Nanoscale Research Letters
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2020
·Vol. 15
·期 1
·1-14
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IF 3.578
Guo Chaozhong,Li Yanrong,Li Zhaoxu,Liu Yao,Si Yujun,Luo Zhongli
Designing appropriate methods to effectively enhance nitrogen-doping efficiency and active-site density is essential to boost the oxygen reduction reaction (ORR) activity of non-platinum Fe/N/C-type electrocatalysts. Here, we propose a facile and effective strategy to design a mesopore-structured Fe/N/C catalyst for the ORR with ultrahigh BET surface area and outstanding conductivity via nanochannels of molecular sieve-confined pyrolysis of Fe 2+ ions coordinated with 2,4,6-tri(2-pyridyl)-1,3,5-triazine complexes as a novel precursor with the stable coordination effect. Combining the nanochannel-confined effect with the stable coordination effect can synergistically improve the thermal stability and stabilize the nitrogen-enriched active sites, and help to control the loss of active N atoms during pyrolysis process and to further obtain a high active-site density for enhancing the ORR activity. The as-prepared Fe/N/C electrocatalyst has exhibited excellent catalytic activity with an onset potential of ~ 0.841 V (versus RHE) closely approaching the Pt/C catalyst and high long-term stability in alkaline electrolyte. Besides, low-hydrogen peroxide yield (< 6.5%) and high electron transfer number (3.88–3.94) can be found on this catalyst, indicating that it is a valuable substitute for traditional Pt/C catalysts. This work paves a new way to design high-performance Fe/N/C electrocatalysts and deepens the understanding of active site and ORR catalysis mechanism.
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ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Guangfu Qian,Jinli Chen,Lin Luo,Hao Zhang,Wei Chen,Zhejiang Gao,Shibin Yin,Panagiotis Tsiakaras
Developing high performance bifunctional transition metal catalysts would be significantly beneficial for electrocatalytic oxidation of urea-rich wastewater. Herein, we synthesize a V2O3 nanosheet anchored N-doped-carbon encapsulated Ni heterostructure (Ni@C–V2O3/NF) for the reactions of urea oxidation (UOR) and hydrogen evolution (HER). Electrochemical results indicate that it exhibits small potentials of 1.32, 1.39, and 1.43 V for UOR and low overpotentials of 36, 254, and 355 mV for HER at ±10, ± 500 and ±1000 mA cm–2, respectively. It can work at 100 mA cm–2 for over 72 h as cathode and anode electrode without obvious attenuation, suggesting an outstanding durability. The reason for this behavior could be ascribed to the N-doped-carbon coating structure, the synergetic effects between Ni and V2O3, and the nano/micro nanosheets architecture self-supported on nickel foam. This work could provide a promising, inexpensive, and green method for the degradation of urea-rich wastewater and hydrogen production.
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JOURNAL OF MATERIALS SCIENCE
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2020
·Vol. 55
·期 31
·15140-15151
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IF 3.553
Lian Jiqiong,Wu Yihui,Sun Jingjing
Developing highly efficient and inexpensive bifunctional electrocatalysts is a grand challenge in water splitting process. In this article, NiFe electrocatalysts on nickel foam are prepared by electrodeposition method using high current density. The optimized NiFe electrocatalyst presented excellent electrocatalytic activities in 1.0 M KOH medium with low overpotentials of 100 mV for hydrogen evolution reaction and 230 mV for oxygen evolution reaction to achieve 10 mA·cm −2 , respectively. Moreover, the optimized NiFe electrocatalyst as bifunctional electrocatalyst toward overall water splitting only needs a small cell voltage of 1.57 V to obtain 10 mA·cm −2 . The extremely electrocatalytic performance of NiFe electrocatalyst is attributed to the fast charge transfer kinetics, large electrochemical surface area, and the conductive nickel foam.
