Constructing heterostructured photocatalysts with highly exposed active sites proves to be an efficient strategy to improve the photocatalytic performance of bismuth-based photocatalysts. In this work, active site-exposed BiWO@BiOCl (BWO@BOC) heterostructure composites based on two bismuth-based materials were fabricated by an growth method for improving the photocatalytic hydrogenation of 4-aniline (4-NA) to -phenylenediamine (PPD). BWO@BOC exhibited enhanced photoactivity for 4-NA hydrogenation compared to pure BWO and BOC.
View Article and Find Full Text PDFSelective CO-to-CO photoreduction is under intensive research and requires photocatalysts with tuned microstructures to accelerate the reaction kinetics. Here, we report CuInS nanosheet arrays with sulfur vacancies (V) grown on the two-dimensional (2D) support of TiCT MXene for CO-to-CO photoreduction. Our results reveal that the use of TiCT induces strong support effect, which causes the hierarchical nanosheet arrays growth of CuInS and simultaneously leads to charge transfer from CuInS to TiCT support, resulting in V formed in CuInS.
View Article and Find Full Text PDFThe application of scattered light via an antenna-reactor configuration is promising for converting thermocatalysts into photocatalysts. However, the efficiency of dielectric antennas in photon-to-chemical conversion remains suboptimal. Herein, we present an effective approach to promote light utilization efficiency by designing dielectric antenna-hybrid bilayered reactors.
View Article and Find Full Text PDFAs vitally prospective candidates for next-generation energy storage systems, room-temperature sodium-sulfur (RT-Na/S) batteries continue to face obstacles in practical implementation due to the severe shuttle effect of sodium polysulfides and sluggish S conversion kinetics. Herein, the study proposes a novel approach involving the design of a B, N co-doped carbon nanotube loaded with highly dispersed and electron-deficient cobalt (Co@BNC) as a highly conductive host for S, aiming to enhance adsorption and catalyze redox reactions. Crucially, the pivotal roles of the carbon substrate in prompting the electrocatalytic activity of Co are elucidated.
View Article and Find Full Text PDFRoom-temperature sodium-sulfur batteries are still hampered by severe shuttle effects and sluggish kinetics. Most of the sulfur hosts require high cost and complex synthesis process. Herein, a facile method is proposed to prepare a phosphorous doped porous carbon (CSBP) with abundant defect sites from camellia shell by oxidation pretreatment combined with HPOactivation.
View Article and Find Full Text PDFThe recycling of scattered light by metals has been emerging as a promising light-manipulation-capture strategy, but how to bring its potential into better play remains to be explored. Herein, we present that constructing dual metal/high-refractive-index dielectric interfaces within the SiO core@TiO shell-Pd satellite@TiO shell effectively strengthens both the scattering efficiency of the dielectric SiO support and electric field confinement. Consequently, the absorption of Pd toward near-field scattered light and the interfacial charge carrier separation are both enhanced.
View Article and Find Full Text PDFAssembling two-dimensional (2D) MXene nanosheets into monolithic three-dimensional (3D) structures is an efficient pathway to transfer the nanoscale properties to practical applications. Nevertheless, the majority of the preparation schemes described in the literature are carried out at relatively high temperatures, which inevitably leads to the notorious high-temperature oxidation issue of MXenes. Preparing MXene-based hydrogels at lower temperatures or even room temperature is of great research importance.
View Article and Find Full Text PDFEngineering the spatial separation and transfer of photogenerated charge carriers has been one of the most enduring research topics in the field of photocatalysis due to its crucial role in determining the performances of photocatalysts. Herein, as a proof-of-concept, TiCT MXene is coupled with a typical heterojunction of TiO@CdS through a co-assembly strategy to boost electron pumping towards improving the photocatalytic efficiency. In addition to the band alignment-mediated electron transfer in TiO@CdS-TiCT heterojunctions, the plasmon-induced electric field enhancement of TiCT is found to cooperate with the electron-reservoir role of TiCT to extract photoinduced electrons.
