent. However, currently reported photovoltaic mid-infrared photodetectors based on two-dimensional heterostructures usually adopt a single pn junction configuration, where the depletion region width is not maximally optimized. Here, we demonstrate the construction of a high performance broadband mid-infrared photodetector based on a MoS2/b-AsP/MoS2npn van der Waals heterostructure. The npn heterojunction can be equivalently represented as two parallel-stacked pn junctions, effectively increasing the thickness of the depletion region. Consequently, the npn device shows a high detectivity of 1.3 × 1010cmHz1/2W-1at the mid-infrared wavelength, which is significantly improved compared with its single pn junction counterpart. Moreover, it exhibits a fast response speed of 12 µs, and a broadband detection capability ranging from visible to mid-infrared wavelengths.
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Rubrolides are natural butyrolactones isolated from the tunicate Ritterella rubra, shows antibacterial, antiviral and plant photosynthesis inhibitory activities. In this study, a facile total synthetic method for preparing the rubrolides from benzaldehyde by a Darzens reaction, aldol reaction and vinylogous aldol condensation in five steps is presented. Three natural rubrolides (E, C and F) were synthesised in the total yields of 25-40%. The bioassay results indicate that rubrolides E, C and F exhibit some herbicidal inhibitory effect against rapeseed, in particular, rubrolide F shows the best herbicidal activities against rapeseed root with the growth inhibitory rate of 72.8%. At greenhouse treatment concentrations of 100 and 500 mg/L, rubrolide F show a positive dose-toxicity correlation towards abutilon plants. Collectively, facile total Synthesis strategy provided the base for further bioactivities study of rubrolides family. Rubrolide F may be act as inhibitor of photosynthesis, and this could be lead structure of new herbicide.
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This work reports on the preparation of uniform vesicle-structural carbon spheres doped with heteroatoms of N, P, and S, with the pore sizes strictly controlled by the hard templates of monodisperse submicron SiO2 spheres. The uniformly doped vesicular carbon microspheres are obtained in three steps: Stöber hydrolysis for the SiO2; in situ polymerization for the immobilization; and alkaline etching after carbonization. The size of the vesicles can be easily adjusted by regulating the particle size of the submicron SiO2 spheres, which has a significant effect on its electromagnetic wave (EMW) absorption performance. Compared with microspheres with pore sizes of 180 and 480 nm, when the vesicle aperture is 327 nm, with only 5.5 wt.% filling load and 1.9 mm thickness, the material shows the best EMW absorption behavior with the effective absorption bandwidth (EAB) covers the entire Ku band (6.32 GHz) and the minimum reflection loss (RLmin) of -36.10 dB, suggesting the optimized pore size of the microspheres can significantly improve the overall impedance matching of the material and achieve broadband wave absorption. This work paves the way for the enhancement of EMW absorption properties of porous material by optimizing the pore size of uniform apertures while maintaining their composition.
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With the application of engineered nanomaterials and antibiotics in the fields of medicine, aerospace, new energy and agriculture, the associated contamination is detected widely in soil-groundwater systems. It is of great scientific and practical significance to deeply explore the environmental interface process between nanoparticles and antibiotics for the scientific assessment of environmental fate and ecological environmental risks, as well as the development of new composite pollution control technologies. In this study, the co-transport behaviors of positively charged titanium dioxide nanoparticles (TiO2-NPs) and negatively charged levofloxacin (LEV) in quartz sand (QS) are investigated in this study. The results show that TiO2-NPs hardly flow out when transported alone in the column because of its positive charge, which creates a strong attraction with the negatively charged quartz sand on the surface. When TiO2-NPs co-migrate with LEV in porous media, the presence of LEV promotes the transport of TiO2-NPs, while the presence of TiO2-NPs inhibits LEV transport. Non-XDLVO interactions based on molecular dynamics (MD) simulations can help explain the observed promotion and inhibition phenomena as well as the correlation between TiO2-NPs and LEV. The results indicate that TiO2-LEV complexes or aggregates can be formed during the co-transportation process of TiO2-NPs and LEV in porous media. As flow velocity increases from 0.204 cm min-1 to 1.630 cm min-1, both the transport capacities of TiO2-NPs and LEV are enhanced significantly. Under the condition of high citric acid (CA) concentration (15 mmol L-1), the transport capacity of TiO2-NPs is slightly inhibited, while the transport capacity of LEV is enhanced. This study provides new insights into the transport of nanometallic oxides and antibiotics in porous media, which suggests that non-XDLVO interactions should be considered together when assessing the environmental risks and fate of nanometallic oxides and antibiotics in soil-groundwater systems.
