The key to fully realizing the potential of high-entropy alloys (HEAs) lies in balancing their inherent local chemical disordering with the long-range ordering required for electrochemical applications. Herein, we synthesized a distinctive L1-(PtIr)(FeMoBi) high-entropy intermetallics (HEIs) exhibiting nanoscale long-range order and atomic scale short-range disorder via a lattice compensation strategy to mitigate the entropy reduction tendency. The (PtIr)(FeMoBi) catalyst exhibited remarkable activity and selectivity of glycollic acid (GA) production via electrocatalytic waste polymer-derived ethylene glycol oxidation reaction (EGOR).
View Article and Find Full Text PDFWhile high-entropy alloy (HEA) catalysts seem to have the potential to break linear scaling relationships (LSRs) due to their structural complexity, the weighted averaging of properties among multiple principal components actually makes it challenging to diverge from the symmetry dependencies imposed by the LSRs. Herein, we develop a 'surface entropy reduction' method to induce the exsolution of a component with weak affinity for others, resulting in the formation of few-atom-layer metal (FL-M) on the surface of HEAs. These exsolved FL-M surpass the confines of the original configurational space of conventional HEAs, and collaborate with the HEA substrate, serving as geometrically separated active sites for multiple intermediates in a complex reaction.
View Article and Find Full Text PDFCyclo[n]carbons have recently attracted significant attention owing to their geometric and electronic structures remaining largely unexplored in the condensed phase. In this work, we focus on two anti-aromatic cyclocarbons, namely C and C. By designing two fully halogenated molecular precursors both including 4-numbered rings, we further extend the on-surface retro-Bergman ring-opening reaction, and successfully produce C and C.
View Article and Find Full Text PDFSwelling is a very common phenomenon in organic substances. However, the swelling behaviors of inorganic substances had rarely been reported. In this study, a new type of swellable organic-inorganic hybrid polymer (PIL@CHT) was designed and successfully synthesized through free-radical copolymerization of polymerizable phosphonium ionic liquid monomer and vinyl-functionalized hydrotalcite (CHT).
View Article and Find Full Text PDFIn this work, a novel ABA-type triblock polycarboxylate superplasticizers (PCEs) with well defined molecular structures were designed and synthesized, firstly, by reversible addition-fragmentation chain transfer (RAFT) polymerization, to explore the structure-property relationship PCEs in the β-hemihydrate gypsum (β-HH) system. Three PCEs with the same molecular weight and different structure were obtained by changing the feed ratio of the RAFT agent, initiator, and monomer. The effect of the chemical structure of PCEs on their dispersing property and water reduction capacity were assessed in gypsum by measuring the flowability of pastes and the adsorption ability of PCEs on gypsum.
View Article and Find Full Text PDFPolymers (Basel)
September 2022
Polyurethane (PU) can be used as a road material binder, and its mechanical properties, durability, temperature stability, and other road performance metrics are good. However, the interlayer bonding between PU mixtures and asphalt mixtures is poor. The influence of the pavement structure, interlayer treatment scheme, load, and environmental factors on the interlayer shear characteristics of PU mixture composite pavement is analysed.
View Article and Find Full Text PDFIn this work, we report a hybrid lithographic method that combines the top-down soft lithography and the bottom-up hydrothermal approach for growing single-crystalline TiO nanorod arrays with arbitrary patterns. The arbitrary patterns of TiO seeds were obtained through the microcontact printing of the TiO seed precursor onto Si substrates using prepatterned poly(dimethylsiloxane) (PDMS) as stamps, followed by a baking process. Afterward, TiO nanorod arrays were selectively grown on patterned TiO seeds through conventional hydrothermal methods.
View Article and Find Full Text PDFHigh-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates.
View Article and Find Full Text PDFACS Appl Mater Interfaces
May 2022
Supercapacitors have received much attention as large-scale energy storage devices for high power density and ultralong cycling life. In this work, sodium vanadate NaVO/poly(3,4-ethylenedioxythiophene) (PEDOT) nanocables with deficient bridge oxygen at the interface (denoted Vo-PNVO) have been tailored for supercapacitors through the polymerization of 3,4-ethylenedioxythiophene and studied using three different electrolytes. Experiments and theoretical calculations reveal that all Na, Zn, and Al ions appear as hydrates in aqueous solutions but insert into the crystal structure as Na ions and Zn-HO and Al-HO hydrates, respectively.
View Article and Find Full Text PDFHaloazaphosphatranes are the halogenated parents of proazaphosphatranes, also known as Verkade's superbase. While the synthesis of iodo-, bromo- and chloroazaphosphatranes was reported more than thirty years ago by J. G.
View Article and Find Full Text PDFBioactive compound 3-aryl-2-oxazolidinone could be synthesized by a green method mixing carbon dioxide, aniline, and ethylene oxide. Our group previously proposed a parallel mechanism for this conversion catalyzed by ionic liquids. Recently, a new study on a similar reaction system of styrene oxide, carbon dioxide, and aniline under the catalysis of KPO gave a different serial mechanism.
View Article and Find Full Text PDFIt is essential to control concentration gradients at specific locations for many biochemical experiments. This paper proposes a tunable concentration gradient generator actuated by acoustically oscillating bubbles trapped in the bubble channels using a controllable position based on the gas permeability of polydimethylsiloxane (PDMS). The gradient generator consists of a glass substrate, a PDMS chip, and a piezoelectric transducer.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2020
For applications in energy storage and conversion, many metal oxide (MO)/C composite fibers have been synthesized using cellulose as the template. However, MO particles in carbon fibers usually experience anomalous growth to a size of >200 nm, which is detrimental to the overall performance of the composite. In this paper, we report the successful development of a generic approach to synthesize a fiber composite with highly dispersed MO nanoparticles (10-80 nm) via simple swelling, nitrogen doping, and carbonization of the cellulose microfibril.
