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At least 289 records · Page 16

Highly Thermal Conductive Nanocomposites

Disclosed are methods for forming carbon-based fillers as may be utilized in forming highly thermal conductive nanocomposite materials. Formation methods include treatment of an expanded graphite with an alcohol/water mixture followed by further exfoliation of the graphite to form extremely thin carbon nanosheets that are on the order of between about 2 and about 10 nanometers in thickness. Disclosed carbon nanosheets can be functionalized and/or can be incorporated in nanocomposites with extremely high thermal conductivities. Disclosed methods and materials can prove highly valuable in many technological applications including, for instance, in formation of heat management materials for protective clothing and as may be useful in space exploration or in others that require efficient yet light-weight and flexible thermal management solutions.

Sun, Ya-Ping↗

Exfoliation of zeolites in functionalized polymers

A method for forming zeolite nanosheets includes forming a mixture including a layered zeolite precursor and a functionalized polymer and exfoliating the layered zeolite precursor to provide the zeolite nanosheets.

36 MATERIALS SCIENCE↗

Surfactant for enhanced oil recovery

A Janus graphene nanosheet (JGN) surfactant formed from a two-dimensional graphene oxide sheet and functionalized to produce an amphiphilic graphene nanosheet. The JGN may be a component of a nanofluid utilized in nanofluid flooding for oil recovery. The JGN may also be used as solid surfactants to form emulsions for oil recovery.

Ren, Zhifeng↗

Phase-inversion polymer composite material, fabricating methods and applications of same

A composite film usable as a separator of an electrochemical device includes hBN nanosheets and at least one polymer. The hBN nanosheets are uniformly dispersed within a matrix of said least one polymer to achieve a highly porous microstructure. Said at least one polymer comprises one or more electrically insulating and electrochemically inert polymers.

Hersam, Mark C.↗

Highly-Cyclable Room-Temperature Phosphorene Polymer Electrolyte Composites for Li Metal Batteries

Despite significant interest toward solid-state electrolytes owing to their superior safety in comparison to liquid-based electrolytes, sluggish ion diffusion and high interfacial resistance limit their application in durable and high-power density batteries. Here, a novel quasi-solid Li + ion conductive nanocomposite polymer electrolyte containing black phosphorous (BP) nanosheets is reported. The developed electrolyte is successfully cycled against Li metal (over 550 h cycling) at 1 mA cm -2 at room temperature. The cycling overpotential is dropped by 75% in comparison to BP-free polymer composite electrolyte indicating lower interfacial resistance at the electrode/electrolyte interfaces. Molecular dynamics simulations reveal that the coordination number of Li + ions around (trifluoromethanesulfonyl)imide (TFSI - ) pairs and ethylene-oxide chains decreases at the Li metal/electrolyte interface, which facilitates the Li + transport through the polymer host. Here, density functional theory calculations confirm that the adsorption of the LiTFSI molecules at the BP surface leads to the weakening of N and Li atomic bonding and enhances the dissociation of Li + ions. This work offers a new potential mechanism to tune the bulk and interfacial ionic conductivity of solid-state electrolytes that may lead to a new generation of lithium polymer batteries with high ionic conduction kinetics and stable long-life cycling.

2D materials↗

High-Performance Piezo-Electrocatalytic Sensing of Ascorbic Acid with Nanostructured Wurtzite Zinc Oxide

We report nanostructured piezoelectric semiconductors offer unprecedented opportunities for high-performance sensing in numerous catalytic processes of biomedical, pharmaceutical, and agricultural interests, leveraging piezocatalysis that enhances the catalytic efficiency with the strain-induced piezoelectric field. Here, we design and demonstrate for the first time a cost-efficient, high-performance piezo-electrocatalytic sensor for detecting L-ascorbic acid (AA), a critical chemical for many organisms, metabolic processes, and medical treatments. We prepared ZnO nanorods and nanosheets to characterize and compare their efficacy for the piezo-electrocatalysis of AA. The electrocatalytic efficacy of AA was significantly boosted by the piezoelectric polarization induced in the nanostructured semiconducting ZnO catalysts. We elucidated the charge transfer between the strained ZnO nanostructures and AA to reveal the mechanism for the related piezo-electrocatalytic process. The low-temperature synthesis of high-quality ZnO nanostructures allows the low-cost, scalable production and integration directly into wearable electrocatalytic sensors whose performance could be boosted by otherwise wasted mechanical energy from the working environment, e.g., the human-generated mechanical signals.