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Levofloxacino , Titanio , Titanio/química , Levofloxacino/química , Porosidad , Nanopartículas/química , Antibacterianos/química , Contaminantes Químicos del Agua/química , Contaminantes del Suelo/química , Nanopartículas del Metal/química , Agua Subterránea/química , Simulación de Dinámica MolecularRESUMEN
OBJECTIVE: To investigate the predictive value of left ventricular global longitudinal peak strain (GLPS) for the prognosis of septic patients. METHODS: A prospective cohort study was conducted. Patients diagnosed with sepsis and admitted to the intensive care unit (ICU) of the First Affiliated Hospital, Sun Yat-sen University from December 2018 to November 2019 were enrolled. The patient characteristics, cardiac ultrasound parameters [left ventricular ejection fraction (LVEF), right ventricular ejection fraction (RVEF), four-dimensional ejection fraction (4DEF), GLPS] and cardiac biomarkers [N-terminal pro-brain natriuretic peptide (NT-proBNP), cardiac troponin T (cTnT)] within 24 hours of ICU admission, organ support therapies, severity of illness, and prognostic indicators were documented. The differences in clinical parameters between patients with varying outcomes during ICU hospitalization were assessed. Pearson correlation analysis was employed to explore the correlation between GLPS and other cardiac systolic parameters, as well as the associations between various cardiac systolic parameters and sequential organ failure assessment (SOFA) score. Receiver operator characteristic curve (ROC curve) was drawn to analyze the predictive capacity of cardiac ultrasound parameters and cardiac biomarkers for death during ICU hospitalization in septic patients. RESULTS: A total of 50 septic patients were enrolled, with 40 surviving and 10 dying during ICU hospitalization, resulting in a mortality of 20.0%. All patients in the death group were male. Compared with the survival group, the patients in the death group were older, had a higher prevalence of diabetes mellitus, and received continuous renal replacement therapy (CRRT) more frequently, additionally, they exhibited more severe illness and had longer length of ICU stay. The levels of GLPS and cTnT in the death group were significantly elevated as compared with the survival group [GLPS: -7.1% (-8.5%, -7.0%) vs. -12.1% (-15.5%, -10.4%), cTnT (µg/L): 0.07 (0.05, 0.08) vs. 0.03 (0.02, 0.13), both P < 0.05]. However, no statistically significant difference was found in other cardiac ultrasound parameters or cardiac biomarkers between the two groups. Pearson correlation analysis revealed a negative correlation between GLPS and LVEF (r = -0.377, P = 0.014) and 4DEF (r = -0.697, P = 0.000), while no correlation was found with RVEF (r = -0.451, P = 0.069). GLPS demonstrated a positive correlation with SOFA score (r = 0.306, P = 0.033), while LVEF (r = 0.112, P = 0.481), RVEF (r = -0.134, P = 0.595), and 4DEF (r = -0.251, P = 0.259) showed no significant correlation with SOFA score. ROC curve analysis indicated that the area under the ROC curve (AUC) of GLPS for predicting death during ICU hospitalization in septic patients was higher than other cardiac systolic parameters, including LVEF, RVEF, and 4DEF, as well as cardiac biomarkers NT-proBNP and cTnT (0.737 vs. 0.628, 0.556, 0.659, 0.580 and 0.724). With an optimal cut-off value of -14.9% for GLPS, the sensitivity and negative predictive value reached to 100%. CONCLUSIONS: GLPS < -14.9% within 24 hours of ICU admission in septic patients indicated a reduced risk of death risk during ICU hospitalization, while also correlating with the severity of organ dysfunction in this patient population.
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Unidades de Cuidados Intensivos , Sepsis , Humanos , Estudios Prospectivos , Pronóstico , Sepsis/diagnóstico , Sepsis/mortalidad , Sepsis/fisiopatología , Troponina T/sangre , Ventrículos Cardíacos/fisiopatología , Ventrículos Cardíacos/diagnóstico por imagen , Biomarcadores/sangre , Ecocardiografía , Función Ventricular Izquierda , Volumen Sistólico , Masculino , Femenino , Péptido Natriurético Encefálico/sangre , Curva ROC , Fragmentos de Péptidos/sangre , Valor Predictivo de las Pruebas , Persona de Mediana EdadRESUMEN
Composite oxides have been widely applied in the hydrogenation of CO/CO2 to methanol or as the component of bifunctional oxide-zeolite for the synthesis of hydrocarbon chemicals. However, it is still challenging to disentangle the stepwise formation mechanism of CH3OH at working conditions and selectively convert CO2 to hydrocarbon chemicals with narrow distribution. Here, we investigate the reaction network of the hydrogenation of CO2 to methanol over a series of spinel oxides (AB2O4), among which the Zn-based nanostructures offer superior performance in methanol synthesis. Through a series of (quasi) in situ spectroscopic characterizations, we evidence that the dissociation of H2 tends to follow a heterolytic pathway and that hydrogenation ability can be regulated by the combination of Zn with Ga or Al. The coordinatively unsaturated metal sites over ZnAl2Ox and ZnGa2Ox originating from oxygen vacancies (OVs) are evidenced to be responsible for the dissociative adsorption and activation of CO2. The evolution of the reaction intermediates, including both carbonaceous and hydrogen species at high temperatures and pressures over the spinel oxides, has been experimentally elaborated at the atomic level. With the integration of a series of zeolites or zeotypes, high selectivities of hydrocarbon chemicals with narrow distributions can be directly produced from CO2 and H2, offering a promising route for CO2 utilization.
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[This corrects the article DOI: 10.3389/fnint.2023.1234471.].