A Core/Shell Bi2S3/BiVO4 Nanoarchitecture for Efficient Photoelectrochemical Water Oxidation.

The construction of nanostructured heterostructure is a potent strategy for achieving high-performance photoelectrochemical (PEC) water splitting. Among these, constructing BiVO4-based heterostructure stands out as a promising method for optimizing light-harvesting efficiency and reducing severe charge recombination. Herein, we present a novel approach to fabricate a type II heterostructure of core/shell Bi2S3/BiVO4 using electrolytic deposition and successive ionic layer adsorption and reaction (SILAR) methods. We identify the type II heterostructure and the difference in fermi energy using UV-Vis spectroscopy, X-ray photoelectron spectroscopy, and PEC measurements. This redistribution of charges due to the fermi energy difference induces an interfacial built-in electric field from BiVO4 to Bi2S3, reinforcing the photogenerated hole transfer kinetics from BiVO4 to Bi2S3. The Bi2S3/BiVO4 heterostructure exhibits a superior photocurrent (6.0 mA cm-2), enhanced charge separation efficiency (85 %), and higher open-circuit photovoltage (350 mV). Additionally, the heterostructure displays a prolonged average lifetime of charge (1.63 ns), verifying this heterojunction could boost interfacial carriers' migration via an additional nonradiative quenching pathway. Furthermore, the lower photoluminescence (PL) intensity demonstrates the interfacial built-in electric field is beneficial for boosting charge migration.

Tuning Surface Electronics State of P-Doped In2.77S4/In(OH)3 toward Efficient Photoelectrochemical Water Oxidation.

Indium sulfide with a two-dimensional layered structure offers a platform for catalyzing water oxidation by a photoelectrochemical process. However, the limited hole holders hinder the weak intrinsic catalytic activity. Here, the nonmetallic phosphorus atom is coordinated to In2.77S4/In(OH)3 through a bridge-bonded sulfur atom. By substituting the S position by the P dopant, the work function (surface potential) is regulated from 445 to 210 mV, and the lower surface potential is shown to be beneficial for holding the photogenerated holes. In2.77S4/In(OH)3/P introduces a built-in electric field under the difference of Fermi energy, and the direction is from the bulk to the surface. This band structure results in upward band bending at the interface of In2.77S4/In(OH)3 and P-doped sites, which is identified by density functional theory calculations (∼0.8 eV work function difference). In2.77S4/In(OH)3/P stands out with the highest oxidation efficiency (ηoxi = 70%) and charge separation efficiency (ηsep = 69%). Importantly, it delivers a remarkable water oxidation photocurrent density of 2.51 mA cm-2 under one sun of illumination.

EndoQuad: a comprehensive genome-wide experimentally validated endogenous G-quadruplex database.

G-quadruplexes (G4s) are non-canonical four-stranded structures and are emerging as novel genetic regulatory elements. However, a comprehensive genomic annotation of endogenous G4s (eG4s) and systematic characterization of their regulatory network are still lacking, posing major challenges for eG4 research. Here, we present EndoQuad (https://EndoQuad.chenzxlab.cn/) to address these pressing issues by integrating high-throughput experimental data. First, based on high-quality genome-wide eG4s mapping datasets (human: 1181; mouse: 24; chicken: 2) generated by G4 ChIP-seq/CUT&Tag, we generate a reference set of genome-wide eG4s. Our multi-omics analyses show that most eG4s are identified in one or a few cell types. The eG4s with higher occurrences across samples are more structurally stable, evolutionarily conserved, enriched in promoter regions, mark highly expressed genes and associate with complex regulatory programs, demonstrating higher confidence level for further experiments. Finally, we integrate millions of functional genomic variants and prioritize eG4s with regulatory functions in disease and cancer contexts. These efforts have culminated in the comprehensive and interactive database of experimentally validated DNA eG4s. As such, EndoQuad enables users to easily access, download and repurpose these data for their own research. EndoQuad will become a one-stop resource for eG4 research and lay the foundation for future functional studies.

Regulation of the surface activity of carbon anodes for rationalization of potassium storage.