30 DIRECT ENERGY CONVERSION↗

Scalable Graphene Oxide Hollow Fiber Membranes for Dye Desalination Enabled by Multi‐Purpose Polyamine Functionalization

2D nanosheets such as graphene oxide (GO) can be stacked to construct membranes with fine-tuned nanochannels to achieve molecular sieving ability. These membranes are often thin to achieve high water permeance, but their fabrication with consistent nanostructures on a large scale presents an enormous challenge. Herein, GO-based hollow fiber membranes (HFMs) are developed for dye desalination by synergistically combining chemical etching to form in-plane nanopores (10–30 nm) to increase water permeance and polyamine functionalization to improve underwater stability and enable facile large-scale production using existing membrane manufacturing processes. HFM modules with areas of 88 cm 2 and GO layer thicknesses of ≈500 nm are fabricated, and they exhibited a stable dye water permeance of 75 L m −2 h −1 bar −1 , rejection of >99.5% for Direct red and Congo red, and Na 2 SO 4 /dye separation factor of 300–500, superior to state-of-the-art commercial membranes. Furthermore, the versatility of this approach is also demonstrated using different short polyamines and porous substrates. This study reveals a scalable way of designing 2D materials into high-performance robust membranes for practical applications.

amine functionalization↗

Optimizing Vertical Crystallization for Efficient Perovskite Solar Cells by Buried Composite Layers

Planar-heterojunction perovskite solar cells (PSCs) have experienced rapid evolution in recent years because of the low-temperature processing, suitable alignment, and high mobility of the tin oxide buried contact layer. However, improper SnO 2 surface states and poor crystallinity of the top perovskite films are still the main obstacles for the planar PSCs in which performance always lags behind their mesoporous counterparts. Herein, a new buried contact is reported by introducing graphitic carbon nitride (g-C 3 N 4 ) into the commonly used SnO 2 which performs outstanding transmittance, conductivity, and surface states for a high-quality electron-transporting layer. Moreover, the vertical composition and crystallinity of the top perovskite film are manipulated by rich amino groups on the edge of the g-C 3 N 4 nanosheets which induce the prenucleation of the lead-rich species at the buried interface. Benefiting from the high-quality buried contacts and the optimized perovskite layers, the resultant PSCs achieve a champion efficiency of 21.5% with all photovoltaic parameters enhanced in comparison with their control counterparts (<20%).

planar-heterojunction perovskite solar cells↗

Scalable thin graphene oxide membranes enabled by polydopamine gutter layer

Two-dimensional (2D) nanosheets have been widely used to fabricate thin-film composite membranes for dye desalination. However, they often need to be thick to mitigate the defects resulting from their random stacking and rough support surface. Herein, bio-adhesive polydopamine (PDA) is used as a gutter layer to prepare graphene oxide (GO)-based membranes by improving the adhesion between the GO and porous support and providing a smooth surface to form thin, highly selective layers. For example, the PDA priming reduces the GO layer thickness by 57 %, from 447 to 190 nm, while achieving similar dye desalination properties. The effect of the dopamine concentration, exposure time, and GO layer thickness on the membrane structure and desalination performance are thoroughly investigated using various techniques, such as scanning electron microscopy (SEM), x-ray photoelectron spectroscopy (XPS), and x-ray diffraction (XRD). The PDA gutter layer is also applied for hollow fiber membranes, achieving water permeance of 79 L m -2 h −1 bar−1 and rejection of ∼99 % for Direct red 80. The membranes were challenged by simulated dye/salt mixtures to elucidate the complicated effect of the compositions on the desalination performance. Furthermore, this study unveils a new avenue to improve separation performance and large-scale manufacturability of 2D material-based membranes.

Dye desalination↗

Atomically dispersed Pt single sites and nanoengineered structural defects enable a high electrocatalytic activity and durability for hydrogen evolution reaction and overall urea electrolysis

The scarcity and high cost of PGM electrocatalysts are the key bottleneck in the mass-scale commercialization of many electrolysis technologies. Bifunctional single-atom electrocatalysts (SACs) are promising alternatives for PGM electrocatalysts in next-generation electrolysis technologies because of their superior intrinsic activity and perfect atom utilization. Regulating the coordination environment of platinum atomic sites identifies their electrocatalytic performance. Therefore, exploring more appropriate supports could facilitate the construction of active and durable electrocatalysts with ultralow noble metal content. Herein, we report on a reliable approach for producing a novel type of SACs composed of atomically dispersed Pt active sites stabilized on defective NiCo layered double hydroxide (Pt/D-NiCo LDH) nanosheets as an ultralow-Pt hybrid electrocatalyst for hydrogen evolution reaction (HER), urea oxidation reaction (UOR), and full urea-water electrolysis. The optimized Pt 1 /D NiCo LDH-24 SAC displays a remarkable HER and UOR performance where it yields a current density of 10 mA cm -2 at 37 mV and 1.25 V vs. RHE for HER and UOR, respectively. Finally, symmetrical urea electrolyzer constructed of Pt 1 /D-NiCo LDH-24 electrodes attains 10 mA cm -2 at a cell voltage of 1.32 V vs. RHE, demonstrating superior activity and durability over 60 h operation when compared to commercial Pt/C( + )||RuO 2 ( - ) system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Understanding Charge Storage in Hydrated Layered Solids MOPO 4 (M = V, Nb) with Tunable Interlayer Chemistry

