Search

An electrochemical quartz crystal microbalance (EQCM) was used to in situ reveal the deposition/dissolution chemistry of MnO2 in aqueous electrolytes, which proceeds by a pH-dependent Mn(iii) (MnOOH and/or Mn3+)-mediated path.

The aqueous zinc (Zn) battery is a safe and eco-friendly energy-storage system. However, the use of Zn metal anodes is impeded by uncontrolled Zn deposition behavior. Herein, we regulate the Zn-ion deposition process for dendrite-free Zn metal anodes using an aminosilane molecular layer with high zincophilic sites and narrow molecule channels. The aminosilane molecular layer causes Zn ions to undergo consecutive processes including being captured by the amine functional groups of aminosilane and diffusing through narrow intermolecular channels before electroplating, which induces partial dehydration of hydrated Zn ions and uniform Zn ion flux, promoting reversible Zn stripping/plating. Through this molecule-induced capture-diffusion-deposition procedure of Zn ions, smooth and compact Zn electrodeposited layers are obtained. Hence, the aminosilane-modified Zn anode has high Coulombic efficiency (∼99.5%), long lifespan (∼3000 h), and high capacity retention in full cells (88.4% for 600 cycles). This strategy not only has great potential for achieving dendrite-free Zn anodes in practical Zn batteries but also suggests an interface-modification principle at the molecular level for other alternative metallic anodes.

Excess greenhouse gas emissions, primarily carbon dioxide (CO2), have caused major environmental concerns worldwide. The electroreduction of CO2 into valuable chemicals using renewable energy is an ecofriendly approach to achieve carbon neutrality. In this regard, copper (Cu) has attracted considerable attention as the only known metallic catalyst available for converting CO2 to high-value multicarbon (C2+) products. The production of C2+ involves complicated C–C coupling steps and thus imposes high demands on intermediate regulation. In this review, we discuss multiple strategies for modulating intermediates to facilitate C2+ formation on Cu-based catalysts. Furthermore, several sophisticated in situ characterization techniques are outlined for elucidating the mechanism of C–C coupling. Lastly, the challenges and future directions of CO2 electroreduction to C2+ are envisioned.

As the genome is organized into a three-dimensional structure in intracellular space, epigenomic information also has a complex spatial arrangement. However, most epigenetic studies describe locations of methylation marks, chromatin accessibility regions, and histone modifications in the horizontal dimension. Proper spatial epigenomic information has rarely been obtained. In this study, we designed spatial chromatin accessibility sequencing (SCA-seq) to resolve the genome conformation by simultaneously capturing the epigenetic information in single-molecular resolution. Using SCA-seq, we simultaneously disclosed spatial interaction of chromatin accessibility (e.g. enhancer-promoter contacts), CpG island methylation, and spatial insulating functions of the CCCTC-binding factor. We demonstrate that SCA-seq paves the way to explore the mechanism of epigenetic interactions and extends our knowledge in 3D packaging of DNA in the nucleus.

supplemental Figure 1-12. Expression levels of 10 lncRNAs by qRT-PCR in 15 GBC tissues and paired non-tumor tissues (Figure 1). Expression levels of 8 mRNAs by qRT-PCR in 15 GBC tissues and paired non-tumor tissues (Figure 2). Molecular characteristics of GCASPC (Figure 3). Nucleotide sequence of the full-length human GCASPC gene (Figure 4). GCASPC has no coding capability (Figure 5). The expression level of GCASPC in gallbladder cancer cells (Figure 6). Manipulation of GCASPC expression level (Figure 7). Anti-proliferative activity of GCASPC (Figure 8). GCASPC acts in trans (Figure 9). The effect of GCASPC on the protein, activity and mRNA levels of PC (Figure 10). GCASPC destabilizes PC protein (Figure 11). GCASPC directly binds to miR-17-3p (Figure 12).

