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Showing papers in "Nature Communications in 2018"


Journal ArticleDOI
TL;DR: Physical structure is known to contribute to the appearance of bird plumage through structural color and specular reflection, but a third mechanism, structural absorption, leads to low reflectance and super black color in birds of paradise feathers.
Abstract: Many studies have shown how pigments and internal nanostructures generate color in nature. External surface structures can also influence appearance, such as by causing multiple scattering of light (structural absorption) to produce a velvety, super black appearance. Here we show that feathers from five species of birds of paradise (Aves: Paradisaeidae) structurally absorb incident light to produce extremely low-reflectance, super black plumages. Directional reflectance of these feathers (0.05-0.31%) approaches that of man-made ultra-absorbent materials. SEM, nano-CT, and ray-tracing simulations show that super black feathers have titled arrays of highly modified barbules, which cause more multiple scattering, resulting in more structural absorption, than normal black feathers. Super black feathers have an extreme directional reflectance bias and appear darkest when viewed from the distal direction. We hypothesize that structurally absorbing, super black plumage evolved through sensory bias to enhance the perceived brilliance of adjacent color patches during courtship display.

5,916 citations


Journal ArticleDOI
TL;DR: FastANI is developed, a method to compute ANI using alignment-free approximate sequence mapping, and it is shown 95% ANI is an accurate threshold for demarcating prokaryotic species by analyzing about 90,000 proKaryotic genomes.
Abstract: A fundamental question in microbiology is whether there is continuum of genetic diversity among genomes, or clear species boundaries prevail instead. Whole-genome similarity metrics such as Average Nucleotide Identity (ANI) help address this question by facilitating high resolution taxonomic analysis of thousands of genomes from diverse phylogenetic lineages. To scale to available genomes and beyond, we present FastANI, a new method to estimate ANI using alignment-free approximate sequence mapping. FastANI is accurate for both finished and draft genomes, and is up to three orders of magnitude faster compared to alignment-based approaches. We leverage FastANI to compute pairwise ANI values among all prokaryotic genomes available in the NCBI database. Our results reveal clear genetic discontinuity, with 99.8% of the total 8 billion genome pairs analyzed conforming to >95% intra-species and <83% inter-species ANI values. This discontinuity is manifested with or without the most frequently sequenced species, and is robust to historic additions in the genome databases. Average Nucleotide Identity (ANI) is a robust and useful measure to gauge genetic relatedness between two genomes. Here, the authors develop FastANI, a method to compute ANI using alignment-free approximate sequence mapping, and show 95% ANI is an accurate threshold for demarcating prokaryotic species by analyzing about 90,000 prokaryotic genomes.

2,176 citations


Journal ArticleDOI
TL;DR: In vivo generation of mouse models carrying clinically relevant mutations using C→T and A→G editors is demonstrated, making it feasible to model and potentially cure relevant genetic diseases.
Abstract: A recently developed adenine base editor (ABE) efficiently converts A to G and is potentially useful for clinical applications. However, its precision and efficiency in vivo remains to be addressed. Here we achieve A-to-G conversion in vivo at frequencies up to 100% by microinjection of ABE mRNA together with sgRNAs. We then generate mouse models harboring clinically relevant mutations at Ar and Hoxd13, which recapitulates respective clinical defects. Furthermore, we achieve both C-to-T and A-to-G base editing by using a combination of ABE and SaBE3, thus creating mouse model harboring multiple mutations. We also demonstrate the specificity of ABE by deep sequencing and whole-genome sequencing (WGS). Taken together, ABE is highly efficient and precise in vivo, making it feasible to model and potentially cure relevant genetic diseases. CRISPR-based base editors allow for single nucleotide genome editing in a range of organisms. Here the authors demonstrate the in vivo generation of mouse models carrying clinically relevant mutations using C→T and A→G editors.

2,114 citations


Journal ArticleDOI
TL;DR: Results add further challenge to the assumption that carotenoids are directly involved in supporting physiological function in vertebrate animals, and suggest that they may play little to no direct role in key physiological processes in birds.
Abstract: Dietary carotenoids have been proposed to boost immune system and antioxidant functions in vertebrate animals, but studies aimed at testing these physiological functions of carotenoids have often failed to find support. Here we subject yellow canaries (Serinus canaria), which possess high levels of carotenoids in their tissue, and white recessive canaries, which possess a knockdown mutation that results in very low levels of tissue carotenoids, to oxidative and pathogen challenges. Across diverse measures of physiological performance, we detect no differences between carotenoid-rich yellow and carotenoid-deficient white canaries. These results add further challenge to the assumption that carotenoids are directly involved in supporting physiological function in vertebrate animals. While some dietary carotenoids provide indirect benefits as retinoid precursors, our observations suggest that carotenoids themselves may play little to no direct role in key physiological processes in birds.