Hydrated layered solids are interesting charge storage hosts with potentially high electrochemical activity and interlayer tunability. Although it is often possible to tune their interlayer distance by a pillaring strategy, the poor electrochemical stability of such artificial structures remains a major issue in device operation. Here we investigate the charge storage properties of MOPO 4 (M = V, Nb) hydrates with a nanosheet morphology to understand the influence of the interlayer environment on cycling stability, as well as ion selectivity. While in hydrated VOPO 4 interlayer H 2 O molecules act as compressible springs to enable fast Li-/Na-ion transport kinetics and reasonable structural reversibility, NbOPO 4 layers with bridging PO 4 groups serving as permanent linkers exhibit highly stable cyclability for Li-ions, owing to a zero-volume-change ion transport process. However, the latter suffers from a much larger migration energy barrier for Na-ions. Lastly, our findings not only highlight a structurally intriguing material system, but also provide insights into reviving materials with an originally unstable interlayer chemical environment, and shed light on the design principles for creating electrochemically stable charge storage hosts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomic-Scale Dynamic Mechanisms of Embedded MoS 2 Wires

Nanowires composed of a 1:1 stoichiometry of transition metals and chalcogen ions can be fabricated from two-dimensional transition metal dichalcogenides (TMDs) by using electron beam irradiation. Wires fabricated through in situ experiments can be geometrically connected to TMD sheets in various ways, and their physical properties can vary accordingly. Understanding the structural transformation caused by electron beams is critical for designing wire-sheet structures for nanoelectronics. In this study, we report the behavior of nanowires formed inside a monolayer MoS 2 sheet by combining phase-contrast images and large-scale atomistic modeling. Here we investigate the effect of vacancies on the dynamic evolution of wires, such as rotations with different edge structures and breaking, by considering the interactions between MoS wires and MoS 2 nanosheets. The obtained insights can be applied to other monolayer TMDs to guide the behavior of TMD wires and fabricate favorable geometries for various applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hydrogen-Bonding Reinforced Flexible Composite Electrodes for Enhanced Energy Storage

The lack of advanced electrode materials is one of the main factors hindering the development of flexible rechargeable aqueous batteries (RABs) for high specific energy density and structural stability. It is also challenging to achieve high-capacity performance for both the positive and negative electrodes simultaneously. In this work, it is demonstrated that, by smartly designing the composite structures of positive and negative electrodes via one-step electrodeposition strategy, the energy storage performance of the RAB is largely enhanced. For positive electrode material synthesis, Co-Cu double hydroxides (Co-Cu-DH) nanosheets are skillfully rooted into electroreduced graphene oxide (eRG) via hydrogen bonding, in which graphene oxide reduction, Co-Cu-DH nucleation/growth, and formation of hydrogen bonding between Co-Cu-DH and eRG simultaneously occur. Moreover, when a RAB based on Co-Cu-DH@eRG//FeOOH@eRG using the same composite design strategy is established, a wide operating voltage window of ≈1.8 V, a high specific energy density of ≈142.8 Wh kg –1 at ≈890 W kg –1 , and long-term cyclic stability (88.5% of capacity retention after 12 000 cycles) are obtained. This study presents a general compositing strategy for the development of advanced electrode materials, and it is expected to stimulate future material synthesis/design in RABs toward the goal of high energy density storage.

25 ENERGY STORAGE↗

Construction of a Pt‐CeO x Interface for the Electrocatalytic Hydrogen Evolution Reaction

Abstract The creation of metal‐metal oxide interfaces is an important approach to fine‐tuning catalyst properties through strong interfacial interactions. This article presents the work on developing interfaces between Pt and CeO x that improve Pt surface energetics for the hydrogen evolution reaction (HER) within an alkaline electrolyte. The Pt‐CeO x interfaces are formed by depositing size‐controlled Pt nanoparticles onto a carbon support already coated with ultrathin CeO x nanosheets. This interface structure facilitates substantial electron transfer from Pt to CeO x , resulting in decreased hydrogen binding energies on Pt surfaces, and water dissociation for the HER, as predicted by the density functional theory (DFT) calculations. Electrochemical testing indicates that both Pt specific activity and mass activity are improved by a factor of 2 to 3 following the formation of Pt‐CeO x interfaces. This study underscores the significance and potential of harnessing robust interfacial effects to enhance electrocatalytic reactions.