Long noncoding RNAs (lncRNA) are being implicated in the development of many cancers. Here, we report the discovery of a critical role for the lncRNA GCASPC in determining the progression of gallbladder cancer. Differentially expressed lncRNAs and mRNAs between gallbladder cancer specimens and paired adjacent nontumor tissues from five patients were identified and validated by an expression microarray analysis. Quantitative real-time PCR was used to measure GCASPC levels in tissues from 42 gallbladder cancer patients, and levels of GCASPC were confirmed further in a separate cohort of 89 gallbladder cancer patients. GCASPC was overexpressed or silenced in several gallbladder cancer cell lines where molecular and biological analyses were performed. GCASPC levels were significantly lower in gallbladder cancer than adjacent nontumor tissues and were associated with tumor size, American Joint Committee on Cancer tumor stage, and patient outcomes. GCASPC overexpression suppressed cell proliferation in vitro and in vivo, whereas GCASPC silencing had opposite effects. By RNA pull-down and mass spectrometry, we identified pyruvate carboxylase as an RNA-binding protein that associated with GCASPC. Because GCASPC is a target of miR-17-3p, we confirmed that both miR-17-3p and GCASPC downregulated pyruvate carboxylase level and activity by limiting protein stability. Taken together, our results defined a novel mechanism of lncRNA-regulated cell proliferation in gallbladder cancer, illuminating a new basis for understanding its pathogenicity. Cancer Res; 76(18); 5361–71. ©2016 AACR.

Supplementary Methods. Description of additional methods and procedures used in the study.

Supplemental Table 1-9. Clinical characteristics of 5 GBC patients used for lncRNA array (Table 1). Clinicopathological characterisitcs of 42 GBC patients (Cohort 1) (Table 2). Clinicopathological characterisitcs of 89 GBC patients (Cohort 2) (Table 3). Correlation between GCASPC expression and GBC clinicopathological characteristics in 42 patients (Cohort 1) (Table 4). Univariate and multivariate analyses of OS in 89 GBC patients by Cox regression analysis (Table 5). Proteins in the three bands specific to GCASPC identified by MALDI-TOF mass spectrometry (Table 6). miRNAs binding sites of GCASPC by MirTarget2 (Table 7). Information on antibodies used for correlation analysis (Table 8). Primer sequence used in this study (Table 9). supplemental Figure 1-12. Expression levels of 10 lncRNAs by qRT-PCR in 15 GBC tissues and paired non-tumor tissues (Figure 1). Expression levels of 8 mRNAs by qRT-PCR in 15 GBC tissues and paired non-tumor tissues (Figure 2). Molecular characteristics of GCASPC (Figure 3). Nucleotide sequence of the full-length human GCASPC gene (Figure 4). GCASPC has no coding capability (Figure 5). The expression level of GCASPC in gallbladder cancer cells (Figure 6). Manipulation of GCASPC expression level (Figure 7). Anti-proliferative activity of GCASPC (Figure 8). GCASPC acts in trans (Figure 9). The effect of GCASPC on the protein, activity and mRNA levels of PC (Figure 10). GCASPC destabilizes PC protein (Figure 11). GCASPC directly binds to miR-17-3p (Figure 12).

Epigenetic modifications of histones are associated with development and pathogenesis of disease. Existing approaches cannot provide insights into long-range interactions and represent the average chromatin state. Here we describe BIND&MODIFY, a method using long-read sequencing for profiling histone modifications and transcription factors on individual DNA fibers. We use recombinant fused protein A-M.EcoGII to tether methyltransferase M.EcoGII to protein binding sites to label neighboring regions by methylation. Aggregated BIND&MODIFY signal matches bulk ChIP-seq and CUT&TAG. BIND&MODIFY can simultaneously measure histone modification status, transcription factor binding, and CpG 5mC methylation at single-molecule resolution and also quantifies correlation between local and distal elements. Epigenetic modifications of histones are associated with development and pathogenesis of disease. Existing approaches cannot provide insights into long-range interactions and represent the average chromatin state. Here we describe BIND&MODIFY, a method using long-read sequencing for profiling histone modifications and transcription factors on individual DNA fibers. We use recombinant fused protein A-M.EcoGII to tether methyltransferase M.EcoGII to protein binding sites to label neighboring regions by methylation. Aggregated BIND&MODIFY signal matches bulk ChIP-seq and CUT&TAG. BIND&MODIFY can simultaneously measure histone modification status, transcription factor binding, and CpG 5mC methylation at single-molecule resolution and also quantifies correlation between local and distal elements.