1,398 citations


Journal ArticleDOI
TL;DR: An ambient-driven actuator that takes advantage of inherent nanoscale molecular channels within a commercial perfluorosulfonic acid ionomer (PFSA) film, fabricated by simple solution processing to realize a rapid response, self-adaptive, and exceptionally stable actuation.
Abstract: The ability to achieve simultaneous intrinsic deformation with fast response in commercially available materials that can safely contact skin continues to be an unresolved challenge for artificial actuating materials. Rather than using a microporous structure, here we show an ambient-driven actuator that takes advantage of inherent nanoscale molecular channels within a commercial perfluorosulfonic acid ionomer (PFSA) film, fabricated by simple solution processing to realize a rapid response, self-adaptive, and exceptionally stable actuation. Selective patterning of PFSA films on an inert soft substrate (polyethylene terephthalate film) facilitates the formation of a range of different geometries, including a 2D (two-dimensional) roll or 3D (three-dimensional) helical structure in response to vapor stimuli. Chemical modification of the surface allowed the development of a kirigami-inspired single-layer actuator for personal humidity and heat management through macroscale geometric design features, to afford a bilayer stimuli-responsive actuator with multicolor switching capability. Intrinsic deformation with fast response in commercially available materials that can safely contact skin continues to be a challenge for artificial actuating materials. Here the authors incorporate nanoscale molecular channels within perfluorosulfonic acid ionomer for self-adaptive and ambient-driven actuation.

1,395 citations


Journal ArticleDOI
TL;DR: The principles behind targeted delivery approaches are reviewed to determine potential reasons for their limited clinical translation and success and criteria and considerations that must be taken into account for the development of novel actively targeted NCs are proposed.
Abstract: Targeted delivery approaches for cancer therapeutics have shown a steep rise over the past few decades. However, compared to the plethora of successful pre-clinical studies, only 15 passively targeted nanocarriers (NCs) have been approved for clinical use and none of the actively targeted NCs have advanced past clinical trials. Herein, we review the principles behind targeted delivery approaches to determine potential reasons for their limited clinical translation and success. We propose criteria and considerations that must be taken into account for the development of novel actively targeted NCs. We also highlight the possible directions for the development of successful tumor targeting strategies.

1,335 citations


Journal ArticleDOI
TL;DR: A simple and robust plate-based single-cell ATAC-seq method that works in fresh and cryopreserved cells and identifies distinct immune cell types and reveal cell type-specific regulatory regions and related transcription factors is developed.
Abstract: The assay for transposase-accessible chromatin using sequencing (ATAC-seq) is widely used to identify regulatory regions throughout the genome. However, very few studies have been performed at the single cell level (scATAC-seq) due to technical challenges. Here we developed a simple and robust plate-based scATAC-seq method, combining upfront bulk Tn5 tagging with single-nuclei sorting. We demonstrate that our method works robustly across various systems, including fresh and cryopreserved cells from primary tissues. By profiling over 3000 splenocytes, we identify distinct immune cell types and reveal cell type-specific regulatory regions and related transcription factors. ATAC-seq is widely used to identify regulatory regions in the genome. Here the authors develop a simple and robust plate-based single-cell ATAC-seq method that works in fresh and cryopreserved cells.

1,260 citations


Journal ArticleDOI
TL;DR: A brief history of gene-editing tools is presented and the wide range of CRISPR-based genome-targeting tools are described, to conclude with future directions and the broader impact ofCRISPR technologies.
Abstract: CRISPR is becoming an indispensable tool in biological research. Once known as the bacterial immune system against invading viruses, the programmable capacity of the Cas9 enzyme is now revolutionizing diverse fields of medical research, biotechnology, and agriculture. CRISPR-Cas9 is no longer just a gene-editing tool; the application areas of catalytically impaired inactive Cas9, including gene regulation, epigenetic editing, chromatin engineering, and imaging, now exceed the gene-editing functionality of WT Cas9. Here, we will present a brief history of gene-editing tools and describe the wide range of CRISPR-based genome-targeting tools. We will conclude with future directions and the broader impact of CRISPR technologies.

