Journal of Materials Chemistry A
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2017
·Vol. 5
·期 34
·17982-17989
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IF 8.867
Xiang Wang,Feng Li,Wenzhu Li,Wenbing Gao,Yu Tang,Rong Li
The development of highly active, stable and affordable hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalysts for renewable energy reserve and conversion remains a serious challenge. In this study, a simple solvothermal strategy is adopted to synthesize hollow bimetallic cobalt-based selenide templated by cobalt-based bimetallic organic frameworks (BM-ZIFs) with superior water splitting activity and stability, owing to the perfect hollow polyhedral structure with numerous active sites. Moreover, the introduction of a transition metal element not only enhances the electroconductibility of the catalyst, but also further improves the electrocatalytic ability via the Jahn–Teller effect. Furthermore, the synthetic method is convenient and low toxic without high temperature carbonization process. The as-synthesized hollow MxCo1−xSe2 polyhedrons exhibit excellent electrocatalytic performances. Particularly, the Zn0.1Co0.9Se2 exhibits low overpotentials of −140 mV and 340 mV at a current density of 10 mA cm−2, a small Tafel slope of 49.9 mV dec−1 and 43.2 mV dec−1 as well as a high current density with robust catalytic stability for both HER in acidic and OER in basic solutions, respectively. This strategy provides a prospect for preparation of homogenously doped and self-templated hollow structure non-noble metal electrocatalysts with high HER and OER performance.
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高影响因子
LANGMUIR
·
2016
·
IF 3.993
Ting Lu,Jian Lin,Xin Liu,Xiaodong Wang,Tao Zhang
By a reverse microemulsion method, a series of IrFe bimetallic nanomaterials of variable morphologies and compositions is synthesized and characterized by 57Fe Mössbauer spectroscopy, XRD, XPS, and TEM. The structure evolution, such as IrFe alloy nanoparticles to Ir nanoparticles on Fe2O3 flakes, can be simply tuned by changing the molar ratio of Ir to Fe precursors. In terms of Fe, the relative content of IrFe alloy decreased with the increase of Fe species doped, while that of Fe2O3 flakes increased until reached 100%. The as-prepared IrFe bimetallic nanomaterials were served as catalysts for the selective hydrogenation of 3-nitrostyrene to 3-aminostyrene, and it is found that the catalytic performance was related to the morphology and composition of these nanomaterials. Ir1Fe4 was subsequently identified to be a highly active and exceedingly selective catalyst with good stability and recyclability for the hydrogenation of 3-nitrostyrene, underscoring a remarkable “synergistic effect” of the two metals appearing as the form of Ir nanoparticles loaded on Fe2O3 flakes. For Ir nanoparticles, they act as an active species for the hydrogenation; for Fe2O3 flakes, they favor the preferential adsorption of nitro groups, which account for the better chemoselectivity to objective product.
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高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2016
·Vol. 21
·期 5
·1287-1295
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IF 2.327
Chao Lei,Qin Yong,Liu Yang,Kong Yong,Chu Fuqiang
N-doped graphene has been extensively explored because of their intriguing properties. However, most of the conventional heat-processed N-doped graphene (HNG) suffer from the poor hydrophilic property and low electric conductivity when using electrode materials. Herein, we present a facile solution-processed strategy to fabricate N-doped graphene through electrochemical exfoliation of graphite in inorganic electrolyte solution. The resulting electrochemically exfoliated N-doped graphene (ENG) has high level of nitrogen (7.9 at.%) and oxygen (16.5 at.%), moreover, excellent electric conductivity (19 s cm −1 ). As a binder-free electrode material for oxygen reduction reaction (ORR), ENG exhibits much better electroactivity than HNG and electrochemically exfoliated graphene (EG), moreover, much better methanol tolerance and long-term durability than that commercial Pt/C catalyst. The results provide new sights into scalable production of noble metal-free catalyst towards ORR.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2017
·Vol. 164
·期 13
·F1483
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IF 3.259
Yingjie Chen,Shiben Liu,Zhihao Shi,Jianhua Yu,Hongzhou Dong,Yong Qin,Liyan Yu,Lifeng Dong
Ag-MFe2O4 (M = Co, Mn) nanocomposites were synthesized and loaded onto carbon supports. As-prepared Ag-MFe2O4/C demonstrated higher catalytic activity for oxygen reduction reaction (ORR) than Ag+MFe2O4/C. The direct coupling and electron transfer between Ag and MFe2O4 in nanocomposites were proposed to enhance their catalytic activities. The Koutecky-Levich plots confirmed a direct four-electron reaction pathway for the ORR on Ag-MFe2O4/C. Furthermore, Ag-MFe2O4/C showed superior catalytic activities and excellent stability for oxygen evolution reaction (OER). Thus, Ag-MFe2O4/C nanoparticle are potential non-Pt candidates with bi-functional catalytic activity for ORR and OER.
