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Various in situ/operando characterization techniques provide a comprehensive understanding of LLZO-based solid-state lithium batteries.

Metal halide perovskites possess intriguing optoelectronic properties, however, the lack of precise control of on-chip fabrication of the large-scale perovskite single crystal arrays restricts its application in integrated devices. Here, we report a space confinement and antisolvent-assisted crystallization method for the homogeneous perovskite single crystal arrays spanning 100 square centimeter areas. This method enables precise control over the crystal arrays, including different array shapes and resolutions with less than 10%-pixel position variation, tunable pixel dimensions from 2 µm to 8 µm as well as the in-plane rotation of each pixel. The crystal pixel could serve as a high-quality whispering gallery mode microcavity with a quality factor of 2915 and a threshold of 4.14 µJ/cm2. Through directly on-chip fabrication on the patterned electrodes, a vertical structured photodetector array is demonstrated with stable photoswitching behavior and the capability to image the input patterns, indicating the potential application in the integrated systems of this method.

Atomic understanding of a chemical reaction can realize the programmable design and synthesis of desired products with specific compositions and structures. Through directly monitoring the phase transition and tracking the dynamic evolution of atoms in a chemical reaction, in situ transmission electron microscopy (TEM) techniques offer the feasibility of revealing the reaction kinetics at the atomic level. Nevertheless, such investigation is quite challenging, especially for reactions involving multi-phase and complex interfaces, such as the widely adopted carbothermal reduction (CTR) reactions. Herein, in-situ TEM is applied to monitor the CTR of Co

Room-temperature sodium-sulfur (RT-Na/S) batteries possess high potential for grid-scale stationary energy storage due to their low cost and high energy density. However, the issues arising from the low S mass loading and poor cycling stability caused by the shuttle effect of polysulfides seriously limit their operating capacity and cycling capability. Herein, sulfur-doped graphene frameworks supporting atomically dispersed 2H-MoS

Heavy Fermion (HF) states emerge in correlated quantum materials due to the intriguing interplay between localized magnetic moments and itinerant electrons but rarely appear in 3d-electron systems due to high itinerancy of d-electrons. Here, an anomalous enhancement of Kondo screening is observed at the Kondo hole of local Fe vacancies in Fe3GeTe2 which is a recently discovered 3d-HF system featuring Kondo lattice and two-dimensional itinerant ferromagnetism. An itinerant Kondo-Ising model is established to reproduce the experimental results and provides insight into the competition between Ising ferromagnetism and Kondo screening. Our work explains the microscopic origin of the d-electron HF states in Fe3GeTe2 and inspires future studies of the enriched quantum many-body effects with Kondo holes.

Compared with traditional solder joint bonding, an anisotropic conductive adhesive (ACA) provides an efficient and simple method for the interconnection of small-scale electronics. The wider applic...

Liquid phase transmission electron microscopy (TEM) provides a useful means to study a wide range of dynamics in solution with near-atomic spatial resolution and sub-microsecond temporal resolution. However, it is still a challenge to control the chemical environment (such as the flow of liquid, flow rate, and the liquid composition) in a liquid cell, and evaluate its effect on the various dynamic phenomena. In this work, we have systematically demonstrated the flow performance of an in situ liquid TEM system, which is based on ‘on-chip flow’ driven by external pressure pumps. We studied the effects of different chemical environments in the liquid cell as well as the electrochemical potential on the deposition and dissolution behavior of Cu crystals. The results show that uniform Cu deposition can be obtained at a higher liquid flow rate (1.38 μl min−1), while at a lower liquid flow rate (0.1 μl min−1), the growth of Cu dendrites was observed. Dendrite formation could be further promoted by in situ addition of foreign ions, such as phosphates. The generality of this technique was confirmed by studying Zn electrodeposition. Our direct observations not only provide new insights into understanding the nucleation and growth but also give guidelines for the design and synthesis of desired nanostructures for specific applications. Finally, the capability of controlling the chemical environment adds another dimension to the existing liquid phase TEM technique, extending the possibilities to study a wide range of dynamic phenomena in liquid media.

