Both the physicochemical properties of catalytic material and the structure of loaded catalyst layer (CL) on gas diffusion electrode (GDE) are of crucial importance in determining the conversion efficiency and product selectivity of carbon dioxide reduction reaction (CORR). However, the highly reducing reaction condition of CORR will lead to the uncontrollable structural and compositional changes of catalysts, making it difficult to tailor surface properties and microstructure of the real active species for favored products. Herein, the interlayer microenvironment of copper-based layered double hydroxides (LDHs) is rationally tuned by a facile ink solvent engineering, which affects both the surface characters and microstructure of CL on GDE, leading to distinct catalytic activity and product selectivity.
View Article and Find Full Text PDFThe development of bifunctional, non-noble metal-based electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) through morphology and electronic engineering is highly attractive for efficient water splitting. Herein, hierarchical nanoarrays consisting of crystalline cobalt phosphide nanorods covered by amorphous Fe-doped cobalt phosphide nanocuboids (CoP/FeCoP) are constructed as bifunctional catalysts for both HER and OER. Experimental results and theoretical calculations reveal that the catalysts exhibit balanced dual-catalytic properties due to simultaneous introduction of Fe doping and phosphorus vacancies, leading to an optimized electronic structure of the CoP/FeCoP.
View Article and Find Full Text PDFEfficient thermal management is essential for low-temperature optoelectronic devices. Traditional liquid nitrogen (LN2) cooling presents challenges such as frequent replenishment needs and limited operational duration. This study introduces micromachined Joule-Thomson (MJT) cooling as a superior alternative for temperature regulation in optoelectronic devices.
View Article and Find Full Text PDFSelf-assembly of nanoparticles into supercrystals represents a powerful approach to create unique and complex superstructures with fascinating properties and novel functions, but the complexity in spatial configuration, and the tunability in lattice structure are still quite limited compared to the crystals formed by atoms and molecules. Herein, shallowly concave gold nanoarrows with a unique concave-convex geometry are synthesized and employed as novel building blocks for shape-directed self-assembly of a wealth of complex 3D supercrystals with unprecedented configurations. The obtained diverse superstructures including six Interlocking-type supercrystals and three Packing-type supercrystals exhibit four types of Bravais lattices (i.
View Article and Find Full Text PDFLiquid-phase electron microscopy (LP-EM) imaging has revolutionized our understanding of nanosynthesis and assembly. However, the current closed geometry limits its application for open systems. The ubiquitous physical process of the coffee-ring phenomenon that underpins materials and engineering science remains elusive at the nanoscale due to the lack of experimental tools.
View Article and Find Full Text PDFPhotoelectrochemical (PEC) water splitting represents an attractive strategy to realize the conversion from solar energy to hydrogen energy, but severe charge recombination in photoanodes significantly limits the conversion efficiency. Herein, a unique BiVO (BVO) nanobowl (NB) heterojunction photoanode, which consists of [001]-oriented BiOCl underlayer and BVO nanobowls containing embedded BiOCl nanocrystals, is fabricated by nanosphere lithography followed by in situ transformation. Experimental characterizations and theoretical simulation prove that nanobowl morphology can effectively enhance light absorption while reducing carrier diffusion path.
View Article and Find Full Text PDFAlthough zinc-based batteries are promising candidates for eco-friendly and cost-effective energy storage devices, their performance is severely retarded by dendrite formation. As the simplest zinc compounds, zinc chalcogenides, and halides are individually applied as a Zn protection layer due to high zinc ion conductivity. However, the mixed-anion compounds are not studied, which constrains the Zn diffusion in single-anion lattices to their own limits.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2022
Lithium metal is the most promising anode for lithium batteries, but the growth of lithium dendrites leads to rapid attenuation of battery capacity and a series of safety problems during the plating/stripping process. Utilization of carbon materials for improving the Li metal anode stability represents a feasible strategy; particularly, the high affinity for lithium endows graphdiyne (GDY) with a promising capability for stabilizing Li metal anodes. Herein, vertically aligned GDY nanowalls (NWs) were uniformly grown on a copper foil, which allowed for dendrite-free, columnar deposition of lithium, desired for a stable Li metal anode.