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JOURNAL OF MATERIALS SCIENCE
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2017
·Vol. 52
·期 13
·8016-8026
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IF 2.599
Yang Hongyu,Wen Chengwei,Tang Zhenghua,Wang Likai,Wang Qiannan,Yan Wei,Wu Wen,Chen Shaowei
Bio-inspired metal nanomaterials are receiving increasing research attentions in catalytic field recently, while peptide-based method represents new revenues to fabricate stable and reactive catalyst under mild and environmental friendly conditions. Among all kinds of noble metals, peptide-based palladium nanomaterials have demonstrated excellent catalytic capabilities in a variety of organic reactions. However, their electrocatalytic properties have not been systematically studied. Herein, R5-templated Pd nanomaterials have been fabricated and employed as potent catalysts for oxygen reduction reaction (ORR). The shape and morphology of these Pd nanomaterials were manipulated by tuning the metal-to-R5 ratio. The as-prepared Pd nanomaterials demonstrated excellent ORR activity in alkaline media. R5-Pd-90 exhibited the best activity which is superior than commercial Pt/C, in terms of onset potential, diffusion-limited current density as well as long-term stability. The correlation between the shape and/or morphology of the peptide-templated Pd nanomaterials and their ORR activity has been successfully established.
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ACS Catalysis
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2017
·
IF 10.614
Bo Song,Kai Li,Ying Yin,Tao Wu,Lianna Dang,Miguel Cabán-Acevedo,Jiecai Han,Tangling Gao,Xianjie Wang,Zhihua Zhang,J. R. Schmidt,Ping Xu,Song Jin
Highly efficient earth-abundant electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are of great importance for renewable energy conversion systems. Herein, guided by theoretical calculations, we demonstrate highly efficient water splitting in alkaline solution using quarternary mixed nickel iron phosphosulfide (Ni1–xFexPS3) nanosheets (NSs), even though neither NiPS3 nor FePS3 is a good HER (or OER) electrocatalyst. With tuned electronic structure and improved electrical conductivity induced by mixing appropriate amount of Fe into NiPS3, Ni0.9Fe0.1PS3 NSs display excellent HER activity (an overpotential of 72 mV vs reversible hydrogen electrode (RHE) at a geometric catalytic current density of −10 mA cm–2 and a Tafel slope of 73 mV dec–1), which is among the best HER catalysts under alkaline conditions. Ni0.9Fe0.1PS3 NSs also show a good apparent OER activity (an overpotential of 329 mV vs RHE at a catalytic current density of 20 mA cm–2 and a Tafel slope of 69 mV dec–1), although structural investigation indicates the formation of Ni(Fe)OOH and Ni(Fe)(OH)2 layers on the catalyst surface after OER reactions as likely the real active species. These mixed nickel iron phosphosulfide non-precious-metal electrocatalysts with enhanced intrinsic activity and long-term stability and durability should have great potential in overall water-splitting applications.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Chaozhong Guo,Rong Hu,Wenli Liao,Zhongbin Li,Lingtao Sun,Dongping Shi,Yanrong Li,Changguo Chen
Recycling and utilizing organic biowastes will effectively help to decrease the damage to the natural environment and synchronously facilitate the development of new carbon materials for energy applications. In this study, we directly convert protein-rich fish-scale biowaste to hierarchically porous three-dimentional (3D)-network nanocarbons via two-step pyrolysis process combined with ZnCl 2 activation and acidic-treatment. It is interestingly found that this material exhibits more excellent oxygen reduction electrocatalytic activity and stability compared to the commercial 20 wt% Pt/C catalyst in both alkaline and acidic solutions, which can be closely correlated to its chemical state of nitrogen atoms, BET surface area and inner porous structure. The addition of ZnCl 2 activator during pyrolysis process can help to produce the 3D network nanostructure and then to enhance the mesopore surface area, making for the improvement of oxygen reduction performance. More remarkably, the ORR onset potential on our material is about 60 mV higher than that on the Pt/C catalyst in alkaline electrolyte. In addition, we also propose that pyridinic- and graphitic-nitrogen species may be key factors to be responsible for the electrocatalytic activity. This study can encourage the exploration of high porosity nanocarbons from widely-existed biowastes, functioning as highly active and stable oxygen reduction electrocatalysts.
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JOURNAL OF POWER SOURCES
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2016
·
IF 6.333
Jiu-Ju Feng,Li-Li He,Rui Fang,Qiao-Li Wang,Junhua Yuan,Ai-Jun Wang
Superlattice arrays, an important type of nanomaterials , have wide applications in catalysis, optic/electronics and energy storage for the synergetic effects determined by both individual metals and collective interactions. Herein, a simple one-pot solvothermal coreduction approach is developed for facile preparation of bimetallic PtAu alloyed superlattice arrays (PtAu SLAs) in oleylamine, with the assistance of urea via hydrogen bonding induced self-assembly. Urea is essential in morphology-controlled process and prevents PtAu nanoparticles from the disordered aggregation. The characterization and formation mechanism of PtAu SLAs are investigated in details. The as-synthesized hybrid nanocrystals exhibit enhanced electrocatalytic performances for oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) in alkaline electrolyte in comparison with commercial Pt-C (50%, wt.%) and Pt black catalysts.
