A facile and scalable in situ synthesis strategy is developed to fabricate carbon-encapsulated Fe3O4 nanoparticles homogeneously embedded in two-dimensional (2D) porous graphitic carbon nanosheets (Fe3O4@C@PGC nanosheets) as a durable high-rate lithium ion battery anode material. With assistance of the surface of NaCl particles, 2D Fe@C@PGC nanosheets can be in situ synthesized by using the Fe(NO3)3·9H2O and C6H12O6 as the metal and carbon precursor, respectively. After annealing under air, the Fe@C@PGC nanosheets can be converted to Fe3O4@C@PGC nanosheets, in which Fe3O4 nanoparticles (∼18.2 nm) coated with conformal and thin onion-like carbon shells are homogeneously embedded in 2D high-conducting carbon nanosheets with a thickness of less than 30 nm. In the constructed architecture, the thin carbon shells can avoid the direct exposure of encapsulated Fe3O4 to the electrolyte and preserve the structural and interfacial stabilization of Fe3O4 nanoparticles. Meanwhile, the flexible and conductive PGC nanosheets can accommodate the mechanical stress induced by the volume change of embedded Fe3O4@C nanoparticles as well as inhibit the aggregation of Fe3O4 nanoparticles and thus maintain the structural and electrical integrity of the Fe3O4@C@PGC electrode during the lithiation/delithiation processes. As a result, this Fe3O4@C@PGC electrode exhibits superhigh rate capability (858, 587, and 311 mAh/g at 5, 10, and 20 C, respectively, 1 C = 1 A/g) and extremely excellent cycling performance at high rates (only 3.47% capacity loss after 350 cycles at a high rate of 10 C), which is the best one ever reported for an Fe3O4-based electrode including various nanostructured Fe3O4 anode materials, composite electrodes, etc.
A facile and scalable in situ chemical vapor deposition (CVD) technique using metal precursors as a catalyst and a three-dimensional (3D) self-assembly of NaCl particles as a template is developed for one-step fabrication of 3D porous graphene networks anchored with Sn nanoparticles (5-30 nm) encapsulated with graphene shells of about 1 nm (Sn@G-PGNWs) as a superior lithium ion battery anode. In the constructed architecture, the CVD-synthesized graphene shells with excellent elasticity can effectively not only avoid the direct exposure of encapsulated Sn to the electrolyte and preserve the structural and interfacial stabilization of Sn nanoparticles but also suppress the aggregation of Sn nanoparticles and buffer the volume expansion, while the interconnected 3D porous graphene networks with high electrical conductivity, large surface area, and high mechanical flexibility tightly pin the core-shell structure of Sn@G and thus lead to remarkably enhanced electrical conductivity and structural integrity of the overall electrode. As a consequence, this 3D hybrid anode exhibits very high rate performance (1022 mAh/g at 0.2 C, 865 mAh/g at 0.5 C, 780 mAh/g at 1 C, 652 mAh/g at 2 C, 459 mAh/g at 5 C, and 270 mAh/g at 10 C, 1 C = 1 A/g) and extremely long cycling stability even at high rates (a high capacity of 682 mAh/g is achieved at 2 A/g and is maintained approximately 96.3% after 1000 cycles). As far as we know, this is the best rate capacity and longest cycle life ever reported for a Sn-based lithium ion battery anode.
A facile and scalable 2D spatial confinement strategy is developed for in situ synthesizing highly crystalline MoS2 nanosheets with few layers (≤5 layers) anchored on 3D porous carbon nanosheet networks (3D FL-MoS2@PCNNs) as lithium-ion battery anode. During the synthesis, 3D self-assembly of cubic NaCl particles is adopted to not only serve as a template to direct the growth of 3D porous carbon nanosheet networks, but also create a 2D-confined space to achieve the construction of few-layer MoS2 nanosheets robustly lain on the surface of carbon nanosheet walls. In the resulting 3D architecture, the intimate contact between the surfaces of MoS2 and carbon nanosheets can effectively avoid the aggregation and restacking of MoS2 as well as remarkably enhance the structural integrity of the electrode, while the conductive matrix of 3D porous carbon nanosheet networks can ensure fast transport of both electrons and ions in the whole electrode. As a result, this unique 3D architecture manifests an outstanding long-life cycling capability at high rates, namely, a specific capacity as large as 709 mAh g(-1) is delivered at 2 A g(-1) and maintains ∼95.2% even after 520 deep charge/discharge cycles. Apart from promising lithium-ion battery anode, this 3D FL-MoS2@PCNN composite also has immense potential for applications in other areas such as supercapacitor, catalysis, and sensors.