The physical and chemical properties of transition metal dichalcogenides can be effectively tuned by doping or alloying, which is essential for their practical applications. However, the microstructure evolutions and their effects on the physical properties induced by alloying from hetero-atoms with different outermost electronic structures are still unclear. Here, we synthesized Nb-substituted WS2 with various Nb concentrations showing unusual changes of optical behaviors and continuous electrical polarity reversal. The fully softened Raman mode, rapidly quenched photoluminescence, and severe electron scattering can be attributed to the combined effects of charge doping and lattice strain caused by atomic Nb doping. Three types of substitution modes of Nb atoms in the WS2 lattice were observed directly from atomic-resolution scanning transmission electron microscopy. Density functional theory calculations further confirm the role of lattice strain in the evolutions of optical and electrical characteristics. With increasing Nb concentration, n-type, ambipolar, and p-type field-effect transistors can be achieved, indicating the capacity of this doping method to engineer the properties of two-dimensional materials for future electronic applications.

Pseudocapacitive energy storage via Li+ storage at the surface/interface of the electrode is promising for achieving both high energy density and high power density in lithium-ion batteries (LIBs). Thus, we created holey graphene (HG) via an etching method, and then in situ grew atomically thin mesoporous NiCo2O4 nanosheets on the HG surface, resulting in a NiCo2O4–HG heterostructure. Since both NiCo2O4 and HG possess atomic thickness and porous structures, the as-prepared nanocomposite enables efficient electrolyte diffusion and mass transfer, providing abundant accessible surface atoms for enhanced redox pseudocapacitance. Moreover, the strong coupling effect between NiCo2O4 and graphene produces an ultra-large interfacial area and enhanced electrical conductivity, and subsequently promotes the intercalation pseudocapacitance. Consequently, the NiCo2O4@HG exhibits a high specific capacity of 1103.4 mA h g−1 at 0.2C, ∼88.9% contribution from pseudocapacitance at 1 mV s−1, excellent rate capability, and ultra-long life up to 450 cycles with 931.2 mA h g−1 retention, significantly outperforming previously reported electrodes. This work suggests that the maximum exposure and utilization of the surface/interfacial active sites is vital for the construction of high-performance pseudocapacitive energy storage devices.

Metal chalcogenides are important members of the two-dimensional (2D) materials family and have been extensively investigated for high-performance electronic device applications. However, when they are produced on a large-scale, their carrier mobilities are strongly influenced by the surface conditions. Here, we print indium sulphide (In2S3) with the thickness down to the single unit cell limit on wafer-scale out of metallic indium liquid, in which structural indium vacancies are formed in an orderly fashion. First principles investigations reveal that the unique ordered-vacancy structure results in a highly dispersive conduction band with low effective electron mass, forming multiple band-like electronic transport channels sandwiched within the crystal structure which are less influenced by the surface conditions. Back-gated field effect transistors are fabricated, and the measured mobility is up to 58 cm2 V-1 s-1 with a high degree of reproducibility, which is amongst one of the highest reported for wafer-scale-grown ultra-thin metal chalcogenides. This establishes ordered-vacancy-enabled semiconductors in the 2D geometry as suitable alternatives for new generation high-performance electronic devices.

SUMMARYCohesin folds chromosomes via DNA loop extrusion. Cohesin-mediated chromosome loops regulate transcription by shaping long-range enhancer-promoter interactions, among other mechanisms. Mutations of cohesin subunits and regulators cause human developmental diseases termed cohesinopathy. Vertebrate cohesin consists of SMC1, SMC3, RAD21, and either STAG1 or STAG2. To probe the physiological functions of cohesin, we created conditional knockout (cKO) mice with Stag2 deleted in the nervous system. Stag2 cKO mice exhibit growth retardation, neurological defects, and premature death, in part due to insufficient myelination of nerve fibers. Stag2 cKO oligodendrocytes exhibit delayed maturation and downregulation of myelination-related genes. Stag2 loss reduces promoter-anchored loops at downregulated genes in oligodendrocytes. Thus, STAG2-cohesin generates promoter-anchored loops at myelination-promoting genes to facilitate their transcription. Our study implicates defective myelination as a contributing factor to cohesinopathy and establishes oligodendrocytes as a relevant cell type to explore the mechanisms by which cohesin regulates transcription.