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RSC Advances
·
2016
·Vol. 6
·期 91
·88788-88796
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IF 3.289
Riyang Shu,Ying Xu,Longlong Ma,Qi Zhang,Tiejun Wang,Pengru Chen,Qingyun Wu
A novel hydrogenolysis process for lignosulfonate depolymerization was proposed using a noble metal catalyst cooperated with metal chloride in methanol. Hydrogenolysis performance was significantly affected by the catalysts, via a synergistic catalytic effect between the Lewis acid (metal chloride) and the noble metal. Reaction conditions were also optimized, with 8.6% aliphatic alcohols and 9.2% monomers obtained at 280 °C for 5 h over Pt/C cooperated with CrCl3. Analysis of the depolymerized products indicated that CrCl3 had a catalytic promoting effect on cleavage of β-O-4 bonds with the synergistic catalytic effect of Pt/C. Meanwhile, the noble metal catalysed saturation of the depolymerized products and suppressed them from condensing into residues. The sulfonic groups of lignosulfonate were cleaved and they did not cause Pt/C poisoning. The catalyst showed good recyclability, with no significant loss of catalytic activity after three runs.
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CARBON
·
2017
·
IF 6.337
Jingyan Liu,Yang Liu,Peng Li,Luhai Wang,Haoran Zhang,Hui Liu,Jialiang Liu,Yixian Wang,Wei Tian,Xiaobo Wang,Zhongtao Li,Mingbo Wu
Fe-N-doped porous carbon derived from petroleum asphalt (NPCA) was prepared via a facile template synthesis method, with urea as nitrogen source while α-Fe 2 O 3 nanoparticles as template and Fe source. The as-prepared NPCA calcined at 900 °C (NPCA-900) exhibits excellent electrocatalytic performance with high diffusion-limiting current density and stability comparable to those of commercial Pt/C catalysts in alkaline environment . The remarkable ORR performance of NPCA could be ascribed to the abundant porosity, large specific surface area (1060 m 2 g −1 ), as well as the doping of Fe-N (especially pyridinic N). The NPCA derived from cheap petroleum asphalt has good application future in the field of catalysis, while it may pave a new way to realize the clean and high value utilization of heavy oils.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2016
·Vol. 24
·期 1
·676-684
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IF 2.76
Tu Baosheng,Shi Nian,Sun Wei,Cao Limei,Yang Ji
In this paper, Pt supports on carbon black powder (Vulcan XC-72) were synthesized via a hydrothermal method for selective catalytic reduction (SCR) of NO with H 2 in the presence of 2 vol% O 2 over a wide temperature of 20–300 °C. The results showed that the 3 and 5 wt% Pt/C catalysts resulted in high NO conversion (>90 %) over a temperature range of 120 to 300 °C, and the maximum NO conversion of 98.6 % was achieved over 5 wt% Pt/C at 120 °C. Meanwhile, the influence of SO 2 and H 2 O on the catalyst performance of 3 wt% Pt/C was investigated. The catalysts exhibited good SO 2 poisoning resistance when the SO 2 concentration was lower than 260 ppm. Moreover, a positive effect on NO conversion was detected with the addition of 3 and 5 vol% H 2 O in the feed gas stream.
TEM image and good NO conversion performance of the Pt/C catalysts
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JOURNAL OF ALLOYS AND COMPOUNDS
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2016
·
IF 3.014
Zhiwei Zhang,Hanning Li,Jie Hu,Baozhong Liu,Qingrui Zhang,Carlos Fernandez,Qiuming Peng
A novel nitrogen-doped biomass carbon/silver (C-N/Ag) composite has been synthesized by a simple method, wherein the precursor of soymilk simultaneously serves as carbon and nitrogen sources, reductant and substrate. The structure, morphology and valence state of samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectra. Results show the formation of nano-sized Ag homogenously disperses on the surface of mesoporous substrate, and the self-reduction role mainly attributes to the presence of unsaturated carbon bonding. Electrochemical properties were characterized by galvanostatic discharge and impedance spectra techniques. The sample prepared with 1 mmol AgNO 3 solution, activated by 0.1 M KOH and annealed at 900 °C shows excellent oxygen reduction reaction activity and good electrochemical durability in alkaline medium. The onset potential, limiting diffusion current density and electron transfer number are 0.93 V, 6.26 mA cm −2 and 4.00, respectively, superior to those of 60 wt.% Ag/C and comparable to 20 wt.% Pt/C catalysts correspondingly. The discharge performance of Zn-air batteries is better than that of 20 wt% Pt/C.
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