1,092 citations


Journal ArticleDOI
Fang Wan1, Linlin Zhang1, Xi Dai1, Xinyu Wang1, Zhiqiang Niu1, Jun Chen1 
TL;DR: A design with sodium vanadate hydrate as cathode is shown, allowing simultaneous proton and zinc-ion insertion/extraction and enhanced performance and the quasi-solid-state zinc/sodium vanadates hydrate battery is a good candidate for flexible energy storage device.
Abstract: Rechargeable aqueous zinc-ion batteries are promising energy storage devices due to their high safety and low cost. However, they remain in their infancy because of the limited choice of positive electrodes with high capacity and satisfactory cycling performance. Furthermore, their energy storage mechanisms are not well established yet. Here we report a highly reversible zinc/sodium vanadate system, where sodium vanadate hydrate nanobelts serve as positive electrode and zinc sulfate aqueous solution with sodium sulfate additive is used as electrolyte. Different from conventional energy release/storage in zinc-ion batteries with only zinc-ion insertion/extraction, zinc/sodium vanadate hydrate batteries possess a simultaneous proton, and zinc-ion insertion/extraction process that is mainly responsible for their excellent performance, such as a high reversible capacity of 380 mAh g–1 and capacity retention of 82% over 1000 cycles. Moreover, the quasi-solid-state zinc/sodium vanadate hydrate battery is also a good candidate for flexible energy storage device. Rechargeable zinc-ion batteries are promising energy storage devices but suffer from the limited choice of positive electrodes. Here Niu and co-workers show a design with sodium vanadate hydrate as cathode, allowing simultaneous proton and zinc-ion insertion/extraction and enhanced performance.

1,010 citations


Journal ArticleDOI
TL;DR: This corrects the article DOI: 10.1038/ncomms14433 to indicate that the author of the paper is a doctor of medicine rather than a scientist, as previously reported.
Abstract: Nature Communications 8: Article number: 14433 (2017) Published online 14 February 2017; Updated 20 April 2018 In this Article, a subset of the H3K27ac ChIP-seq data (15 benign meningiomas and 2 dura samples (Sample IDs: MN-297, MN-288, MN-292, MN-163, MN-1037, MN-105, MN-201, MN-249, MN-191, MN-1066, MN-169, MN-291, MN-24, MN-79, MN-1044, CONTROL1, CONTROL2) was reported previously in a publication by the corresponding author1.

998 citations


Journal ArticleDOI
TL;DR: Yang et al. modify the oxide based electron transporting layer with organic acid and obtain planar-type cells with high certified efficiency of 21.5% and decent stability and success in suppressing hysteresis and record efficiency for planars-type devices using EDTA-complexed tin oxide (SnO2) electron-transport layer.
Abstract: Even though the mesoporous-type perovskite solar cell (PSC) is known for high efficiency, its planar-type counterpart exhibits lower efficiency and hysteretic response. Herein, we report success in suppressing hysteresis and record efficiency for planar-type devices using EDTA-complexed tin oxide (SnO2) electron-transport layer. The Fermi level of EDTA-complexed SnO2 is better matched with the conduction band of perovskite, leading to high open-circuit voltage. Its electron mobility is about three times larger than that of the SnO2. The record power conversion efficiency of planar-type PSCs with EDTA-complexed SnO2 increases to 21.60% (certified at 21.52% by Newport) with negligible hysteresis. Meanwhile, the low-temperature processed EDTA-complexed SnO2 enables 18.28% efficiency for a flexible device. Moreover, the unsealed PSCs with EDTA-complexed SnO2 degrade only by 8% exposed in an ambient atmosphere after 2880 h, and only by 14% after 120 h under irradiation at 100 mW cm−2. The development of high efficiency planar-type perovskite solar cell has been lagging behind the mesoporous-type counterpart. Here Yang et al. modify the oxide based electron transporting layer with organic acid and obtain planar-type cells with high certified efficiency of 21.5% and decent stability.