SUMMARYAneuploidy, defective differentiation, and inactivation of the tumor suppressor TP53 all occur frequently during tumorigenesis. Here, we probe the potential links among these cancer traits by inactivating TP53 in human embryonic stem cells (hESCs). TP53−/− hESCs exhibit increased proliferation rates, mitotic errors, and low-grade structural aneuploidy; produce poorly differentiated immature teratomas in mice; and fail to differentiate into neural progenitor cells (NPC) in vitro. Genome-wide CRISPR screen reveals requirements of ciliogenesis and sonic hedgehog (Shh) pathways for hESC differentiation into NPCs. TP53 deletion causes abnormal ciliogenesis in neural rosettes. In addition to restraining cell proliferation through CDKN1A, TP53 activates the transcription of BBS9, which encodes a ciliogenesis regulator required for proper Shh signaling and NPC formation. This developmentally regulated transcriptional program of TP53 promotes ciliogenesis, restrains Shh signaling, and commits hESCs to neural lineages.

Heavy Fermion (HF) states emerge in correlated quantum materials due to the intriguing interplay between localized magnetic moments and itinerant electrons but rarely appear in 3d-electron systems due to high itinerancy of d-electrons. Here, an anomalous enhancement of Kondo screening is observed at the Kondo hole of local Fe vacancies in Fe

Transition metal dissolution in cathode active material for Li-based batteries is a critical aspect that limits the cycle life of these devices. Although several approaches have been proposed to tackle this issue, this detrimental process is not yet overcome. Here, benefitting from the knowledge developed in the semiconductor research field, we apply an epitaxial method to construct an atomic wetting layer of LaTMO

Aneuploidy, defective differentiation, and inactivation of the tumor suppressor TP53 all occur frequently during tumorigenesis. Here, we probe the potential links among these cancer traits by inactivating TP53 in human embryonic stem cells (hESCs). TP53

Efficient photo-electrocatalysts for hydrogen evolution reaction (HER) are synthesized using a facile one-step hydrothermal method. With metal-ion bridges, highly dispersed molybdenum disulfide (MoS2) nanolayers are vertically grown on the reduced graphene oxide (RGO) to form RGO-M-MoS2 photocatalysts for HER, where M = Fe3+, Co2+, Ni2+, Cu2+ and Zn2+. The results show that the cross-bridging ions can modulate the MoS2 growth priority and act as efficient charge transfer channels between RGO and MoS2, and combine the advantages of the high conductivity of graphene with the photo-electrochemical activity of MoS2. The metal-ion bridged MoS2-M-RGO heterostructures demonstrate superior catalytic activity toward hydrogen evolution reaction in acid medium, evidenced by the remarkable higher catalytic current density at low overpotential compared with that of MoS2-RGO without metal-ion bridge. This study provides a novel and facile route for establishing efficient composite photo-electrocatalysts for water splitting to generate hydrogen.

The poor cycling stability resulting from the large volume expansion caused by lithiation is a critical issue for Si-based anodes. Herein, we report for the first time of a new yolk-shell structured high tap density composite made of a carbon-coated rigid SiO2 outer shell to confine multiple Si NPs (yolks) and carbon nanotubes (CNTs) with embedded Fe2 O3 nanoparticles (NPs). The high tap density achieved and superior conductivity can be attributed to the efficiently utilised inner void containing multiple Si yolks, Fe2 O3 NPs, and CNTs Li+ storage materials, and the bridged spaces between the inner Si yolks and outer shell through a conductive CNTs "highway". Half cells can achieve a high area capacity of 3.6 mAh cm-2 and 95 % reversible capacity retention after 450 cycles. The full cell constructed using a Li-rich Li2 V2 O5 cathode can achieve a high reversible capacity of 260 mAh g-1 after 300 cycles.

L11-CoPt(1 1 1) films were successfully fabricated on glass substrates at 300–400 °C, using Pt(1 1 1) underlayer. Magnetocrystalline anisotropy energy shows a maximum of 1.8 × 106 J/m3 at 350 °C. The mechanism of L11-CoPt ordering after introducing Pt underlayer is considered to be strain- or stress-induced ordering. The effect of CoPt layer thickness on phase structure and magnetic properties were investigated to confirm the ordering mechanism. Perpendicular magnetic anisotropy has been obtained in all CoPt films, while the squareness ratio and coercivity decrease with increasing film thickness, indicating decreased ordering due to the relaxation of strain or stress in thick films.