The gradient temperature was manipulated to construct hollow irregular carbon spheres with regulated intrinsic defects and surface area targeting favorable potassium storage. An enlarged surface area, increased intrinsic defects, and superior conductivity induced more surface-active interfaces. These actions facilitated a high reversible capacity as well as excellent cycling stability.

Evolution and function of developmentally dynamic pseudogenes in mammals.

BACKGROUND: Pseudogenes are excellent markers for genome evolution, which are emerging as crucial regulators of development and disease, especially cancer. However, systematic functional characterization and evolution of pseudogenes remain largely unexplored. RESULTS: To systematically characterize pseudogenes, we date the origin of human and mouse pseudogenes across vertebrates and observe a burst of pseudogene gain in these two lineages. Based on a hybrid sequencing dataset combining full-length PacBio sequencing, sample-matched Illumina sequencing, and public time-course transcriptome data, we observe that abundant mammalian pseudogenes could be transcribed, which contribute to the establishment of organ identity. Our analyses reveal that developmentally dynamic pseudogenes are evolutionarily conserved and show an increasing weight during development. Besides, they are involved in complex transcriptional and post-transcriptional modulation, exhibiting the signatures of functional enrichment. Coding potential evaluation suggests that 19% of human pseudogenes could be translated, thus serving as a new way for protein innovation. Moreover, pseudogenes carry disease-associated SNPs and conduce to cancer transcriptome perturbation. CONCLUSIONS: Our discovery reveals an unexpectedly high abundance of mammalian pseudogenes that can be transcribed and translated, and these pseudogenes represent a novel regulatory layer. Our study also prioritizes developmentally dynamic pseudogenes with signatures of functional enrichment and provides a hybrid sequencing dataset for further unraveling their biological mechanisms in organ development and carcinogenesis in the future.

Fe-Co controlled super-hygroscopic hydrogels toward efficient atmospheric water harvesting.

Extracting atmospheric moisture for freshwater production is an appealing way to mitigate the global water crisis. However, the low moisture sorption capacity and high desorption temperature are the major bottlenecks for efficient atmospheric water harvesting. Herein, we develop a transition metal super-hygroscopic hydrogel by an economical strategy, which is constructed through a facile coordination between metal salts and ethanolamine. When the empty electron orbital of the metal ion is coordinated with the lone electron pair of nitrogen or oxygen atom, the water active sorption site is formed. A single water layer is bonded on the sites by a coordination effect, followed by physical interaction with water to form multi-layer structures. The Fe and Co ions in the hydrogel function as dual sorption sites to capture moisture, which can harvest additional water by the synergistic effect of bimetals. As a result, the bimetal hydrogel contributes to a high water uptake of 5.22 g g-1 at 95% RH, triggering the desorption process by one solar intensity due to its low desorption temperature (≤50 °C).

Dynamic Spatial-temporal Expression Ratio of X Chromosome to Autosomes but Stable Dosage Compensation in Mammals.

In the evolutionary model of dosage compensation, per-allele expression level of the X chromosome has been proposed to have twofold up-regulation to compensate its dose reduction in males (XY) compared to females (XX). However, the expression regulation of X-linked genes is still controversial, and comprehensive evaluations are still lacking. By integrating multi-omics datasets in mammals, we investigated the expression ratios including X to autosomes (X:AA ratio) and X to orthologs (X:XX ratio) at the transcriptome, translatome, and proteome levels. We revealed a dynamic spatial-temporal X:AA ratio during development in humans and mice. Meanwhile, by tracing the evolution of orthologous gene expression in chickens, platypuses, and opossums, we found a stable expression ratio of X-linked genes in humans to their autosomal orthologs in other species (X:XX ≈ 1) across tissues and developmental stages, demonstrating stable dosage compensation in mammals. We also found that different epigenetic regulations contributed to the high tissue specificity and stage specificity of X-linked gene expression, thus affecting X:AA ratios. It could be concluded that the dynamics of X:AA ratios were attributed to the different gene contents and expression preferences of the X chromosome, rather than the stable dosage compensation.

Novel High-Performance and Low-Cost Electrochromic Prussian White Film.