View Article and Find Full Text PDFRegulating chemical bonds to balance the adsorption and disassociation of water molecules on catalyst surfaces is crucial for overall water splitting in alkaline solution. Here we report a facile strategy for designing NiWC-WC Janus structures with abundant Ni-W metallic bonds on surfaces through interfacial engineering. Inserting Ni atoms into the WC crystals in reaction progress generates a new NiWC phase, making the inert W atoms in WC be active sites in NiWC for overall water splitting.
View Article and Find Full Text PDFVanadium pentoxide (V2O5)-based composites show outstanding performances as cathode materials in lithium-ion batteries. However, their inferior thermal conductivity restricts the heat dissipation through the cathode electrode. In this study, we measured the thermal conductivity of V2O5 nanowires using the thermal bridge method and found that their thermal conductivity is 3.
View Article and Find Full Text PDFWith the development of micro/nano satellites and formation flying, more advanced spatial propulsion technology is required. In this paper, a review of microthrusters developments that based on micro electromechanical systems (MEMS) technology adopted in microthrusters is summarized. The microthrusters in previous research are classified and summarized according to the types of propellants and the working principles they utilized.
View Article and Find Full Text PDFDeveloping highly efficient electrocatalysts while revealing the active site and reaction mechanism is essential for electrocatalytic water splitting. To overcome the number and location limitations of defects in the electrocatalyst induced by conventional transition-metal atom (e.g.
View Article and Find Full Text PDFThe homogeneous cycloaddition reaction of CO and epichlorohydrin catalyzed by amine-functionalized ionic liquid (AFIL) to yield cyclic carbonate is reported in this study. The AFIL has the dual function of ionic liquid and organic base. The experimental study indicates that AFIL can efficiently catalyze the conversion of CO and epichlorohydrin to the product 3-chloro-1,2-propylene.
View Article and Find Full Text PDFCompared with nanosized materials, the long-pathway isolation of the interior part from the electrolyte for bulk electrode materials may result in high ionic diffusion barrier, leading to the poor rate behavior. Either the modification of lattice or the construction of a porous structure is generally effective to decrease the ion-diffusion barrier; however, achieving these multiscaled modulations simultaneously via a facile approach is still a challenge. Herein, we manipulate a bifunctional dopant to prepare micron-sized NaV(PO) with extraordinary synergy of hierarchical architecture and lattice distortion.
View Article and Find Full Text PDFA local electric field is induced to engineer the interface of vanadium pentoxide nanofibers (V O -NF) to manipulate the charge transport behavior and obtain high-energy and durable supercapacitors. The interface of V O -NF is modified with oxygen vacancies (Vö) in a one-step polymerization process of polyaniline (PANI). In the charge storage process, the local electric field deriving from the lopsided charge distribution around Vö will provide Coulombic forces to promote the charge transport in the resultant Vö-V O /PANI nanocable electrode.
View Article and Find Full Text PDFOxygen vacancies (Vö) play a crucial role in energy storage materials. Oxygen-vacancy-enriched vanadium pentoxide/poly(3,4-ethylenedioxythiophene) (Vö-VO/PEDOT) nanocables were prepared through the one-pot oxidative polymerization of PEDOT. PEDOT is used to create tunable concentrations of Vö in the surface layer of VO, which has been confirmed by X-ray absorption near edge structure (XANES) analysis and X-ray photoelectron spectroscopy (XPS) measurements.
View Article and Find Full Text PDFA method for the qualitative analysis of compositions of anthraquinone working solution (WS)/hydrogenated working solution (HWS) by gas chromatography-mass spectrometry (GC-MS) was developed. The composition of ethylanthraquinone (eAQ) WS/HWS was identified by GC-MS. Then the samples of amylanthraquinone (AAQ) WS/HWS were analyzed by GC-MS.
View Article and Find Full Text PDFACS Appl Mater Interfaces
April 2019
A kind of oil/water separation membrane, combining poly(ionic liquid) (PIL) and three-dimensional (3D) wire mesh, was designed and prepared via one-step photopolymerization of an ionic liquid monomer 1,8-triethylene glycoldiyl-3,3'-divinylimidazolium dibromide ([DVIm-(EG)]Br) with acrylic acid in the mesh. The composite membrane (PIL@Mesh) had the advantages of anti-oil-adhesion property and high mechanical strength simultaneously. The morphology of PIL@Mesh characterized by scanning electron microscopy (SEM) and Cryo-SEM demonstrated that PIL swelled in water to construct microscale 3D networks.
View Article and Find Full Text PDFA soluble and easily dispersive cross-linked poly(ionic liquid), copolymer of 1-vinyl-3-butylimidazolium bromide ([VBIM][Br]) and divinylbenzene (DVB), was used as a precursor for nitrogen doped porous carbons (NPCs) with SiO (from tetraethyl orthosilicate) as a template. The NPCs were characterized by infrared (IR) spectroscopy, nitrogen adsorption-desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Raman spectroscopy, thermo gravimetric analysis (TGA), elemental analysis and X-ray photoelectron spectroscopy (XPS). The specific surface area and porosity of NPCs depended on the carbonization temperature, the SiO/[VBIM][Br] ratio and the precursors.
View Article and Find Full Text PDFPhys Chem Chem Phys
February 2019
The electrochemical properties of VPO4O as a cathode for Mg batteries were studied by performing first principles calculations. Mg insertion features a plateau at about 2.8 V up to Mg0.
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