The separation of electron–hole pairs has a significant influence on the photocatalytic process on semiconductors. In this work, BiOCl nanosheets with oxygen vacancies (BiOCl-OVs) have been prepare...

Transition metals with desirable valence states have been proposed as efficient non-noble-metal electrocatalytic systems for selective water splitting. In this work, two-dimensional (2D) nitrogen-doped leaf-like carbon matrix arrays functionalized with multi-valence-state transition metal (cobalt) hybrids were successfully prepared by in situ calcination of the corresponding bimetallic leaf-like zeolitic imidazolate framework (ZIF-L) in an inert atmosphere. The 2D morphology of the matrix along with the particle size and surface valence state of the anchored particles has been successfully controlled via precisely adjusting the Co2+/(Zn2+ + Co2+) ratio in the bimetallic ZIF-L precursor. Electrochemical measurements show that the kinetics of and stability towards the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are highly dependent on the particle size as well as the valence states. It was found that the particles with sizes less than 60 nm exhibit mixed Co0/Co2+ valence states, and therefore demonstrate bi-functional electrocatalytic performance. The theoretical simulations revealed that the bi-functional electrocatalytic activity should be attributed to the synergetic effect of mixed Co0/Co2+ and electronic coupling in the hybrids, which are of benefit to the catalytic kinetics and dynamics. High HER and OER activities of the hybrids have been verified, in which overpotentials of 171 and 280 mV to deliver a current density of 10 mA cm−2 for the HER and OER, respectively, were achieved. The obtained correlation between non-noble-metal-based carbon composites and HER/OER activities may be exploited as a rational guideline in the design and engineering of electrocatalysts.

Developing efficient electrocatalysts for the oxygen evolution reaction (OER) is highly challenging for hydrogen production from water splitting, due to the high energy barrier for OO bond formation and the restriction of the scaling relation between the multiple reaction intermediates. In order to simultaneously address these concerns, an Ir/Ni(OH)

The mixed caesium and formamidinium lead triiodide perovskite system (Cs1−xFAxPbI3) in the form of quantum dots (QDs) offers a pathway towards stable perovskite-based photovoltaics and optoelectronics. However, it remains challenging to synthesize such multinary QDs with desirable properties for high-performance QD solar cells (QDSCs). Here we report an effective oleic acid (OA) ligand-assisted cation-exchange strategy that allows controllable synthesis of Cs1−xFAxPbI3 QDs across the whole composition range (x = 0–1), which is inaccessible in large-grain polycrystalline thin films. In an OA-rich environment, the cross-exchange of cations is facilitated, enabling rapid formation of Cs1−xFAxPbI3 QDs with reduced defect density. The hero Cs0.5FA0.5PbI3 QDSC achieves a certified record power conversion efficiency (PCE) of 16.6% with negligible hysteresis. We further demonstrate that the QD devices exhibit substantially enhanced photostability compared with their thin-film counterparts because of suppressed phase segregation, and they retain 94% of the original PCE under continuous 1-sun illumination for 600 h.

Tailoring catalysts with balanced adsorption capabilities toward multiple reaction intermediates is highly desirable for complex electrocatalytic reactions, but rather challenging. Here, Ni single atom-decorated carbon nanosheets are developed as multifunctional supports for engineering heterostructured electrocatalysts toward hydrogen evolution in alkaline media. The Ni single atoms (Ni–N4) are actively dedicated to cleaving the H–OH bonds as well as facilitating Had spillover to metallic Pt sites. For the case of supported Pt electrocatalysts, a Pt/PtOx configuration is generated at the heterointerface via Pt–O–C (Ni) interfacial bonding, with oxidized Pt species located at the interface and metallic Pt formed in the near-interface area. Further, the oxidized Pt species are also active for boosting the water dissociation step. These findings not only open up a new avenue toward the development of multifunctional catalyst supports but also demonstrate the importance of regulating interface chemistry of heterostructured electrocatalysts at atomic level.