Prussian white (PW), due to its low cost, easy synthesis, open structure, and fast ion extraction/interaction, is introduced to the electrochromic field. The PW films were successfully grown on indium tin oxide (ITO) glass by a facial hydrothermal method. Impressively, the PW film exhibits excellent electrochemical cycling stability without obvious decay over 10 000 cycles and a high coloration efficiency of 149.3 cm2 C-1. The film also provides the large optical transmittance contrast (over 70%) in a wide wavelength range of 650-800 nm. Furthermore, the PW film shows the rapid coloration and bleaching response. These results suggest that PW is a promising practical candidate of high-performance electrochromic material.

GenOrigin: A comprehensive protein-coding gene origination database on the evolutionary timescale of life.

The origination of new genes contributes to the biological diversity of life. New genes may quickly build their network, exert important functions, and generate novel phenotypes. Dating gene age and inferring the origination mechanisms of new genes, like primate-specific genes, is the basis for the functional study of the genes. However, no comprehensive resource of gene age estimates across species is available. Here, we systematically date the age of 9,102,113 protein-coding genes from 565 species in the Ensembl and Ensembl Genomes databases, including 82 bacteria, 57 protists, 134 fungi, 58 plants, 56 metazoa, and 178 vertebrates, using a protein-family-based pipeline with Wagner parsimony algorithm. We also collect gene age estimate data from other studies and uniformly distribute the gene age estimates to time ranges in a million years for comparison across studies. All the data are cataloged into GenOrigin (http://genorigin.chenzxlab.cn/), a user-friendly new database of gene age estimates, where users can browse gene age estimates by species, age, and gene ontology. In GenOrigin, the information such as gene age estimates, annotation, gene ontology, ortholog, and paralog, as well as detailed gene presence/absence views for gene age inference based on the species tree with evolutionary timescale, is provided to researchers for exploring gene functions.

Construction of direct Z-scheme photocatalyst by the interfacial interaction of WO3 and SiC to enhance the redox activity of electrons and holes.

The direct Z-scheme heterojunction structure benefits separation and migration of photoinduced carriers while maintaining original redox ability of each component. Nowadays, most Z-scheme structures are fabricated by g-C3N4 with other narrow band photocatalysts due to its low conduction band (CB). In this paper, SiC, another kind of photoelectric semiconductor with low CB, was employed to prepare direct Z-scheme photocatalyst with 2D WO3 by simple water oxidation precipitation method. The component and interface band structure of Z-scheme heterojunction WO3/SiC (WS) were verified by XPS, KPFM, Mott-Schottky method. The photodegradation efficiency and rate constant values of WS-1 for degrading RhB enhanced 2.5 and 5.3 times respectively compared with pristine WO3. Radical capture experiments and ESR tests affirmed that WS-1 photocatalyst produced •OH and •O2－active species, which further confirmed the photogenerated carriers were transmitted through the Z-scheme mode in principle. Band structure investigation showed that the direct Z-scheme structure assembled by WO3 with high valence band (VB) and SiC with low CB could maintain the high photocatalytic activity of active species. Therefore, this study offers a feasible method for construction of a novel and efficient direct Z-scheme photocatalyst.

Hierarchical Copper Sulfide Porous Nanocages for Rechargeable Multivalent-Ion Batteries.

Copper sulfide (CuS) has been identified as a promising positive electrode material for some multivalent-ion batteries (such as the magnesium-ion battery) because of its high theoretical capacity, environmental friendliness, and wide availability. However, the clumsy multivalent-ion with high polarity inclines toward sluggish ion insertion/de-insertion, leading to inadequate electrochemical performance. In this work, the hierarchical CuS porous nanocages are successfully fabricated via a facile one-step room-temperature liquid-phase process and evaluated as positive electrode materials for rechargeable magnesium batteries. Owing to the structural advantages, a high reversible magnesium storage capacity of 228 mA h g-1 is attained, which is superior to the previously reported results under similar conditions. Besides, the application of CuS as positive electrode materials for calcium-ion, zinc-ion, iron-ion, and aluminum-ion batteries is investigated. The hierarchical CuS porous nanocages display promising electrochemical performance in those multivalent-ion battery systems. Our work proves the superiority of the nanostructure design in improving the electrochemical performance of positive electrode materials for multivalent-ion batteries.