Journal ArticleDOI
Jarrod R. McClean1, Sergio Boixo1, Vadim Smelyanskiy1, Ryan Babbush1, Hartmut Neven1 
TL;DR: In this article, the authors show that for a wide class of reasonable parameterized quantum circuits, the probability that the gradient along any reasonable direction is non-zero to some fixed precision is exponentially small as a function of the number of qubits.
Abstract: Many experimental proposals for noisy intermediate scale quantum devices involve training a parameterized quantum circuit with a classical optimization loop. Such hybrid quantum-classical algorithms are popular for applications in quantum simulation, optimization, and machine learning. Due to its simplicity and hardware efficiency, random circuits are often proposed as initial guesses for exploring the space of quantum states. We show that the exponential dimension of Hilbert space and the gradient estimation complexity make this choice unsuitable for hybrid quantum-classical algorithms run on more than a few qubits. Specifically, we show that for a wide class of reasonable parameterized quantum circuits, the probability that the gradient along any reasonable direction is non-zero to some fixed precision is exponentially small as a function of the number of qubits. We argue that this is related to the 2-design characteristic of random circuits, and that solutions to this problem must be studied. Gradient-based hybrid quantum-classical algorithms are often initialised with random, unstructured guesses. Here, the authors show that this approach will fail in the long run, due to the exponentially-small probability of finding a large enough gradient along any direction.

Journal ArticleDOI
TL;DR: It is shown that reducing molecular friction by using highly crystalline graphite and mild oxidizing conditions is the key to high quality graphene.
Abstract: Oxidative wet-chemical delamination of graphene from graphite is expected to become a scalable production method. However, the formation process of the intermediate stage-1 graphite sulfate by sulfuric acid intercalation and its subsequent oxidation are poorly understood and lattice defect formation must be avoided. Here, we demonstrate film formation of micrometer-sized graphene flakes with lattice defects down to 0.02% and visualize the carbon lattice by transmission electron microscopy at atomic resolution. Interestingly, we find that only well-ordered, highly crystalline graphite delaminates into oxo-functionalized graphene, whereas other graphite grades do not form a proper stage-1 intercalate and revert back to graphite upon hydrolysis. Ab initio molecular dynamics simulations show that ideal stacking and electronic oxidation of the graphite layers significantly reduce the friction of the moving sulfuric acid molecules, thereby facilitating intercalation. Furthermore, the evaluation of the stability of oxo-species in graphite sulfate supports an oxidation mechanism that obviates intercalation of the oxidant. Scalable graphene production from graphite via an intercalation-oxidation-reduction process is still hampered by low reproducibility and many lattice defects. Here, the authors show that reducing molecular friction by using highly crystalline graphite and mild oxidizing conditions is the key to high quality graphene.

Journal ArticleDOI
TL;DR: A skin-inspired highly stretchable and conformable matrix network (SCMN) that successfully expands the e-skin sensing functionality including but not limited to temperature, in-plane strain, humidity, light, magnetic field, pressure, and proximity is presented.
Abstract: Mechanosensation electronics (or Electronic skin, e-skin) consists of mechanically flexible and stretchable sensor networks that can detect and quantify various stimuli to mimic the human somatosensory system, with the sensations of touch, heat/cold, and pain in skin through various sensory receptors and neural pathways. Here we present a skin-inspired highly stretchable and conformable matrix network (SCMN) that successfully expands the e-skin sensing functionality including but not limited to temperature, in-plane strain, humidity, light, magnetic field, pressure, and proximity. The actualized specific expandable sensor units integrated on a structured polyimide network, potentially in three-dimensional (3D) integration scheme, can also fulfill simultaneous multi-stimulus sensing and achieve an adjustable sensing range and large-area expandability. We further construct a personalized intelligent prosthesis and demonstrate its use in real-time spatial pressure mapping and temperature estimation. Looking forward, this SCMN has broader applications in humanoid robotics, new prosthetics, human-machine interfaces, and health-monitoring technologies.

Journal ArticleDOI
TL;DR: It is established that graft-derived macrophages acquire, over time, microglia characteristics, including ramified morphology, longevity, radio-resistance and clonal expansion, however, even after prolonged CNS residence, transcriptomes and chromatin accessibility landscapes of engrafted, BM-derived Macrophages remain distinct from yolk sac-derived host microglial.
Abstract: Microglia are yolk sac-derived macrophages residing in the parenchyma of brain and spinal cord, where they interact with neurons and other glial. After different conditioning paradigms and bone marrow (BM) or hematopoietic stem cell (HSC) transplantation, graft-derived cells seed the brain and persistently contribute to the parenchymal brain macrophage compartment. Here we establish that graft-derived macrophages acquire, over time, microglia characteristics, including ramified morphology, longevity, radio-resistance and clonal expansion. However, even after prolonged CNS residence, transcriptomes and chromatin accessibility landscapes of engrafted, BM-derived macrophages remain distinct from yolk sac-derived host microglia. Furthermore, engrafted BM-derived cells display discrete responses to peripheral endotoxin challenge, as compared to host microglia. In human HSC transplant recipients, engrafted cells also remain distinct from host microglia, extending our finding to clinical settings. Collectively, our data emphasize the molecular and functional heterogeneity of parenchymal brain macrophages and highlight potential clinical implications for HSC gene therapies aimed to ameliorate lysosomal storage disorders, microgliopathies or general monogenic immuno-deficiencies. Irradiation depletes brain microglia cells and induces replenishment of the pool by bone marrow (BM)-derived macrophage. Here the authors show, using mouse BM chimera, that BM-derived macrophages establish long-term residency in the brain, but remain distinct from resident microglia in their transcriptome and gene accessibility landscape.