View Article and Find Full Text PDFFormamidinium-cesium (FA-Cs) perovskites are an attractive candidate for perovskite solar cells (PSCs) with high stability, but they tend to suffer from high intrinsic defect density, especially at grain boundaries. Herein, a common heterocyclic conjugated molecule, orotic acid (ORO), was employed as a novel bifunctional additive to simultaneously achieve crystallization regulation and defect passivation of an FA-Cs perovskite toward efficient and stable PSCs. ORO was introduced to an FA-Cs perovskite precursor solution as an effective coordination-induced crystallization regulator to improve the grain size and crystallinity.
View Article and Find Full Text PDFDeveloping efficient, nanostructured electrocatalysts with the desired compositions and structures is of great significance for improving the efficiency of water splitting toward hydrogen production. In this regard, metal-organic framework (MOF) derived nanoarrays have attracted great attention as promising electrocatalysts because of their diverse compositions and adjustable structures. In this review, the recent progress in MOF-derived nanoarrays for electrochemical water splitting is summarized, highlighting the structural design of the MOF-derived nanoarrays and the electrocatalytic performance of the derived composite carbon materials, oxides, hydroxides, sulfides, and phosphides.
View Article and Find Full Text PDFPhotoelectrochemical (PEC) water splitting is a promising way to convert solar energy into hydrogen energy, but the efficiency is limited by severe charge recombination especially in photoanodes. Herein, to reduce the charge recombination in the bulk phase and at the surface of the BiVO photoanodes, oxygen vacancy introduction and cocatalyst loading were realized simultaneously by one-step photocathode deposition. A unique re-BiVO/FeOOH photoanode was obtained by the photocathodic reduction of BiVO in an electrolyte containing Fe, where the oxygen vacancies were introduced during the reduction process and the deposition of the FeOOH cocatalyst on the surface was induced by the generated OH.
View Article and Find Full Text PDFResearch (Wash D C)
July 2021
Programing the self-assembly of colloidal nanoparticles into predetermined superstructures represents an attractive strategy to realize functional assemblies and novel nanodevices, but it remains a challenge. Herein, gold nanoarrows (GNAs) showing a distinct convex-concave structure were employed as unique building blocks for programmable self-assembly involving multiple assembly modes. Regioselective adsorption of 1,10-decanedithiol on the vertexes, edges, and facets of GNAs allowed for programmable self-assembly of GNAs with five distinct assembly modes, and regioselective blocking with 1-dodecanethiol followed by adsorption of 1,10-decanedithiol gave rise to programmable self-assembly with six assembly modes including three novel wing-engaged modes.
View Article and Find Full Text PDFControlling and tuning surface properties of a catalyst have always been a prime challenge for efficient hydrogen production water splitting. Here, we report a facile method for tuning both charger transfer and sorption-desorption properties of NiFe layered double hydroxide (LDH) by intercalating a conductive polymer of polypyrrole (ppy) an interlayer confined polymerization synthesis (ICPS) process. characterizations and electrochemical quartz-crystal microbalance with dissipation (EQCM-D) tracking experiments showed that the intercalated ppy not only improved the charge transfer property of the resulting hybrid catalyst LDH-ppy but also made it more flexible and adaptive for quick and reversible sorption-desorption of reactants and intermediates during the oxygen evolution reaction (OER) process.
View Article and Find Full Text PDFPhytolith-occluded carbon (PhytOC) is an important long-term stable carbon fraction in grassland ecosystems and plays a promising role in global carbon sequestration. Determination of the PhytOC traits of different plants in major grassland types is crucial for precisely assessing their phytolith carbon sequestration potential. Precipitation is the predominant factor in controlling net primary productivity (NPP) and species composition of the semiarid steppe grasslands.
View Article and Find Full Text PDFβ-Phase anhydrous guanine (β-AG) crystals are one of the most widespread organic crystals to construct optical structures in organisms. Currently, no synthetic method is available that allows for producing guanine crystals with similar control in size, morphology, and crystallography as in biological ones. Herein, a facile one-step synthesis route to fabricate bio-inspired guanine microplatelets with (100) exposing planes in almost pure β-phase is reported.