Solvent Engineering of a Dopant-Free Spiro-OMeTAD Hole-Transport Layer for Centimeter-Scale Perovskite Solar Cells with High Efficiency and Thermal Stability.

High efficiency and environmental stability are mandatory performance requirements for commercialization of perovskite solar cells (PSCs). Herein, efficient centimeter-scale PSCs with improved stability were achieved by incorporating an additive-free 2,2',7,7'-tetrakis[N,N-di(p-methoxyphenyl)amino]-9,9'-spirobifluorene (spiro-OMeTAD) hole-transporting material (HTM) through simply substituting the usual chlorobenzene solvent with pentachloroethane (PC). A stabilized power conversion efficiency (PCE) of 16.1% under simulated AM 1.5G 1 sun illumination with an aperture of 1.00 cm2 was achieved for PSCs using an additive-free spiro-OMeTAD layer cast from PC. X-ray analysis suggested that chlorine radicals from PC transfer partially to spiro-OMeTAD and are retained in the HTM layer, resulting in conductivity improvement. Moreover, unencapsulated PSCs with a centimeter-scale active area cast from PC retained >70% of their initial PCE after ageing at 80 °C for 500 h, in contrast with less than 20% retention for control devices. Morphological and X-ray analyses of the aged cells revealed that the perovskite and HTM layers remain almost unchanged in the cells with a spiro-OMeTAD layer cast from PC whereas serious degradation occurred in the control cells. This study not only reveals the decomposition mechanism of PSCs in the presence of HTM additives but also opens up a broad range of organic semiconductors for radical doping.

Modulated transition metal-oxygen covalency in the octahedral sites of CoFe layered double hydroxides with vanadium doping leading to highly efficient electrocatalysts.

The development of efficient and stable non-noble-metal electrocatalytic materials for the oxygen evolution reaction (OER) is a huge and important challenge at present. Herein, we report the prominent enhancement of OER activity via doping vanadium into CoFe-based layered double hydroxide (LDH) electrocatalysts. Electrochemical characterization shows that the Co2Fe0.5V0.5 LDH grown on carbon papers (CPs) has an enormous electrochemical surface area (ECSA) and exhibits the smallest overpotential of 242 mV at 10 mA cm-2, which only requires a small Tafel slope of 41.4 mV dec-1 in 1 M KOH solution. The X-ray photoelectron spectroscopy (XPS) peak position of Co, Fe and O moves slightly to higher binding energy, elucidating the improved covalency of the metal-oxygen bond after V doping. DFT+U simulation indicates that the outstanding electrocatalytic activity of Co2Fe0.5V0.5 could be ascribed to the increased metal-oxygen covalency in LDH after V element doping, and facilitates the charge-transfer from oxygen to the metal. This finely tuned strategy by V doping into the CoFe-based LDH matrix can adjust the covalency of metal-oxygen bridges and enhance its electrocatalytic activity for the OER. In this work, we also present a general method to study various highly efficient metal hydroxide catalysts for the OER.

High Energy Capacitors Based on All Metal-Organic Frameworks Derivatives and Solar-Charging Station Application.

High energy and efficient solar charging stations using electrochemical capacitors (ECs) are a promising portable power source for the future. In this work, two kinds of metal-organic framework (MOF) derivatives, NiO/Co3 O4 microcubes and Fe2 O3 microleaves, are prepared via thermal treatment and assembled into electrochemical capacitors, which deliver a relatively high specific energy density of 46 Wh kg-1 at 690 W kg-1 . In addition, a solar-charging power system consisting of the electrochemical capacitors and monocrystalline silicon plates is fabricated and a motor fan or 25 LEDs for 5 and 30 min, respectively, is powered. This work not only adds two novel materials to the growing categories of MOF-derived advanced materials, but also successfully achieves an efficient solar-ECs system for the first time based on all MOF derivatives, which has a certain reference for developing efficient solar-charge systems.

In-Fiber Mach-Zehnder Interferometer Based on Three-Core Fiber for Measurement of Directional Bending.