Journal ArticleDOI
TL;DR: Using a range of ocean temperature data including global records of daily satellite observations, daily in situ measurements and gridded monthly in situ-based data sets, this work identifies significant increases in marine heatwaves over the past century.
Abstract: Heatwaves are important climatic extremes in atmospheric and oceanic systems that can have devastating and long-term impacts on ecosystems, with subsequent socioeconomic consequences. Recent prominent marine heatwaves have attracted considerable scientific and public interest. Despite this, a comprehensive assessment of how these ocean temperature extremes have been changing globally is missing. Using a range of ocean temperature data including global records of daily satellite observations, daily in situ measurements and gridded monthly in situ-based data sets, we identify significant increases in marine heatwaves over the past century. We find that from 1925 to 2016, global average marine heatwave frequency and duration increased by 34% and 17%, respectively, resulting in a 54% increase in annual marine heatwave days globally. Importantly, these trends can largely be explained by increases in mean ocean temperatures, suggesting that we can expect further increases in marine heatwave days under continued global warming.

Journal ArticleDOI
TL;DR: Structurally reinforced polyaniline-intercalated MnO2 nanolayers that boost performance by eliminating phase transformation are reported, which sheds light on the design of advanced cathodes for aqueous zinc-ion batteries.
Abstract: Rechargeable zinc-manganese dioxide batteries that use mild aqueous electrolytes are attracting extensive attention due to high energy density and environmental friendliness. Unfortunately, manganese dioxide suffers from substantial phase changes (e.g., from initial α-, β-, or γ-phase to a layered structure and subsequent structural collapse) during cycling, leading to very poor stability at high charge/discharge depth. Herein, cyclability is improved by the design of a polyaniline-intercalated layered manganese dioxide, in which the polymer-strengthened layered structure and nanoscale size of manganese dioxide serves to eliminate phase changes and facilitate charge storage. Accordingly, an unprecedented stability of 200 cycles with at a high capacity of 280 mA h g-1 (i.e., 90% utilization of the theoretical capacity of manganese dioxide) is achieved, as well as a long-term stability of 5000 cycles at a utilization of 40%. The encouraging performance sheds light on the design of advanced cathodes for aqueous zinc-ion batteries.

Journal ArticleDOI
TL;DR: In this paper, the authors review emerging data suggesting that microbial tryptophan catabolites resulting from proteolysis are influencing host health and suggest that these metabolites activate the immune system through binding to the aryl hydrocarbon receptor (AHR), enhance the intestinal epithelial barrier, stimulate gastrointestinal motility, as well as secretion of gut hormones, exert anti-inflammatory, anti-oxidative or toxic effects in systemic circulation, and putatively modulate gut microbial composition.
Abstract: Accumulating evidence implicates metabolites produced by gut microbes as crucial mediators of diet-induced host-microbial cross-talk. Here, we review emerging data suggesting that microbial tryptophan catabolites resulting from proteolysis are influencing host health. These metabolites are suggested to activate the immune system through binding to the aryl hydrocarbon receptor (AHR), enhance the intestinal epithelial barrier, stimulate gastrointestinal motility, as well as secretion of gut hormones, exert anti-inflammatory, anti-oxidative or toxic effects in systemic circulation, and putatively modulate gut microbial composition. Tryptophan catabolites thus affect various physiological processes and may contribute to intestinal and systemic homeostasis in health and disease.