Core-shell and hollow nanostructures have been receiving significant interest due to their potential in wide scientific and technological fields. Given such large scope, however, they still lag far behind in terms of the ambition toward controllably, or even programmatically, synthesizing libraries of core-shell structures on a large scale. Here, a general route for the programmable preparation of complex core-shell nanostructures by using liquid metal (LM) droplets as reformable templates is presented, and the triggering of a localized galvanic replacement reaction in one ultrasonication system is demonstrated. Benefiting from the activity and mobility of the metal components in LM templates, high-level compositional diversity control and quantitative regulation of both the core and the shell layers of the heterogeneous products are achieved, which cannot be realized with a solid-template synthetic route.

Transition metal phosphides are promising alternatives to the precious metal catalysts for various electrocatalysis applications. Controllable and precise surface engineering of electrocatalysts is the key challenge to enhance their performance. Herein, we demonstrate an ion-exchange strategy to produce cobalt phosphide nanowires which have a conductive core and a thickness-controlled surface layer with sulfur dopants, phosphorus vacancies, and amorphous domains. They are applied for hydrogen evolution reaction with high stability, achieving a current density of 100 mA cm-2 at an overpotential of 114 mV. Based on both comprehensive state-of-the-art experimental characterizations and theoretical investigations, the excellent catalytic performance is attributed to increased active sites, facilitated charge transfer and transport, as well as weakened H adsorption and strengthened H2O adsorption due to the synergistic effects of S dopants and P vacancies. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) This research is financially supported by the National Natural Science Foundation of China (21703201), the Natural Science Foundation of Jiangsu Province (Grant No. BK20170486), Six Talent Peaks Project in Jiangsu Province (2019-XCL-101), AME-IRG grant (AMEIRG18-0016) from Agency for Science, Technology and Research (A*STAR) of Singapore and AcRF tier 2 grant (MOE2017-T2-2-005) from Ministry of Education (Singapore).

To address the increasing energy demand, rapid consumption of non-renewable fuels, and serious environmental problems, it is very crucial to develop efficient, economical, and environmental-friendly energy conversion/storage devices. Lithium batteries are one of the most attractive and encouraging candidates. However, up to date, their performance is still far from satisfactory. Hence, researchers have been focusing on developing suitable materials as efficient electrodes, separators, electrolytes, etc., to improve their performance. Among all the diverse materials, organic-inorganic hybrids have attracted much attention because they not only possess characteristics of both the organic and inorganic parts but also own specific properties generated from their synergistic effects. It is feasible to obtain organic-inorganic hybrids with desirable properties through the proper hybridization of suitable organic and inorganic precursors. Herein, we made a brief summary of the categories, synthesis strategies, and application of organic-inorganic hybrids in lithium batteries, with special emphasis on the construction of favored organic-inorganic hybrids and their derivatives as efficient electrodes and separators for lithium batteries. These organic-inorganic hybrids have demonstrated their potential to enhance the performance of lithium batteries and other energy conversion/storage devices to the satisfactory level.

As a rising star in the family of graphene analogues, germanene shows great potential for electronic and optical device applications due to its unique structure and electronic properties. It is revealed that the hydrogen terminated germanene not only maintains a high carrier mobility similar to that of germanene, but also exhibits strong light-matter interaction with a direct band gap, exhibiting great potential for photoelectronics. In this work, few-layer germanane (GeH) nanosheets with controllable thickness are successfully synthesized by a solution-based exfoliation-centrifugation route. Instead of complicated microfabrication techniques, a robust photoelectrochemical (PEC)-type photodetector, which can be extended to flexible device, is developed by simply using the GeH nanosheet film as an active electrode. The device exhibits an outstanding photocurrent density of 2.9 µA cm-2 with zero bias potential, excellent responsivity at around 22 µA W-1 under illumination with intensity ranging from 60 to 140 mW cm-2 , as well as short response time (with rise and decay times, tr = 0.24 s and td = 0.74 s). This efficient strategy for a constructing GeH-based PEC-type photodetector suggests a path to promising high-performance, self-powered, flexible photodetectors, and it also paves the way to a practical application of germanene.