The soil carbon (C) saturation concept suggests an upper limit to the storage of soil organic carbon (SOC). It is set by the mechanisms that protect soil organic matter from mineralization. Biochar has the capacity to protect new C, including rhizodeposits and microbial necromass. However, the decadal-scale mechanisms by which biochar influences the molecular diversity, spatial heterogeneity, and temporal changes in SOC persistence, remain unresolved. Here we show that the soil C storage ceiling of a Ferralsol under subtropical pasture was raised by a second application of Eucalyptus saligna biochar 8.2 years after the first application—the first application raised the soil C storage ceiling by 9.3 Mg new C ha−1 and the second application raised this by another 2.3 Mg new C ha−1. Linking direct visual evidence from one-, two-, and three-dimensional analyses with SOC quantification, we found high spatial heterogeneity of C functional groups that resulted in the retention of rhizodeposits and microbial necromass in microaggregates (53–250 µm) and the mineral fraction (

Aqueous zinc (Zn) batteries have long been considered a potentially more sustainable alternative to lithium-ion batteries because of their better environmental compatibility, enhanced safety and cost advantage. However, in the presence of an aqueous electrolyte, the Zn anode is poised to undergo dendrite failure, corrosion and hydrogen evolution, all of which resonate with each other leading to fast performance degradation. Here, in a break from the current aqueous battery path, we report a low-cost hydrous organic electrolyte involving a hydrated Zn(BF4)2 salt and an ethylene glycol solvent, which not only promotes the in situ formation of a favourable ZnF2 passivation layer to protect Zn from dendrite growth and side reactions but also embraces excellent non-flammability. Remarkably, the present Zn anode sustains a long-term cycling over 4,000 h at a current density of 0.5 mA cm−2 with a high Coulombic efficiency of 99.4% and shows an areal capacity as high as 5 mAh cm−2. Equally intriguingly, the electrolyte can run across a wide temperature range from −30 °C to 40 °C without seriously compromising performance. The Zn//V2O5 full cells with our electrolyte also perform much better in terms of capacity retention than a device with an aqueous ZnSO4 electrolyte. Our findings suggest a promising direction for developing electrolyte solutions for practical Zn batteries which combine safety, performance and sustainability. Aqueous Zn batteries offer safety, but the Zn anodes are vulnerable to dendrite failure and side reaction. Here the authors show a low-cost electrolyte that involves hydrate salt and organic solvent but proves inflammable. The Zn battery cell delivers excellent performance even at a low temperature of −30 °C.

Development of multiple-component catalyst materials is a new trend in electrochemical CO2 reduction reaction (eCO2RR). A new type of metal-oxide interaction is reported here to improve carbon monoxide production via synergistic effect between the CO2-to hydrocarbon selective metal material and CO2-to hydrogen generation oxide material. Cu/Sb2O3 material originates from the hetero-structured CuO/Sb2O3 by a facile two-step hydrolysis and precipitation method, cooperative to inhibit hydrogen evolution or methane product, achieving CO Faradaic efficiency to 92% in CO2 saturated KCl electrolyte at −0.99 V with good stability. The formation of a stable *COOH intermediate by electronic and geometric effects via Cu and Sb2O3 are responsible to promote CO selectivity. Cu-Sb2O3 interface interaction also destabilizes the adsorption *H as well, an intermediate for H2 evolution. This study proposes a versatile design strategy for construction and utilization of metal-oxide interface for eCO2RR.

As the genome has a three-dimensional structure in intracellular space, epigenomic information also has a complex spatial arrangement. However, the majority of epigenetic studies describe locations of methylation marks, chromatin accessibility regions, and histone modifications in the linear dimension. Proper spatial epigenomic information has rarely been obtained. In this study, we designed spatial chromatin accessibility sequencing (SCA-seq) to reveal the three-dimensional map of chromatin accessibility and simultaneously capture the genome conformation. Using SCA-seq, we simultaneously disclosed spatial regulation of chromatin accessibility (e.g. enhancer-promoter contacts), CpG island methylation and spatial insulating functions of the CCCTC-binding factor. We demonstrate that SCA-seq paves the way to explore epigenomic information in the three-dimensional space and extends our knowledge in next-generation genome architecture.