Journal ArticleDOI
TL;DR: A soft carbon anode, namely highly nitrogen-doped soft carbon nanofibers, with superior rate capability and cyclability based on a surface dominated charge storage mechanism is reported.
Abstract: Potassium-ion batteries are a promising alternative to lithium-ion batteries. However, it is challenging to achieve fast charging/discharging and long cycle life with the current electrode materials because of the sluggish potassiation kinetics. Here we report a soft carbon anode, namely highly nitrogen-doped carbon nanofibers, with superior rate capability and cyclability. The anode delivers reversible capacities of 248 mAh g–1 at 25 mA g–1 and 101 mAh g–1 at 20 A g–1, and retains 146 mAh g–1 at 2 A g–1 after 4000 cycles. Surface-dominated K-storage is verified by quantitative kinetics analysis and theoretical investigation. A full cell coupling the anode and Prussian blue cathode delivers a reversible capacity of 195 mAh g–1 at 0.2 A g–1. Considering the cost-effectiveness and material sustainability, our work may shed some light on searching for K-storage materials with high performance. The development of potassium ion batteries calls for cheap, sustainable, and high-performance electrode materials. Here, the authors report a highly nitrogen-doped soft carbon anode that exhibits superior rate capability and cyclability based on a surface dominated charge storage mechanism.

Journal ArticleDOI
TL;DR: A map of the cellular landscape of the human liver using single-cell RNA sequencing is reported, and distinct populations of intrahepatic macrophages that may play specific roles in liver disease are identified.
Abstract: The liver is the largest solid organ in the body and is critical for metabolic and immune functions. However, little is known about the cells that make up the human liver and its immune microenvironment. Here we report a map of the cellular landscape of the human liver using single-cell RNA sequencing. We provide the transcriptional profiles of 8444 parenchymal and non-parenchymal cells obtained from the fractionation of fresh hepatic tissue from five human livers. Using gene expression patterns, flow cytometry, and immunohistochemical examinations, we identify 20 discrete cell populations of hepatocytes, endothelial cells, cholangiocytes, hepatic stellate cells, B cells, conventional and non-conventional T cells, NK-like cells, and distinct intrahepatic monocyte/macrophage populations. Together, our study presents a comprehensive view of the human liver at single-cell resolution that outlines the characteristics of resident cells in the liver, and in particular provides a map of the human hepatic immune microenvironment.

Journal ArticleDOI
TL;DR: It is shown in grassland mesocosms that drought promotes destabilising properties in soil bacterial, but not fungal, co-occurrence networks, and that changes in bacterial communities link more strongly to soil functioning during recovery than do changes in fungal communities.
Abstract: Soil microbial communities play a crucial role in ecosystem functioning, but it is unknown how co-occurrence networks within these communities respond to disturbances such as climate extremes This represents an important knowledge gap because changes in microbial networks could have implications for their functioning and vulnerability to future disturbances Here, we show in grassland mesocosms that drought promotes destabilising properties in soil bacterial, but not fungal, co-occurrence networks, and that changes in bacterial communities link more strongly to soil functioning during recovery than do changes in fungal communities Moreover, we reveal that drought has a prolonged effect on bacterial communities and their co-occurrence networks via changes in vegetation composition and resultant reductions in soil moisture Our results provide new insight in the mechanisms through which drought alters soil microbial communities with potential long-term consequences, including future plant community composition and the ability of aboveground and belowground communities to withstand future disturbances

Journal ArticleDOI
TL;DR: A hybrid catalyst constructed by iron and dinickel phosphides on nickel foams that drives both the hydrogen and oxygen evolution reactions well in base, and thus substantially expedites overall water splitting is reported, which outperforms the integrated iridium (IV) oxide and platinum couple (1.57 V).
Abstract: Water electrolysis is an advanced energy conversion technology to produce hydrogen as a clean and sustainable chemical fuel, which potentially stores the abundant but intermittent renewable energy sources scalably. Since the overall water splitting is an uphill reaction in low efficiency, innovative breakthroughs are desirable to greatly improve the efficiency by rationally designing non-precious metal-based robust bifunctional catalysts for promoting both the cathodic hydrogen evolution and anodic oxygen evolution reactions. We report a hybrid catalyst constructed by iron and dinickel phosphides on nickel foams that drives both the hydrogen and oxygen evolution reactions well in base, and thus substantially expedites overall water splitting at 10 mA cm−2 with 1.42 V, which outperforms the integrated iridium (IV) oxide and platinum couple (1.57 V), and are among the best activities currently. Especially, it delivers 500 mA cm−2 at 1.72 V without decay even after the durability test for 40 h, providing great potential for large-scale applications.