25 ENERGY STORAGE↗

Oxidation‐Driven Enhancement of Intrinsic Properties in MXene Electrodes for High‐Performance Flexible Energy Storage

Abstract MXenes, a novel class of 2D materials, exhibit great potential for energy storage due to their unique layered structure and excellent electrical conductivity. However, improving the intrinsic electrochemical storage capacity of MXenes remains a significant challenge, often requiring the incorporation of other Faradaic materials. Oxidation, in particular, poses a key issue that impacts the capacity of MXene devices. In this study, controlled oxidation is employed to create nanoscale holes within MXene, transforming them into holey MXene (H‐MXene) nanosheets. These porous structures shorten ion transport distances and increase ion transport pathways, thereby significantly enhancing the electrochemical storage capacity of MXenes. The resulting H‐MXene micro‐supercapacitors (MSCs) demonstrate exceptional performance, achieving an aerial capacitance 2.5 times that of unmodified MXene electrodes, along with excellent cycling stability, retaining 91.7% of their capacitance after 10 000 cycles. Additionally, a flexible integrated system combining energy storage and sensing functionalities is developed, showcasing its scalability in self‐powered sensing applications. The incorporation of self‐healing polyurethane (PU) enables the device to retain 90% of its storage capacity after undergoing self‐healing. This study presents a novel approach for developing high‐performance MXene‐based energy storage devices and provides valuable insights into efficient ion transport and storage in 2D materials.

Cheng, Yongfa [Department of Materials Science and↗

Efficient Energy Funneling in Quasi‐2D Perovskites: From Light Emission to Lasing

Abstract Quasi‐2D Ruddlesden–Popper halide perovskites with a large exciton binding energy, self‐assembled quantum wells, and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi‐2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower‐dimensional nanosheets (high‐bandgap domains) to 3D nanocrystals (low‐bandgap domains). High‐quality quasi‐2D perovskite (PEA) 2 (FA) 3 Pb 4 Br 13 films are fabricated by solution engineering. Grazing‐incidence wide‐angle X‐ray scattering measurements are conducted to study the crystal orientation, and transient absorption spectroscopy measurements are conducted to study the charge‐carrier dynamics. These data show that highly oriented 2D crystal films have a faster energy transfer from the high‐bandgap domains to the low‐bandgap domains (<0.5 ps) compared to the randomly oriented films. High‐performance light‐emitting diodes can be realized with these highly oriented 2D films. Finally, amplified spontaneous emission with a low threshold 4.16 µJ cm −2 is achieved and distributed feedback lasers are also demonstrated. These results show that it is important to control the morphology of the quasi‐2D films to achieve efficient energy transfer, which is a critical requirement for light‐emitting devices.

Lei, Lei↗

3D Artificial Solid-Electrolyte Interphase for Lithium Metal Anodes Enabled by Insulator–Metal–Insulator Layered Heterostructures

Despite considerable efforts to prevent lithium (Li) dendrite growth, stable cycling of Li metal anodes with various structures remains extremely difficult due to the direct contact of the liquid electrolyte with Li. Rational design of solid-electrolyte interphase (SEI) for 3D electrodes is a promising but still challenging strategy for preventing Li dendrite growth and avoiding lithium–electrolyte side reactions in Li-metal batteries. Here, a 3D architecture is constructed with g-C 3 N 4 /graphene/g-C 3 N 4 insulator–metal–insulator sandwiched nanosheets to guide uniform Li plating/stripping in the van der Waals gap between the graphene and the g-C 3 N 4 , and the function of which can be regarded as a 3D artificial SEI. Li deposition on the surface of g-C 3 N 4 is suppressed due to its insulating nature. However, its uniform lithiophilic sites and nanopore channels enable homogeneous lithium plating between the graphene and the g-C 3 N 4 , prohibiting the direct contact of the electrolyte with the Li metal. The use of the g-C 3 N 4 -layer-modified 3D anode enables long-term Li deposition with a high Coulombic efficiency and stable cycling of full cells under high cathode loading, limited Li excess, and lean electrolyte conditions. The concept of a 3D artificial SEI will shed light on developing safe and stable Li-metal anodes.

25 ENERGY STORAGE↗