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1. chinaXiv:201803.01543 [pdf]

Ultrafine nickel nanoparticles modified reduced graphene oxide as efficient non-platinum catalysts for methanol oxidation

Hongmei Sun; Jun Liu; Zhenfei Tian; Yixing Ye; Changhao Liang
Subjects: Physics >> Interdisciplinary Physics and Related Areas of Science and Technology

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.

submitted time 2018-03-30 Hits2575Downloads1282 Comment 0

2. chinaXiv:201803.01544 [pdf]

Ni3+ doped cobalt-??nickel layered double hydroxides as high performance electrode material for supercapacitors

Hongmei Sun; Yixing Ye; Zhenfei Tian; Shouliang Wu; Jun Liu
Subjects: Physics >> Interdisciplinary Physics and Related Areas of Science and Technology

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.

submitted time 2018-03-30 Hits2488Downloads1204 Comment 0

3. chinaXiv:201803.01545 [pdf]

Site-specifically Immobilize Pt Nanocrystals on NiFe Layered Double Hydroxide: Old Catalysts with Enhanced Stability Through strong Fe3+-O(H)-Pt Interfacial Contact

Yechuang Han; Pengfei Li; Jun Liu; Shouliang Wu ; Yixing Ye; Zhenfei Tian; Changhao Liang
Subjects: Physics >> Interdisciplinary Physics and Related Areas of Science and Technology

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).

submitted time 2018-03-30 Hits2485Downloads1167 Comment 0

4. chinaXiv:201711.00003 [pdf]

Highly-dispersed ultrafine Pt nanoparticles on reduced graphene oxide nanosheets In situ sacrificial template synthesis and superior electrocatalytic performance for methanol oxidation.pdf

Shouliang Wu; Jun Liu ; Zhenfei Tian; Yunyu Cai; Yixing Ye; Qinglin Yuan; Changhao Liang
Subjects: Materials Science >> Materials Chemistry

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.

submitted time 2017-11-01 Hits16181Downloads1522 Comment 0

5. chinaXiv:201711.00004 [pdf]

Co-doped Ni hydroxide and oxide nanosheet networks Laser-Assisted Synthesis Effective Doping, and Ultrahigh Pseudocapacitor Performance.pdf

Dewei Liang; Shouliang Wu; Jun Liu; Zhenfei Tian; Changhao Liang
Subjects: Materials Science >> Materials Chemistry

Morphology control and impurity doping are two widely applied strategies to improve the electrochemical performance of nanomaterials. Herein, we report an environmentally friendly approach to obtain Co-doped Ni(OH)2 nanosheet networks using a laser-induced cobalt colloid as a doping precursor followed by an aging treatment in a hybrid medium of nickel ions. The shape and specific surface area of the doped Ni(OH)2 can be successfully adjusted by changing the concentration of sodium thiosulfate. Furthermore, a Co-doped Ni(OH)2 nanosheet network was further converted into Co-doped NiO with its pristine morphology retained via facile thermal decomposition in air. The structure and electrochemical performance of the as-prepared samples are investigated with scanning and transmission electron microscopy, energy dispersive x-ray analysis, x-ray diffraction, Fourier transform infrared spectroscopy, the nitrogen adsorption-desorption isotherm technique, and electrochemical measurements. The Co-doped Ni(OH)2 electrode shows an ultrahigh specific capacitance of 1421 F/g at a current density of 6 A/g, and a good retention level of 76% after 1000 cycles, in sharp contrast with only a 47% retention level of the pure Ni(OH)2 electrode at the same current density. In addition, the Co-doped NiO electrode exhibits a capacitance of 720 F/g at 6 A/g and 92% retention after 1000 cycles, which is also superior to those values for relevant pure NiO electrodes. The Co2+ partially substitutes for Ni2+ in the metal hydroxide and oxide, resulting in an increase of free holes in the valence band, and, therefore, enhancement of the p-type conductivity of Ni(OH)2 and NiO. Moreover, such novel mesoporous nanosheet network structures are also able to enlarge the electrode-electrolyte contact area and shorten the path length for ion transport. The synergetic effect of these two results is responsible for the observed ultrahigh pseudocapacitor performance.

submitted time 2017-11-01 Hits16277Downloads1463 Comment 0

6. chinaXiv:201710.00079 [pdf]

A general strategy toward transition metal carbidecarbon coreshell nanospheres and their application for supercapacitor electrode.pdf

Hemin Zhang; Jun Liu; Zhenfei Tian; Yixing Ye; Yunyu Cai; Changhao Liang; Kazuya Terabe
Subjects: Materials Science >> Materials Chemistry

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.

submitted time 2017-10-31 Hits16377Downloads1523 Comment 0

7. chinaXiv:201710.00080 [pdf]

Recent Advances in Ligand-Free, Charged and Defect-Rich Catalysts Developed by Laser Ablation and Processing in Liquids.pdf

Dongshi Zhang; Jun Liu,; Pengfei Li; Zhenfei Tian; Changhao Liang
Subjects: Physics >> General Physics: Statistical and Quantum Mechanics, Quantum Information, etc.

Catalysts are the foundation of sustainable and renewable energies to address the depletion of natural fossil fuels problem. Because the catalysts’ activity is surface chemistry dependent, those “naked”, so-called ligand-free catalysts with more active sites exposing to the reactants are more preferable. With ligand-free, highly surface charged nanomaterials as the innate products, a newly emerging technique―laser synthesis and processing in liquids―is gaining increasing attention. The priority of laser-synthesized ligand-free metallic catalysts over chemically-synthesized counterparts has been confirmed by increasing groups through comparative studies on their catalytic activities. Besides the ligand-free metallic catalysts, this technique also excels at synthesis of bimetallic-alloy, core-shell and defect-rich semiconductor catalysts, and show good compatibility with other techniques (e.g., hydrothermal treatment and electrophoresis) to develop advanced catalysts such as ternary oxide, doped semiconductor, supported composite, nanoparticle-polymer matrix and film catalysts. Following the concept of why to choose, how to synthesize and where to use, in this review, we first introduce the advantages of this technique and the synthesized catalysts, secondly show how to develop complex catalysts using the laser-generated particles as the building blocks, and finally present the exciting application examples for photodegradation, water splitting and fuel cells.

submitted time 2017-10-31 Hits1418Downloads799 Comment 0

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