This review provides enriched information for understanding the charge storage mechanisms of transition metal dichalcogenides (TMDs), as well as the importance of intrinsic structure engineering for enhancing the performance of TMDs in energy storage.
A general ultrathin-nanosheet-induced strategy for producing a 3D mesoporous network of Co 3 O 4 is reported. The fabrication process introduces a 3D N-doped carbon network to adsorb metal cobalt ions via dipping process. Then, this carbon matrix serves as the sacrificed template, whose N-doping effect and ultrathin nanosheet features play critical roles for controlling the formation of Co 3 O 4 networks. The obtained material exhibits a 3D interconnected architecture with large specific surface area and abundant mesopores, which is constructed by nanoparticles. Merited by the optimized structure in three length scales of nano particles-mesopores-networks, this Co 3 O 4 nanostructure possesses superior performance as a LIB anode: high capacity (1033 mAh g −1 at 0.1 A g −1 ) and long-life stability (700 cycles at 5 A g −1 ). Moreover, this strategy is verified to be effective for producing other transition metal oxides, including
Reversible protonic ceramic electrochemical cells (R-PCECs) are a promising option for efficient and low-cost generation of electricity and hydrogen. Commercialization of R-PCECs, however, hinges on the development of highly active and robust air electrodes. Here, we report an air electrode consisting of PrBa 0.8 Ca 0.2 Co 2 O 5+δ and in situ exsolved BaCoO 3−δ nanoparticles (PBCC−BCO) that shows minimal polarization resistance (∼0.24 Ω cm 2 at 600 °C) and high stability when exposed to humidified air with 3−50% H 2 O. An R-PCEC utilizing PBCC-BCO demonstrates remarkable performances at 600 °C: achieving a peak power density of 1.06 W cm −2 in the fuel cell mode and a current density of 1.51 A cm −2 at 1.3 V in an electrolysis mode. More importantly, the R-PCECs demonstrate an exceptionally high durability over 1833 h of continuous operation in the electrolysis mode. This work offers an efficient approach to design of high-performance and durable electrodes for R-PCECs.
Although they are widely used as cocatalysts in promoting photocatalysis, practical application of noble metals is limited by their high cost and rarity. Development of noble-metal-free cocatalysts is thus highly demanded. Herein titanium carbide (Ti C ) MXene is shown to be a highly efficient noble-metal-free cocatalyst with commercial titania (P25) for photocatalytic CO reduction. Surface alkalinization of Ti C dramatically enhances the activity; the evolution rates of CO (11.74 μmol g h ) and CH (16.61 μmol g h ) are 3- and 277-times higher than those of bare P25, respectively. The significantly enhanced activity is attributed to the superior electrical conductivity and charge-carrier separation ability, as well as the abundant CO adsorption and activation sites of surface-alkalinized Ti C MXene, indicating its promise as a highly-active noble-metal-free cocatalysts for photocatalytic CO reduction.
Reduced graphene oxide-azobenzene (RGO-AZO) hybrids were prepared via covalent functionalization for long-term solar thermal storage. Thermal barrier (ΔEa) of cis to tran reversion and thermal storage (ΔH) were improved by molecular hydrogen bonds (H-bonds) through ortho- or para-substitution of AZO. Intramolecular H-bonds thermally stabilized cis-ortho-AZO on RGO with a long-term half-life of 5400 h (ΔEa = 1.2 eV), which was much longer than that of RGO-para-AZO (116 h). RGO-para-AZO with one intermolecular H-bond showed a high density of thermal storage up to 269.8 kJ kg−1 compared with RGO-ortho-AZO (149.6 kJ kg−1) with multiple intra- and intermolecular H-bonds of AZO according to relaxed stable structures. Thermal storage in experiment was the same order magnitude to theoretical data based on ΔH calculated by density functional theory and packing density. Photoactive RGO-AZO hybrid can be developed for high-performance solar thermal storage by optimizing molecular H-bonds.
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