Introduction Core strength training has been extensively used in competitive sports training, achieving remarkable results in the most competitive sports training by maximizing athletes’ strength and accuracy. It is believed that a specific protocol for female university tennis players can bring the same results. Objective Verify the effectiveness of core strength training in the performance of female university tennis players. Methods Randomized controlled trial of female university tennis players (n=40) with a specific core strength training protocol versus traditional strength training methods. Changes in tactical skills pre and post-experiment were compared. Descriptive statistical treatment of the collected results was confronted with current literature. Results Compared with traditional strength training, core strength training proved to be more conducive to developing core strength in female college tennis players. Conclusion Core strength training assists in the development of skills and tactics in female college tennis players. Evidence level II; Therapeutic Studies - Investigating the results. RESUMO Introdução O treino de fortalecimento do core tem sido amplamente utilizado no treinamento esportivo competitivo, alcançando resultados notáveis no treino esportivo mais acirrado ao maximizar a força e precisão dos atletas. Acredita-se que um protocolo específico para as tenistas universitárias possa causar os mesmos resultados. Objetivo Verificar a eficácia do treinamento de força do core no treinamento de tenistas universitárias. Métodos Estudo randomizado controlado de tenistas universitárias (n=40) com protocolo específico de fortalecimento de core para fortalecimento versus métodos tradicionais de treino de força. Foram comparadas as alterações das habilidades táticas pré e pós experimento. O tratamento estatístico descritivo dos resultados coletados foi confrontado com a literatura atual. Resultados Comparado com o treinamento de força tradicional, o treinamento de força do core revelou-se mais propício ao desenvolvimento da força do core em tenistas universitárias. Conclusão O treinamento de força do core auxilia no desenvolvimento da habilidade e tática das tenistas universitárias. Nível de evidência II; Estudos terapêuticos - Investigação de resultados. RESUMEN Introducción El entrenamiento de la fuerza del core se ha utilizado ampliamente en el entrenamiento deportivo de competición, logrando resultados notables en el entrenamiento deportivo más competitivo al maximizar la fuerza y la precisión de los atletas. Se cree que un protocolo específico para los tenistas universitarios puede provocar los mismos resultados. Objetivo Comprobar la eficacia del entrenamiento de la fuerza del core en el entrenamiento de las tenistas universitarias. Métodos Estudio controlado aleatorio de jugadoras de tenis universitarias (n=40) con un protocolo específico de entrenamiento de la fuerza del core para el fortalecimiento frente a los métodos tradicionales de entrenamiento de la fuerza. Se compararon los cambios en las habilidades tácticas antes y después del experimento. El tratamiento estadístico descriptivo de los resultados recogidos se confrontó con la literatura actual. Resultados En comparación con el entrenamiento de fuerza tradicional, el entrenamiento de fuerza del core demostró ser más propicio para el desarrollo de la fuerza del core en las tenistas universitarias. Conclusión El entrenamiento de la fuerza del core ayuda al desarrollo de la habilidad y la táctica de las tenistas universitarias. Nivel de evidencia II; Estudios terapéuticos - Investigación de resultados.

Here we describe a powerful method, BIND&MODIFY, for probing histone modifications and transcription factors at single molecular level. This is the Protocol V2. Our approach used the recombinant fused protein A-M.EcoGII, which tethers the methyltransferase M.EcoGII to the protein binding sites and locally labels the neighboring DNA regions via artificial methylations. This method could reveal ingle-molecule heterogenous histone modification status and CpG methylation at the same time, and could enable quantify the correlation between the distal elements. Further applications based on this method's concept could be applied to probe multiple protein binding events on the same single molecular DNA. The method proposed herein may soon become an essential tool for third-generation sequencing in the future.

Refereed/Peer-reviewed Soil organic carbon management is a nature-based carbon dioxide removal technology at the same time contributing to soil health and agricultural productivity. The soil science communities are refuting the traditional assumptions of the nature of soil organic matter (SOM) as based on 'humic substances' that are operationally-defined and have not been observed by contemporary, in situ spectromicroscopic techniques. Instead, new theories suggest that the interactions between molecular diversity of organic compounds, their spatial heterogeneity and temporal variability controls the formation and persistence of SOM. A mechanistic understanding of these processes occurring within organo-mineral and organo-organic assemblages requires non-invasive techniques that minimize any disturbance to the physical and chemical integrity of the sample. Here, we present a theory-driven review where a combination of in situ methods serve as potential solutions to better understand the persistence and dynamics of SOM and its effects on nutrient distribution at a micro- and nano-scale. We explore underlying theories in light of advances in available methodologies, their historical development and future opportunities. Examples of interdisciplinary approaches that have been utilized in other areas of science but not in soils offer both deductive and inductive analytical opportunities. We show how different conceptual methods across scales inform each other, and how important and indispensable high-resolution investigations are to resolving next-generation questions.