Journal ArticleDOI
TL;DR: The authors leverage strongly localised plasmonic heating of graphene carriers to detect a second photothermoelectric effect occurring across a homogeneous channel in the presence of an electronic temperature gradient.
Abstract: Graphene has emerged as a promising material for optoelectronics due to its potential for ultrafast and broad-band photodetection. The photoresponse of graphene junctions is characterized by two competing photocurrent generation mechanisms: a conventional photovoltaic effect and a more dominant hot-carrier-assisted photothermoelectric (PTE) effect. The PTE effect is understood to rely on variations in the Seebeck coefficient through the graphene doping profile. A second PTE effect can occur across a homogeneous graphene channel in the presence of an electronic temperature gradient. Here, we study the latter effect facilitated by strongly localised plasmonic heating of graphene carriers in the presence of nanostructured electrical contacts resulting in electronic temperatures of the order of 2000 K. At certain conditions, the plasmon-induced PTE photocurrent contribution can be isolated. In this regime, the device effectively operates as a sensitive electronic thermometer and as such represents an enabling technology for development of hot carrier based plasmonic devices.

Journal ArticleDOI
TL;DR: L lamellar stacked MXene membranes with aligned and regular subnanometer channels are designed, taking advantage of the abundant surface-terminating groups on the MXene nanosheets, which exhibit excellent gas separation performance with H2 permeability >2200 Barrer and H2/CO2 selectivity >160, superior to the state-of-the-art membranes.
Abstract: Molecular sieving membranes with sufficient and uniform nanochannels that break the permeability-selectivity trade-off are desirable for energy-efficient gas separation, and the arising two-dimensional (2D) materials provide new routes for membrane development. However, for 2D lamellar membranes, disordered interlayer nanochannels for mass transport are usually formed between randomly stacked neighboring nanosheets, which is obstructive for highly efficient separation. Therefore, manufacturing lamellar membranes with highly ordered nanochannel structures for fast and precise molecular sieving is still challenging. Here, we report on lamellar stacked MXene membranes with aligned and regular subnanometer channels, taking advantage of the abundant surface-terminating groups on the MXene nanosheets, which exhibit excellent gas separation performance with H2 permeability >2200 Barrer and H2/CO2 selectivity >160, superior to the state-of-the-art membranes. The results of molecular dynamics simulations quantitatively support the experiments, confirming the subnanometer interlayer spacing between the neighboring MXene nanosheets as molecular sieving channels for gas separation. Two-dimensional materials show great potential for membrane technologies, but their disordered channels hinder their molecular sieving performance. Here, Wang, Gogotsi and colleagues design a MXene membrane with ordered nanochannels that exhibits an excellent H2/CO2 gas separation performance.

Journal ArticleDOI
TL;DR: Solution-processable halide perovskites have high luminous efficiency and excellent chemical tunability, making them ideal candidates for light-emitting diodes, and Yang et al. achieve high external quantum efficiency of 14% in the devices by fine-tuning the phase and passivating the surface defects.
Abstract: Perovskite light-emitting diodes (LEDs) are attracting great attention due to their efficient and narrow emission. Quasi-two-dimensional perovskites with Ruddlesden–Popper-type layered structures can enlarge exciton binding energy and confine charge carriers and are considered good candidate materials for efficient LEDs. However, these materials usually contain a mixture of phases and the phase impurity could cause low emission efficiency. In addition, converting three-dimensional into quasi-two-dimensional perovskite introduces more defects on the surface or at the grain boundaries due to the reduction of crystal sizes. Both factors limit the emission efficiency of LEDs. Here, firstly, through composition and phase engineering, optimal quasi-two-dimensional perovskites are selected. Secondly, surface passivation is carried out by coating organic small molecule trioctylphosphine oxide on the perovskite thin film surface. Accordingly, green LEDs based on quasi-two-dimensional perovskite reach a current efficiency of 62.4 cd A−1 and external quantum efficiency of 14.36%.

Journal ArticleDOI
TL;DR: The results reveal a mechanism by which plants determine the composition of rhizosphere microbiota, plant performance and plant-herbivore interactions of the next generation by modifying root-associated microbiota.
Abstract: By changing soil properties, plants can modify their growth environment. Although the soil microbiota is known to play a key role in the resulting plant-soil feedbacks, the proximal mechanisms underlying this phenomenon remain unknown. We found that benzoxazinoids, a class of defensive secondary metabolites that are released by roots of cereals such as wheat and maize, alter root-associated fungal and bacterial communities, decrease plant growth, increase jasmonate signaling and plant defenses, and suppress herbivore performance in the next plant generation. Complementation experiments demonstrate that the benzoxazinoid breakdown product 6-methoxy-benzoxazolin-2-one (MBOA), which accumulates in the soil during the conditioning phase, is both sufficient and necessary to trigger the observed phenotypic changes. Sterilization, fungal and bacterial profiling and complementation experiments reveal that MBOA acts indirectly by altering root-associated microbiota. Our results reveal a mechanism by which plants determine the composition of rhizosphere microbiota, plant performance and plant-herbivore interactions of the next generation.