View Article and Find Full Text PDFWe use liquid-phase transmission electron microscopy (TEM) to study self-assembly dynamics of charged gold nanoarrows (GNAs), which reveal an unexpected "colloid-atom duality". On one hand, they assemble following the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory for when van der Waals attraction overruns slightly screened electrostatic repulsion. Due to concaveness in shape, GNAs adopt zipper motifs with lateral offset in their assembly matching with our modeling of inter-GNA interaction, which form into unconventional structures resembling degenerate crystals.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2020
The development of transition-metal-oxides (TMOs)-based bifunctional catalysts toward efficient overall water splitting through delicate control of composition and structure is a challenging task. Herein, the rational design and controllable fabrication of unique heterostructured inter-doped ruthenium-cobalt oxide [(Ru-Co)O ] hollow nanosheet arrays on carbon cloth is reported. Benefiting from the desirable compositional and structural advantages of more exposed active sites, optimized electronic structure, and interfacial synergy effect, the (Ru-Co)O nanoarrays exhibited outstanding performance as a bifunctional catalyst.
View Article and Find Full Text PDFA seed-mediated electroless deposition (SMED) approach for fabrication of large-area and uniform gold nanoparticle films as efficient and reproducible as surface-enhanced Raman scattering (SERS) substrates was presented. This approach involved a seeding pretreatment procedure and a subsequent growth step. The former referred to activation of polylysine-coated glass slides in gold seed solution, and the latter required a careful control of the reactant concentration and reaction time.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2018
One of the key aspects contributing to the rapid development of perovskite solar cells is to prepare high-quality perovskite films via morphology control and interface engineering. Here, we demonstrate that the additive HPbI works effectively on both morphology control and grain boundary passivation of CHNHPbICl thin films. By inducing HPbI to the crystal transformation process, high-quality perovskite films consisting of micro-sized grains with boundaries passivated by PbI can be readily produced.
View Article and Find Full Text PDFAn efficient photoanode based on CdS nanorod@SnO nanobowl (CdS NR@SnO NB) arrays is designed and fabricated by the preparation of SnO nanobowl arrays via nanosphere lithography followed by hydrothermal growth of CdS nanorods on the inner surface of the SnO nanobowls. A photoelectrochemical (PEC) device constructed by using this hierarchical CdS NR@SnO NB photoanode presents significantly enhanced performance with a photocurrent density of 3.8 mA cm at 1.
View Article and Find Full Text PDFSelf-assembly of colloidal nanocrystals into complex superstructures offers notable opportunities to create functional devices and artificial materials with unusual properties. Anisotropic nanoparticles with nonspherical shapes, such as rods, plates, polyhedra, and multipods, enable the formation of a diverse range of ordered superlattices. However, the structural complexity and tunability of nanocrystal superlattices are restricted by the limited geometries of the anisotropic nanoparticles available for supercrystal self-assembly.
View Article and Find Full Text PDFSci Bull (Beijing)
September 2017
Long wavelength light-responsive drug delivery systems based on mesoporous silica nanoparticles (MSNs) have attracted much attention in the last few years. In this paper, a red light (660 nm)-responsive drug delivery system based on low-cost cyclodextrin (CD)-gated MSNs containing a photodynamic therapy (PDT) photosensitizer (Chlorin e6, Ce6) was developed for the first time. The drug release experiment in water demonstrated that with the irradiation of red light, Ce6 can be excited to generate singlet oxygen, which can further cleave the singlet oxygen sensitive linker to trigger the departure of CD and the release of cargo.
View Article and Find Full Text PDFThe rational design and controllable fabrication of electrode materials with tailored structures and superior performance is highly desirable for the next-generation lithium ion batteries (LIBs). In this work, a novel three-dimensional (3D) graphite foam (GF)@SnO nanorod arrays (NRAs)@polyaniline (PANI) hybrid architecture was constructed via solvothermal growth followed by electrochemical deposition. Aligned SnO NRAs were uniformly grown on the surface of GF, and a PANI shell with a thickness of ∼40 nm was coated on individual SnO nanorods, forming a SnO@PANI core-shell structure.
View Article and Find Full Text PDFA novel multifunctional composite comprising mesocrystalline SnO nanorods (NRs) vertically aligned on reduced graphene oxide (rGO) sheets was synthesized and developed for sequential capture of endogenous peptides and phosphopeptides. With the hydrophobicity of rGO and high affinity of SnO nanorods, sequential enrichment of endogenous peptides and phosphopeptides could be easily achieved through a modulation of elution buffer. With this multifunctional nanomaterial, 36 peptides were observed from diluted bovine serum albumin (BSA) tryptic digest and 4 phosphopeptides could be selectively captured from β-casein digest.
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