We synthesized 20 years of research to explain the interrelated processes that determine soil and plant responses to biochar. The properties of biochar and its effects within agricultural ecosystems largely depend on feedstock and pyrolysis conditions. We describe three stages of reactions of biochar in soil: dissolution (1–3 weeks); reactive surface development (1–6 months); and aging (beyond 6 months). As biochar ages, it is incorporated into soil aggregates, protecting the biochar carbon and promoting the stabilization of rhizodeposits and microbial products. Biochar carbon persists in soil for hundreds to thousands of years. By increasing pH, porosity, and water availability, biochars can create favorable conditions for root development and microbial functions. Biochars can catalyze biotic and abiotic reactions, particularly in the rhizosphere, that increase nutrient supply and uptake by plants, reduce phytotoxins, stimulate plant development, and increase resilience to disease and environmental stressors. Meta-analyses found that, on average, biochars increase P availability by a factor of 4.6; decrease plant tissue concentration of heavy metals by 17%–39%; build soil organic carbon through negative priming by 3.8% (range −21% to +20%); and reduce non-CO greenhouse gas emissions from soil by 12%–50%. Meta-analyses show average crop yield increases of 10%–42% with biochar addition, with greatest increases in low-nutrient P-sorbing acidic soils (common in the tropics), and in sandy soils in drylands due to increase in nutrient retention and water holding capacity. Studies report a wide range of plant responses to biochars due to the diversity of biochars and contexts in which biochars have been applied. Crop yields increase strongly if site-specific soil constraints and nutrient and water limitations are mitigated by appropriate biochar formulations. Biochars can be tailored to address site constraints through feedstock selection, by modifying pyrolysis conditions, through pre- or post-production treatments, or co-application with organic or mineral fertilizers. We demonstrate how, when used wisely, biochar mitigates climate change and supports food security and the circular economy., Program of Competitive Growth of Kazan Federal University and the “RUDN University program 5-100” La Trobe University. Grant Number: LTU SFWE RFA 2000004349

Biochars have potential to reduce soil acidity and Al3+ toxicity, and increase the availability of soil nutrients. This study aimed to compare the effectiveness of biochars and their raw feedstocks in amelioration of soil acidity. Ten ameliorants comprising of five biochars (pyrolyzed at 550°C) and their corresponding feedstocks (wheat chaff, canola stubble, vetch hay, lucerne pellets, and poultry litter) were added (1% of soil weight) to sandy Tenosol and loamy Chromosol with both having similar Al3+ concentrations but Chromosol having nine times greater pH buffer capacity. The soils with the ameliorants were incubated for 7 weeks (incubation phase), before being planted with an Al-sensitive wheat (ES8) for 18 days (plant phase). Biochars outperformed their feedstocks in increasing soil pH, leading to a significant reduction of Al3+ toxicity. Biochar additions increased shoot growth by 137‒341% for Tenosol and 10‒295% for Chromosol, whereas their feedstocks increased shoot growth by 25‒233% for Tenosol and -38‒136% for Chromosol. Poultry-litter biochar increased soil pH greater than the corresponding poultry-litter treatments by 1.59 units in the Tenosol and 0.79 units in the Chromosol at the end of the plant phase. In addition, all organic amendments (except wheat-chaff and its biochar) significantly increased shoot P concentrations with poultry-litter biochar achieving the highest Olsen P and shoot P concentrations in both soils. Evidently, high alkalinity and nutrient contents of poultry-litter biochar resulted in the greatest increases in soil pH and shoot biomass in both soils. Biochars were more effective at ameliorating soil acidity than their corresponding feedstocks primarily via increasing soil pH and supplying plant nutrients, depending on soil type. Poultry-litter biochar was the most effective on both soils.

