RESUMEN
Designing in-plane supercapacitors with high electrode materials selectivity is an indispensable approach to improve electrochemical performance. In this work, a facile template method was employed to fabricate in-plane supercapacitors. This template method could select any electrochemical active materials as electrode materials of in-plane supercapacitors. Hence, a high electrochemical performance material Mn-Co LDO-2S with optimized metal-sulfur bonds proportion and abundant sulfur vacancies was employed as electrode material of symmetrical in-plane supercapacitor (SPS). SPS exhibits excellent electrochemical performance finally, and has considerable area energy density 55.0µWh cm-2with an area power density of 0.7 mW cm-2. As a result, introducing sulfur atoms and sulfur vacancies are efficient approaches to improve electrode materials' electrochemical performance, and template method that proposed in this work is a promising approach to widen selectivity of in-plane supercapacitors' electrode materials.
RESUMEN
Moiré superlattices (MSLs) of two-dimensional (2D) van der Waals materials have attracted considerable attention in recent years; however, studies of bottom-up growth of twisted MSL structures via solution-processed crystallization are rarely reported. Through facile one-pot solvothermal synthesis, here we demonstrate a nonclassical surfactant/nanosheet-co-mediated crystallization pathway for formation of MSL structures with two models of SnS2 and SnSe2. Our experimental results reveal that attractive interactions between 2D inorganic building blocks and surfactant organic molecules during the initial stage of crystallization are crucial to drive surfactant-covered nanosheets to crystallize into molecule-intercalated nanosheet aggregates. Under the high-pressure condition, further crystallograpic fusion can occur if the reaction time is prolonged, which alters the interactions of adjacent layers during the coalescence of small-grain-size 2D domains due to insertion of foreign molecules, leading to interlayer rotations. This work uncovers an interesting organic-inorganic cocrystallization growth mode and provides a novel pathway for large-scale fabrication of MSLs.
RESUMEN
Integrating the battery behavior and supercapacitor behavior in a single electrode to obtain better electrochemical performance has been widely researched. However, there is still a lack of research studies on an integrated battery-capacitor supercapacitor electrode (BatCap electrode). In this work, an integrated BatCap electrode porous carbon-coated Mn-Ni-layered double oxide (Mn-Ni LDO-C) was fabricated successfully using controllable heat treatment of polypyrrole-precoated Mn-Ni-layered double hydroxide (Mn-Ni LDH@PPy). This Mn-Ni LDO-C electrode was grown on Ni foam directly and possessed a hierarchical structure that consisted of a pyridinic N (N-6)-doped porous carbon shell and a Mn-Ni LDO core within abundant oxygen vacancies. Benefiting from the synergistic effect of N-6-doped porous carbon and increased oxygen vacancies, Mn-Ni LDO-C exhibited excellent electrochemical performance. The capacity of Mn-Ni LDO-C reached 2.36 C cm-2 (1478.1 C g-1) at 1 mA cm-2 and remained at 92.1% of the initial capacity after 5000 cycles at a current density of 20 mA cm-2. The aqueous battery-supercapacitor hybrid device Mn-Ni LDO-C//active carbon (Mn-Ni LDO-C//AC) also presented superior cycle stability: it retained 85.3% of the original capacity after 5000 cycles at 2 A g-1. Meanwhile, Mn-Ni LDO-C//AC could work normally under a wider potential window (2.0 V), so that the device held the highest energy density of 78.2 Wh kg-1 at a power density of 499.7 W kg-1 and retained 39.1 Wh kg-1 at the highest power density of 31.3 kW kg-1. Two Mn-Ni LDO-C//AC devices connected in series could light a light-emitting diode (LED) bulb easily and keep the LED brightly illuminated for more than 10 min. In general, this work synthesized an integrated BatCap electrode Mn-Ni LDO-C; the integrated electrode exhibited high electrochemical performance, thus has a promising application prospect in the field of energy storage.