View Article and Find Full Text PDFLow-temperature assembly of MXene nanosheets into three-dimensional (3D) robust aerogels addresses the crucial stability concern of the nano-building blocks during the fabrication process, which is of key importance for transforming the fascinating properties at the nanoscale into the macroscopic scale for practical applications. Herein, suitable cross-linking agents (amino-propyltriethoxysilane, Mn, Fe, Zn, and Co) as interfacial mediators to engineer the interlayer interactions are reported to realize the graphene oxide (GO)-assisted assembly of TiCT MXene aerogel at room temperature. This elaborate aerogel construction not only suppresses the oxidation degradation of TiCT but also generates porous aerogels with a high TiCT content (87 wt%) and robustness, thereby guaranteeing the functional accessibility of TiCT nanosheets and operational reliability as integrated functional materials.
View Article and Find Full Text PDFElectrochemical sodium-ion storage has come out as a promising technology for energy storage, where the development of electrode material that affords high volumetric capacity and long-term cycling stability remains highly desired yet a challenge. Herein, Ti C T (MXene)-based films are prepared by using sulfur (S) as the mediator to modulate the surface chemistry and microstructure, generating S-doped mesoporous Ti C T films with high flexibility. The mesoporous architecture offers desirable surface accessibility without significantly sacrificing the high density of Ti C T film.
View Article and Find Full Text PDFHard carbon is the most attractive anode material for electrochemical sodium/potassium-ion storage. The preparation of hard carbon spheres directly from the broad sources of biomass is of great interest but barely reported. Herein, we developed a simple two-step hydrothermal method to construct porous carbon microspheres directly from the original waste biomass of camellia shells.
View Article and Find Full Text PDFThe development of high-performance anode materials for potassium-based energy storage devices with long-term cyclability requires combined innovations from rational material design to electrolyte optimization. A three-dimensional K -pre-intercalated Ti C T MXene with enlarged interlayer distance was constructed for efficient electrochemical potassium-ion storage. We found that the optimized solvation structure of the concentrated ether-based electrolyte leads to the formation of a thin and inorganic-rich solid electrolyte interphase (SEI) on the K -pre-intercalated Ti C T electrode, which is beneficial for interfacial stability and reaction kinetics.
View Article and Find Full Text PDFSolar-powered N reduction in aqueous solution is becoming a research hotspot for ammonia production. Schottky junctions at the metal/semiconductor interface have been effective to build up a one-way channel for the delivery of photogenerated electrons toward photoredox reactions. However, their applications for enhancing the aqueous phase reduction of N to ammonia have been bottlenecked by the difficulty of N activation and the competing H evolution reaction (HER) at the metal surface.
View Article and Find Full Text PDFThe rational design and synthesis of MoS-based electrocatalysts with desirable active sites for the hydrogen evolution reaction have been actively pursued. Herein, we demonstrate a microwave-assisted steam heating method for the rapid and efficient synthesis of lamellar MoS-based materials with favorable exposed active edge sites. Based on this new strategy, we have further separately introduced reduced graphene oxide (rGO) and carbon nanotubes (CNTs), two typical carbon allotropes widely used to boost the electrocatalytic activity of MoS, to comparatively assess the support interactions and their effects on the electrocatalytic activity of MoS.
View Article and Find Full Text PDFControllable conversion of biomass to value-added carbon materials is attractive towards a wide variety of potential applications. Herein, hydrothermal treatment and KOH activation are successively employed to treat the cheap and abundant camellia oleifera shell as a new carbon raw material. It is shown that this stepwise activation process allows the production of porous nitrogen-doped carbon with optimized surface chemistry and porous structure compared to the counterparts prepared by a single activation procedure.
View Article and Find Full Text PDFA comparatively facile and ecofriendly process has been developed to synthesize porous carbon materials from shells. Potassium carbonate solution (KCO) impregnation is introduced to modify the functional groups on the surface of shells, which may play a role in promoting the development of pore structure during carbonization treatment. Moreover, a small amount of naturally embedded nitrogen and sulfur in the shells can also bring about the formation of pores.
View Article and Find Full Text PDFThree-dimensional graphene (3DG) is promising for constructing monolithic photocatalysts for solar energy conversion. However, the structure-associated light-shielding effect and the intricate porous architecture of 3DG result in intrinsic limitations in light penetration and mass transfer over 3DG supported hybrids, which restricts their photocatalytic efficiency. Here, taking 3DG-organic hybrids as examples, we report a geometry regulation strategy to minimize such structural restrictions, which not only favors the interaction between light and the photoactive component, but also facilitates reactant adsorption over the 3DG-organic hybrids, thereby cooperatively boosting their photoactivity.