A highly sensitive directional bending sensor based on a three-core fiber (TCF) Mach-Zehnder interferometer (MZI) is presented in this study. This MZI-based bending sensor was fabricated by fusion-splicing a section of TCF between two single-mode fibers (SMF) with core-offset. Due to the location of the core in the TCF, a bend applied to the TCF-based MZI led to an elongation or shortening of the core, which makes the sensor suitable for directional bending measurement. To analyze the bending characteristics, two types of TCF-based sensors, with the fusion-spliced core located at different positions between the SMFs, were investigated. A swept source was employed in the measurement technique. The experimental results showed that, for the two types of sensors in this setup, the bending sensitivities of the two sensors were 15.36 nm/m-1 and 3.11 nm/m-1 at the bending direction of 0°, and -20.48 nm/m-1 and -5.29 nm/m-1 at the bending direction of 180°. The temperature sensitivities of the two sensors were 0.043 nm/°C and 0.041 nm/°C, respectively. The proposed sensors are compact, versatile, inexpensive to fabricate, and are expected to have potential applications in biomedical sensing.

Spacer layer design for efficient fully printable mesoscopic perovskite solar cells.

The spacer layer is a key component of fully printable mesoscopic perovskite solar cells, but its precise characteristics are far from being understood in relation to the device design. In the present work, we perform a detailed systematic study on the effects of spacer parameters, such as size of building blocks, layer thickness, etc., on properties of the perovskite filler, insulating ability and performance of fully printable mesoscopic perovskite solar cells by combining the techniques of time-resolved photoluminescence, high-resolution TEM, insulating resistance measurements, impedance spectroscopy and J-V characteristics. Drawing on the deep understanding from these studies, we formulate key principles, which are anticipated to guide the design of the advanced spacer layer for fully printable mesoscopic perovskite solar cells.

Boron-Doped Graphite for High Work Function Carbon Electrode in Printable Hole-Conductor-Free Mesoscopic Perovskite Solar Cells.

Work function of carbon electrodes is critical in obtaining high open-circuit voltage as well as high device performance for carbon-based perovskite solar cells. Herein, we propose a novel strategy to upshift work function of carbon electrode by incorporating boron atom into graphite lattice and employ it in printable hole-conductor-free mesoscopic perovskite solar cells. The high-work-function boron-doped carbon electrode facilitates hole extraction from perovskite as verified by photoluminescence. Meanwhile, the carbon electrode is endowed with an improved conductivity because of a higher graphitization carbon of boron-doped graphite. These advantages of the boron-doped carbon electrode result in a low charge transfer resistance at carbon/perovskite interface and an extended carrier recombination lifetime. Together with the merit of both high work function and conductivity, the power conversion efficiency of hole-conductor-free mesoscopic perovskite solar cells is increased from 12.4% for the pristine graphite electrode-based cells to 13.6% for the boron-doped graphite electrode-based cells with an enhanced open-circuit voltage and fill factor.

Efficient Compact-Layer-Free, Hole-Conductor-Free, Fully Printable Mesoscopic Perovskite Solar Cell.

A compact-layer-free, hole-conductor-free, fully printable mesoscopic perovskite solar cell presents a power conversion efficiency of over 13%, which is comparable to that of the device with a TiO2 compact layer. The different wettability of the perovskite precursor solution on the surface of FTO and TiO2 possesses a significant effect on realizing efficient mesoscopic perovskite solar cell. This result shows a promising future in printable solar cells by further simplifying the fabrication process and lowering the preparation costs.

Hydrothermal core-shell carbon nanoparticle films: thinning the shell leads to dramatic pH response.

Carbon nanoparticles with phenylsulfonate negative surface functionality (Emperor 2000, Cabot Corp.) are coated with positive chitosan followed by hydrothermal carbonization to give highly pH-responsive core-shell nanocarbon composite materials. With optimised core-shell ratio (resulting in an average shell thickness of ca. 4 nm, estimated from SANS data) modified electrodes exhibit highly pH-sensitive resistance, capacitance, and Faradaic electron transfer responses (solution based, covalently bound, or hydrothermally embedded). A shell "double layer exclusion" mechanism is discussed to explain the observed pH switching effects. Based on this mechanism, a broader range of future applications of responsive core-shell nanoparticles are envisaged.