分类: 物理学 >> 交叉学科物理及相关领域的科学与技术 提交时间: 2018-03-30
摘要: Synthesis of low-cost, highly-active and durable non-platinum metal catalysts for methanol oxidation reaction (MOR) is always full of challenge. Here, Ni nanoparticles modified reduced graphene oxide (Ni/rGO) as an efficient non-platinum catalyst were synthesized by laser ablation of Ni target in graphene oxide (GO) solution and the following in situ reduction process. It found that GO played an important role to restrict the growth and aggregation of ultrafine nickel colloids (< 5 nm) in the process of laser ablation. The resulting Ni/rGO catalyst showed advantageous in active sites and charge transport resulting from the small particle size, uniform dispersion and electronic effect arising from the electron interactions between reduced graphene oxide (rGO) and Ni. The obtained Ni/rGO exhibited the ultrahigh catalytic mass activity of 1600 mA/mg, methanol saturation concentration (4 M), which was superior to that of the reported Ni-based catalysts. Remarkably the mass activities of Ni/rGO before and after 1000 cycles exceed that of the commercial Pt/C catalyst, indicating excellent catalytic activity and stability.
分类: 物理学 >> 交叉学科物理及相关领域的科学与技术 提交时间: 2018-03-30
摘要: Co-Ni layered double hydroxides (LDHs), as promising supercapacitor electrode materials with high specific capacity, have suffered poor rate property and cycle stability. By doping and topochemical oxidation of Ni ions is considered as efficivent rout to overcome these drawbacks. In this work, Ni3+ doped cobalt-nickel layered double hydroxides (Co-Ni-LDHs) were synthesized by pluse laser ablation of Ni taget in CoCl2 aqeous solution. The existence of Ni3+ ions doped in Co-Ni-LDHs decline the conductive resistance, and increase the mobility of surface charge and transfer rate of electrolyte. As a results, the Ni3+ doped Co-Ni-LDHs display a maximum specific capacitance of 2275 F/g and 1450 F/g at the current density of 1 A/g and 20 A/g, respectivly, indicating a high rate specific capacitance. Moreover, the capacitance retention is to be 80% after 1800 cycles at the current density of 6 A/g, manifesting good cycling stability of Ni3+ doped Co-Ni-LDHs.
分类: 物理学 >> 交叉学科物理及相关领域的科学与技术 提交时间: 2018-03-30
摘要: Agglomeration-triggered deactivation of supported platinum electrocatalysts markedly hinders their application in methanol oxidation reaction (MOR). In this study, graphene-supported nickel–iron layered double hydroxide (NiFe–LDH/rGO), in which Fe3+ was introduced to replace Ni2+ partially in the Ni(OH)2 lattice to provide stronger metal–support bonding sites, was utilized to immobilize Pt nanoparticles (NPs). Given the optimized metal–support interfacial contact (Fe3+–O(H)–Pt) between Pt NPs and NiFe–LDH/rGO nanosheets for Pt/NiFe–LDH/rGO electrocatalysts, the Pt/NiFe–LDH/rGO electrocatalysts displayed dramatically enhanced durability than that of Pt/Ni(OH)2/rGO counterpart as well as commercial Pt/C, and 86.5% of its initial catalytic activity can be maintained even after 1200 cycles of cyclic voltammetry (CV) tests during MOR. First-principle calculations toward the resultant M–O(H)–Pt (M = Fe3+, Ni2+) interfacial structure further corroborates that the NiFe–LDH nanosheets can provide stronger bonding sites (via the Fe3+–O(H)–Pt bonds) to immobilize Pt NPs than those of Ni(OH)2 nanosheets (via the Ni2+–O(H)–Pt bonds).
分类: 材料科学 >> 材料化学 提交时间: 2017-11-01
摘要: Doping additional ions into semiconductor is a potential strategy to modify the electronic structure of semiconductor materials. By using a highly reactive colloidal Cu clusters as doping precursor, we present here the successful doping of Cu ions into TiO2 nanocrystalline that simultaneously transformed from amorphous anodic TiO2 nanotubes during a dissolution and recrystallization process. The Cu-doped TiO2 nanoparticles (Cu-TNPs) film was characterized by X-ray diffraction, scanning and transmission electron microscopy and Raman spectroscopy. The Cu-TNPs show a rugby-like shape with exposed active {101}, {001} facets and the long-axis parallel to [001] lattice direction. The substitutional Cu2+ ions dopants in TiO2 nanocrystals caused the swelling of the crystalline unit cell. Such efficient doping design facilitate the improvement of nanostructured TiO2 as a potential biosensor for glucose molecules.
分类: 材料科学 >> 材料化学 提交时间: 2017-11-01
摘要: We report a simple and environment-friendly route to prepare platinum/reduced graphene oxide (Pt/rGO) nanocomposites (NCs) with highly reactive MnOx colloids as reducing agents and sacrificial templates. The colloids are obtained by laser ablation of a metallic Mn target in graphene oxide (GO)-containing solution. Structural and morphological investigations of the as-prepared NCs revealed that ultrafine Pt nanoparticles (NPs) with an average size of 1.8 (± 0.6) nm are uniformly dispersed on the surfaces of rGO nanosheets. Compared with commercial Pt/C catalysts, Pt/rGO NCs with highly electrochemically active surface areas show remarkably improved catalytic activity and durability toward methanol oxidation. All of these superior characteristics can be attributed to the small particle size and uniform distribution of the Pt NPs, as well as the excellent electrical conductivity and stability of the rGO catalyst support. These findings suggest that Pt/rGO electrocatalysts are promising candidate materials for practical use in fuel cells.
分类: 材料科学 >> 材料化学 提交时间: 2017-10-31
摘要: A general and straightforward strategy was developed for fabricating transition metal carbide (TMC)/carbon (C) core/shell nanospheres (NSs) by laser ablation of transition metals in acetone/ethanol liquid. Various TMC/C core/shell NSs such as TaC/C, NbC/C, HfC/C, and MoC/C core/shell NSs were successfully fabricated, highlighting the generality of this method. Crucially, this approach is green, facile, catalyst-free, and especially can be operated under ambient environments. Interestingly, all of the as-synthesized TMCs in the NS cores showed a cubic phase and structures similar to that of NaCl-type. The cores were further encapsulated by amorphous carbon shell with different thickness. As an example of the functional properties of these compound materials, the TaC/C core/shell NSs obtained were investigated as a supercapacitor electrode, which showed a large specific capacitance, excellent rate capability and remarkable cycling ability, revealing that the NSs could be used as new electrode materials for electrochemical energy storage. The photoluminescence of TaC/C core/shell NSs exhibited strong emission under the specific excitation wavelength at room temperature, showing potential biomedical applications due to the good biocompatibility of carbon shell. Besides, the basic physical and chemical reactions involved in the unique formation mechanism under highly nonequilibrium states induced by ultrafast laser ablation were discussed.