View Article and Find Full Text PDFAssembly of two-dimensional (2D) layered structures into three-dimensional (3D) macroscopic hydrogel has been an enduring attracting research theme. However, the anisotropic intersheet cross-linking to form TiCT MXene-based hydrogel remains intrinsically challenging because of the superior hydrophilic nature of 2D TiCT . Herein, TiCT MXene is ingeniously assembled into the 3D macroscopic hydrogel under mild conditions by a graphene oxide (GO)-assisted self-convergence process.
View Article and Find Full Text PDFUltrathin two-dimensional (2D) nanostructures have attracted increasing research interest for energy storage and conversion. However, tackling the key problem of lattice mismatch inducing the instability of ulreathin nanostructures during phase transformations is still a critical challenge. Herein, we describe a facile and scalable strategy for the growth of ultrathin nickel phosphide (Ni P) nanosheets (NSs) with exposed (001) facets.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2018
Two-dimensional (2D) heterostructured materials, combining the collective advantages of individual building blocks and synergistic properties, have spurred great interest as a new paradigm in materials science. The family of 2D transition-metal carbides and nitrides, MXenes, has emerged as an attractive platform to construct functional materials with enhanced performance for diverse applications. Here, we synthesized 2D MoS -on-MXene heterostructures through in situ sulfidation of Mo TiC T MXene.
View Article and Find Full Text PDF2D transition metal carbides and nitrides, named MXenes, are attracting increasing attentions and showing competitive performance in energy storage devices including electrochemical capacitors, lithium- and sodium-ion batteries, and lithium-sulfur batteries. However, similar to other 2D materials, MXene nanosheets are inclined to stack together, limiting the device performance. In order to fully utilize MXenes' electrochemical energy storage capability, here, processing of 2D MXene flakes into hollow spheres and 3D architectures via a template method is reported.
View Article and Find Full Text PDFThree-dimensional metal carbide MXene/reduced graphene oxide hybrid nanosheets are prepared and applied as a cathode host material for lithium-sulfur batteries. The composite cathodes are obtained through a facile and effective two-step liquid-phase impregnation method. Owing to the unique 3 D layer structure and functional 2 D surfaces of MXene and reduced graphene oxide nanosheets for effective trapping of sulfur and lithium polysulfides, the MXene/reduced graphene oxide/sulfur composite cathodes deliver a high initial capacity of 1144.
View Article and Find Full Text PDFAs a new family member of room-temperature aprotic metal-O batteries, Na-O batteries, are attracting growing attention because of their relatively high theoretical specific energy and particularly their uncompromised round-trip efficiency. Here, a hierarchical porous carbon sphere (PCS) electrode that has outstanding properties to realize Na-O batteries with excellent electrochemical performances is reported. The controlled porosity of the PCS electrode, with macropores formed between PCSs and nanopores inside each PCS, enables effective formation/decomposition of NaO by facilitating the electrolyte impregnation and oxygen diffusion to the inner part of the oxygen electrode.
View Article and Find Full Text PDFRechargeable batteries, such as lithium-ion and sodium-ion batteries, have been considered as promising energy conversion and storage devices with applications ranging from small portable electronics, medium-sized power sources for electromobility, to large-scale grid energy storage systems. Wide implementations of these rechargeable batteries require the development of electrode materials that can provide higher storage capacities than current commercial battery systems. Within this greater context, this review will present recent progresses in the development of the 2D material as anode materials for battery applications represented by studies conducted on graphene, molybdenum disulfide, and MXenes.
View Article and Find Full Text PDFSodium-ion batteries (NIBs) are an emerging technology, which can meet increasing demands for large-scale energy storage. One of the most promising cathode material candidates for sodium-ion batteries is Na V (PO ) due to its high capacity, thermal stability, and sodium (Na) Superionic Conductor 3D (NASICON)-type framework. In this work, the authors have significantly improved electrochemical performance and cycling stability of Na V (PO ) by introducing a 3D interconnected conductive network in the form of carbon fiber derived from ordinary paper towel.
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