Developing efficient electrocatalysts for the oxygen evolution reaction (OER) is highly challenging for hydrogen production from water splitting, due to the high energy barrier for OO bond formation and the restriction of the scaling relation between the multiple reaction intermediates. In order to simultaneously address these concerns, an Ir/Ni(OH)2 heterostructure with abundant heterointerfaces is deliberately designed as an efficient electrocatalyst system, with Ir nanoparticles (NPs) homogeneously confined on the Ni(OH)2 nanosheets. The strong electronic interaction and chemical bonding across the interface between the Ir and Ni(OH)2 can effectively stabilize the metastable electrophilic Ir(V) species, which is vital to boost the formation of OO bonds. Meanwhile, the adsorption of the multiple intermediates is synergistically optimized at the heterointerface, which breaks the restrictive scaling relation and substantially accelerates the OER kinetics. In addition, the severe agglomeration of Ir species is greatly mitigated by the confinement effect, ensuring the structural integrity of the catalyst and the constant exposure of active sites. Owing to its well-defined multifunctional interfaces, the Ir/Ni(OH)2 heterostructure exhibits exceptional OER activity and durability in alkaline media. The present results highlight the significance of heterostructure interface engineering toward the rational design and development of advanced electrocatalysts for the OER and beyond.

Pd- or Pt-based precious catalysts (PPC) are considered to be the best candidates toward high performance directly ethanol fuel cells (DEFC) applications, owing to their high intrinsic activity for ethanol oxidation reaction (EOR). However, the current major barrier for their commercialization is incompletely oxidized intermediates (IOI, such as CO) that poison the catalysts to affect the durability of the cells. Meanwhile, deactivated PPC catalyst is difficult to be recycled, thus impairing the economic benefits for the commercial applications. Moreover, because of the side effects of additive corrosion and aging, the carbon and organic binders widely used in current catalyst design would make the interactions of the IOI more complex to accelerate activity loss. Here, we report a Pd/amorphous SrRuO3 (Pd/a-SrRuO3) hybrid film as a promising material to overcome these problems. Perovskite SrRuO3 can effectively generate oxygen-contains (*OH, *OOH) for intermediates oxidation, providing an ideal platform to promote self-cleaning of CO on Pd activity sites. On the other hand, in analogy to typical self-adapting effect of amorphous catalyst in oxygen reduction reaction process, metastable state of amorphous SrRuO3 in this work is expected to prolong the activity adaptation region at the initial stage of cycling. Furthermore, our conceptual framework of directly depositing Pd/a-SrRuO3 film on operational electrode provides an effective solution to avoid the side effects related with carbon and binders, leading to superior reactivation phenomena with 98% efficiency. As a result, our designed Pd/a-SrRuO3 hybrid film exhibits superior EOR activity (4.0 A mg-1 Pd), durability (i-t, 60,000s), self-adapting region (exceeding 400 cycles with ending activity of 3.0 A mg-1 Pd at 1000th cycle), and also a long-term operation (CP) up to 300,000s with 10 times reactivation. This demonstration of a Pd/Pt-based hybrid catalyst with dual-capability of self-cleaning and self-adapting characteristics is an important step towards the development of highly durable EOR catalysts, with an enormous potential to promote practical application of DEFC.

In this communication, we demonstrate the development of nickel oxide nanosheets array on carbon cloth (nio na/cc) as an integrated three-dimensional oxygen-evolving electrode. the electrode exhibits high catalytic activity with an onset overpotential of 295 mv and a tafel slope of 116 mv/dec. it needs an overpotential of 422 mv to drive current density of 10 ma/cm(2) and maintains its catalytic activity for at least 10 h. copyright (c) 2015, hydrogen energy publications, llc. published by elsevier ltd. all rights reserved.

Active and stable electrocatalysts made from earth-abundant elements are key to water splitting for hydrogen production through electrolysis. The growth of NiSe nanowire film on nickel foam (NiSe/NF) in situ by hydrothermal treatment of NF using NaHSe as Se source is presented. When used as a 3D oxygen evolution electrode, the NiSe/NF exhibits high activity with an overpotential of 270 mV required to achieve 20 mA cm(-2) and strong durability in 1.0 M KOH, and the NiOOH species formed at the NiSe surface serves as the actual catalytic site. The system is also highly efficient for catalyzing the hydrogen evolution reaction in basic media. This bifunctional electrode enables a high-performance alkaline water electrolyzer with 10 mA cm(-2) at a cell voltage of 1.63 V.