RESUMEN
Due to the diversity of sulfur valence in cobalt-based sulfides, it is difficult to control the crystal phase and composition of the products during synthesis. Herein, a one-pot hydrothermal method is reported to self-assemble the cobalt sulfides (CoS2, Co9S8and Co3S4) with hollow nanostructures. The whole preparation process is simple and mild, avoiding high temperature calcination. The performances of the three kinds of cobalt sulfide in superior supercapacitors and electrocatalytic oxygen evolution performance applications follow the order of CoS2 > Co9S8 > Co3S4. Further analysis demonstrates that the performance difference in these cobalt sulfides may be attributed to three factors: the presence ofS22-,the coordination environment of Co and the presence of continuous network of Co-Co bonds. The distinctive electrochemical performance of CoS2and Co9S8may help us to better understand the excellent electrochemical activity of metal polysulfides and metal sulfides after doping or alloying. Therefore, this work may provide a reference in understanding and designing the electrode materials for highly efficient applications in the fields of energy storage and conversion.
RESUMEN
The spin state of antibonding orbital (eg) occupancy in LaCoO3 is recognized as a descriptor for its oxygen electrocatalysis. However, the Co(III) cation in typical LaCoO3 (LCO) favors low spin state, which is mediocre for absorbing oxygen-containing groups involved in oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), thus hindering its further development in electrocatalysis. Herein, both experimental and theoretical results reveal the enhancement of bifunctional electrocatalytic activity in LaCoO3 by N doping. More specifically, electron energy loss spectroscopy and superconducting quantum interference devices magnetic analysis demonstrate that the Co(III) cation in N-doped LaCoO3 (LCON) achieves a moderate eg occupancy (≈1) compared with its low spin state in LaCO3. First-principle calculation results reveal that N dopants play a bifunctional role of tuning the spin-state transition of Co(III) cations and increasing the electrical conductivity of LCO. Thus, the optimized LCON exhibits an OER overpotential of 1.69 V at the current density of 50 mA/cm2 (1.94 V for pristine LCO) and yields an ORR limiting current density of 5.78 mA/cm2 (4.01 mA/cm2 for pristine LCO), which offers a new strategy to simultaneously modulate the magnetic and electronic structures of LCO to further enhance its electrocatalytic activity.
RESUMEN
Self-assembly of nanoscale building units into mesoscopically ordered superstructures opens the possibility for tailored applications. Nonetheless, the realization of precise controllability related specifically to the atomic scale has been challenging. Here, first, we explore the key role of a molecular surfactant in adjusting the growth kinetics of two-dimensional (2D) layered SnS2. Experimentally, we show that high pressure both enhances the adsorption energy of the surfactant sodium dodecylbenzene sulfonate (SDBS) on the SnS2(001) surface at the initial nucleation stage and induces the subsequent oriented attachment (OA) growth of 2D crystallites with monolayer thickness, leading to the formation of a monolayer amorphous carbon-bridged nanosheet mesocrystal. It is notable that such a nanosheet-coalesced mesocrystal is metastable with a flowerlike morphology and can be turned into a single crystal via crystallographic fusion. Subsequently, direct encapsulation of the mesocrystal via FeCl3-induced pyrrole monomer self-polymerization generates conformal polypyrrole (PPy) coating, and carbonization of the resulting nanocomposites generates Fe-N-S-co-doped carbons that are embedded with well-dispersed SnS/FeCl3 quantum sheets; this process skillfully integrated structural phase transformation, pyrolysis graphitization, and self-doping. Interestingly, such an integrated design not only guarantees the flowerlike morphology of the final nanohybrids but also, more importantly, allows the thickness of petalous carbon and the size of the nanoconfined particles to be controlled. Benefiting from the unique structural features, the resultant nanohybrids exhibited the brilliant electrochemical performance while simultaneously acting as a reliable platform for exploring the structure-performance correlation of a Li-ion battery (LIB).
RESUMEN
In this article, mechanical grinding, an effortless and super-effective synthetic strategy, is used to successfully synthesize a TiO2 quantum dot (TiO2QD)/graphitic carbon nitride (g-C3N4) heterostructure. X-ray photoelectron spectroscopy results together with transmission electron microscopy reveal the formation of the TiO2QD/g-C3N4 heterostructure with strong interfacial interaction. Because of the advantages of this characteristic, the prepared heterostructure exhibits excellent properties for photocatalytic wastewater treatment. Notably, the optimum photocatalytic activity of the TiO2QD/g-C3N4 heterostructure is nearly 3.4 times higher than that of the g-C3N4 nanosheets used for the photodegradation of rhodamine B pollutant. In addition, the stability and possible degradation mechanism of the TiO2QD/g-C3N4 heterojunction are studied in detail. This method may stimulate an effective approach to synthesizing QD-sensitized semiconductor materials and facilitate their application in environmental protection.