Journal ArticleDOI
TL;DR: A review of recent advances in developing highly doped UCNPs is surveyed, the strategies that bypass the concentration quenching effect are highlighted, and new optical properties as well as emerging applications enabled by these nanoparticles are discussed.
Abstract: Lanthanide-doped upconversion nanoparticles (UCNPs) are capable of converting near-infra-red excitation into visible and ultraviolet emission. Their unique optical properties have advanced a broad range of applications, such as fluorescent microscopy, deep-tissue bioimaging, nanomedicine, optogenetics, security labelling and volumetric display. However, the constraint of concentration quenching on upconversion luminescence has hampered the nanoscience community to develop bright UCNPs with a large number of dopants. This review surveys recent advances in developing highly doped UCNPs, highlights the strategies that bypass the concentration quenching effect, and discusses new optical properties as well as emerging applications enabled by these nanoparticles.

Journal ArticleDOI
TL;DR: A strategy for fabrication of ACs comprising only isolated nickel/iron atoms anchored on graphdiyne is reported, which shows high hydrogen evolution electrocatalysis activities and motivates the authors to develop a general approach in the field of single-atom transition-metal catalysis.
Abstract: Electrocatalysis by atomic catalysts is a major focus of chemical and energy conversion effort. Although transition-metal-based bulk electrocatalysts for electrochemical application on energy conversion processes have been reported frequently, anchoring the stable transition-metal atoms (e.g. nickel and iron) still remains a practical challenge. Here we report a strategy for fabrication of ACs comprising only isolated nickel/iron atoms anchored on graphdiyne. Our findings identify the very narrow size distributions of both nickel (1.23 A) and iron (1.02 A), typical sizes of single-atom nickel and iron. The precision of this method motivates us to develop a general approach in the field of single-atom transition-metal catalysis. Such atomic catalysts have high catalytic activity and stability for hydrogen evolution reactions.

Journal ArticleDOI
TL;DR: The authors report on the development of injectable, biocompatible carbon nanotube reinforced quaternized chitosan cryogels with shape memory, conductivity and antibacterial properties for hemostatic control for lethal noncompressible hemorrhage hemostasis and wound healing.
Abstract: Developing injectable antibacterial and conductive shape memory hemostatic with high blood absorption and fast recovery for irregularly shaped and noncompressible hemorrhage remains a challenge. Here we report injectable antibacterial conductive cryogels based on carbon nanotube (CNT) and glycidyl methacrylate functionalized quaternized chitosan for lethal noncompressible hemorrhage hemostasis and wound healing. These cryogels present robust mechanical strength, rapid blood-triggered shape recovery and absorption speed, and high blood uptake capacity. Moreover, cryogels show better blood-clotting ability, higher blood cell and platelet adhesion and activation than gelatin sponge and gauze. Cryogel with 4 mg/mL CNT (QCSG/CNT4) shows better hemostatic capability than gauze and gelatin hemostatic sponge in mouse-liver injury model and mouse-tail amputation model, and better wound healing performance than Tegaderm™ film. Importantly, QCSG/CNT4 presents excellent hemostatic performance in rabbit liver defect lethal noncompressible hemorrhage model and even better hemostatic ability than Combat Gauze in standardized circular liver bleeding model.

Journal ArticleDOI
TL;DR: A mathematical expression is derived to compute PrediXcan results using summary data, and the effects of gene expression variation on human phenotypes in 44 GTEx tissues and >100 phenotypes are investigated.
Abstract: Scalable, integrative methods to understand mechanisms that link genetic variants with phenotypes are needed. Here we derive a mathematical expression to compute PrediXcan (a gene mapping approach) results using summary data (S-PrediXcan) and show its accuracy and general robustness to misspecified reference sets. We apply this framework to 44 GTEx tissues and 100+ phenotypes from GWAS and meta-analysis studies, creating a growing public catalog of associations that seeks to capture the effects of gene expression variation on human phenotypes. Replication in an independent cohort is shown. Most of the associations are tissue specific, suggesting context specificity of the trait etiology. Colocalized significant associations in unexpected tissues underscore the need for an agnostic scanning of multiple contexts to improve our ability to detect causal regulatory mechanisms. Monogenic disease genes are enriched among significant associations for related traits, suggesting that smaller alterations of these genes may cause a spectrum of milder phenotypes.