Excess anion uptake in the form of nitrate has been shown to reduce soil acidification. The question is to what extent the deep placement of calcium nitrate can increase this root-induced alkalization in reducing subsurface soil acidity. Wheat and canola were grown for 35 days in reconstructed soil columns comprising of topsoil (pHCaCl2 5.4) in 0–10 cm and subsurface soil (pHCaCl2 4.8) in 10–50 cm. Two forms of 15N-enriched fertilizers (urea versus calcium nitrate at 237 mg N per column) with or without P fertilizer (NaH2PO4 at 99 mg P per column) were placed at 0–10, 10–20, or 20–30 cm depth. Root proliferation, rhizosphere pH, and shoot 15N recovery were quantified. Uptake of Ca(NO3)2 increased pH up to 0.5 and 0.2 units in the rhizosphere and bulk soil, respectively, in all treated layers compared to those with urea. The combined application of nitrate and P fertilizer facilitated plant nitrate uptake and hence rhizosphere alkalization. Significant increases up to 10% and 22% in shoot and root biomass, respectively, were observed in the combination of nitrate and P treatments compared with the combined urea and P treatments. The nitrate treatment significantly increased the 15N recovery of fertilizer in both wheat and canola up to 20% compared with the urea treatment. The increased nitrate uptake reduced subsurface acidity. The combination of nitrate and P treatment can facilitate alkalinity movement downward, hence ameliorating subsurface soil acidity.

Zinc-anode-based batteries have been widely studied because of their low cost, high capacity, and high energy density. However, the formation of dendrites on the zinc anode during cycling severely ...

Great progress has been made in the development of cathode materials for Al-metal batteries. However, the in-depth study of Al anodes, especially the battery instability caused by Al dendrite growth, has not received much attention. In this work, we have identified the in-situ formation of Al dendrite growth, which is proved to bottleneck the practical use of Al-metal batteries. The dendrite formation severely affects battery performance, such as voltage and efficiency fluctuations, unstable cycling, etc. To further demonstrate the detailed growing process of dendrites, we make a comprehensive investigation into the interfacial chemistry of Al anode. We have found that the naturally formed Al2O3 surface film is dissolved in the ionic liquid electrolyte during Al plating, accompanied by the formation of solid-electrolyte interphase containing Al-Cl and Al-O like species on the anode surface before dendrite growth. To suppress this dendrite growth, we propose the use of porous Al, which provides a homogeneous ion flux and decreases the local current density. As a result, the porous anode maintains stable cycling over a wide range of current densities and areal capacities. The Al-graphite battery shows stable cycling up to 18000 times without capacity decay. This work suggests the significance of suppressing dendrite growth for the real applications and commercialization of Al-metal batteries and will draw attention to the battery design from the anode side.

Conventional approaches to studying 5mC marks in single cells or samples with picogram input DNA amounts usually suffer from low genome coverage due to DNA degradation. Many methods have been developed to optimize the library construction efficiency for bisulfite-treated DNA. However, most of these approaches ignored the amplification bias of bisulfite-treated DNA, which leads to shallow genome coverage. In this study, we developed the T7-assisted enzymatic methyl-sequencing method (TEAM-seq), which adopts enzymatic conversion to minimize DNA degradation and T7 polymerase-assisted unbiased amplification. We demonstrate that TEAM-seq delivered, to the best of our knowledge, the highest reported coverage(70% for 100pg, 35% for 20pg) of single cell genomes in whole-genome 5mC sequencing.

Volumetric and areal capacitance are as important as gravimetric capacitance for small energy storage devices. However, achieving both a high volumetric and a high areal capacitance is still a big challenge. Here we report a dense redox organic molecules/graphene network, in which highly redox active sodium anthraquinone-2-sulfonate (AQS) molecules are anchored on interconnected and highly conductive graphene sheets by noncovalent π–π interactions to form high-performance supercapacitors (SCs). The AQS/graphene (AQS/G) has a high volumetric specific capacitance of up to 650 F cm−3 and an excellent rate capability (422 F cm−3 even at 30 A g−1), as well as a good cycling stability. A maximum areal specific capacitance of 13.3 F cm−2 is achieved at a high mass loading of 32 mg cm−2 (200 μm in thickness), which is amongst the highest values recorded for organic-based materials for SCs. An asymmetric SC constructed with AQS/G and RuO2/graphene delivers a maximum volumetric energy density of 44 W h L−1. This outstanding performance is attributed to the excellent electron conduction and ion transport provided by the dense but interconnected graphene network. This work suggests a new way for organic-based high-performance electrode materials to be used in electrochemical energy storage devices.