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NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 35
·14970-14978
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IF 3.288
Jingchuang Zhao,Yingzhen Zhang,Xianyu Kang,Yancai Li
Direct methanol fuel cells (DMFCs) have been extensively studied for developing a new non-precious metal catalyst to replace commercial platinum catalysts, due to their expensive cost and susceptibility to CO poisoning. In this work, nanocomposites of nickel oxide/nickel supported by N-doped carbon (NiO/Ni–N/C) were prepared by using a hydrothermal method and further carbonization at different temperatures. The surface morphology and composition of the NiO/Ni–N/C nanocomposites were characterized by using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). As observed through electrochemical experiments, the NiO/Ni–N/C nanocomposite modified glassy carbon electrode (NiO/Ni–N/C/GCE) exhibits high electrocatalytic activity for the methanol oxidation reaction (MOR) in alkaline solution. Among the nanocomposites, NiO/Ni–N/C carbonized at 500 °C (NiO/Ni–N/C500) displays the highest mass activity (1043 mA mgNi−1) at 0.73 V (vs. Ag/AgCl), which is much higher than that of Ni(OH)2/N–C and NiO/Ni–N/C carbonized at other temperatures (400, 600, and 700 °C). In addition, the catalytic activity of NiO/Ni–N/C500 is 2.12 times that of the commercial Pt/C. NiO/Ni–N/C500/GCE also possesses fast kinetics, excellent stability and CO tolerance. Therefore, the NiO/Ni–N/C500 nanocomposites have great application potential as MOR catalysts.
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Tungsten
·
2020
·Vol. 2
·期 2
·194-202
·
IF 0
Yu Xue-Ping,Yang Chan,Song Pin,Peng Juan
Ultra-small MoS 2 quantum dots (QDs) with an average size of 2.48 nm coated on Au nanoparticles with a core-satellite structure (Au/MoS 2 QDs) are successfully prepared by a self-assembly strategy through the strong bonding between Au and S. Benefited from the unique structure, the Au/MoS 2 QDs hybrid exhibits outstanding electrocatalytic performance toward hydrogen evolution reaction (HER). The Au/MoS 2 QDs hybrid needs overpotentials of 112, 146, and 206 mV to approach current densities of 10, 20, and 50 mA·cm −2 in 0.5 mol·L −1 H 2 SO 4 (pH = 0.3), respectively. And a low Tafel slope (83 mV·dec −1 ) is obtained. The catalyst also displays satisfactory stability and durability, indicating a negligible current density loss after 20 h of electrolysis. The high hydrogen generation activities and stability are attributed to the great number of active sites, high conductivity and synergistic effects between gold nanoparticles (Au NPs) and MoS 2 QDs. Last but not least, this strategy opens up a favorable way to combine MoS 2 QDs with other metals.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Shaoqi Yang,Guangming Cai,Xingmei Lu,Chenguang Wang,Mi Feng,Junli Xu,Qing Zhou,Jiayu Xin,Longlong Ma
Hydrodeoxygenation (HDO) of lignin-derived phenols and dimeric ethers to biofuels has great significance for advanced utilization of renewable lignocelluloses and the future biobased economy. Herein, we find that the deoxygenation process during the lignin-derived model compound HDO process could efficiently be catalyzed by low-cost protic ionic liquids under mild conditions. 2-Hydroxy-N-(2-hydroxyethyl)-N-methylethanaminium trifluoromethanesulfonate ([BHEM]CF3SO3) shows the highest catalytic activity for the deoxygenation reaction during the lignin-derived compound HDO process with Rh/C as the hydrogenation catalyst. The conversion of phenol is 100% under 4 MPa H2 at 130 °C for 6 h, and the yield of cyclohexane is 93.3%. Furthermore, the catalytic system with [BHEM]CF3SO3 as the deoxygenation catalyst and Rh/C as the hydrogenation catalyst demonstrates efficient catalytic activity for various lignin-derived phenols and dimeric ethers with ≥99.0% conversion and >90.0% selectivity. The catalytic system is reused five times for HDO of phenol to test its stability.
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LANGMUIR
·
2020
·
IF 3.557
Guohong Ren,Xichen Zhang,Zhicheng Zhang,Ying Liang,Shishan Wu,Jian Shen
Pt-based nanomaterials have been proven to be effective catalysts for direct alcohol fuel cells (DAFCs). Specifically, the ternary nanoalloys (NAs) composed of Pt with other noble metals and transition metals can not only reduce the component of Pt but also enhance the electrocatalytic property and durability for alcohol oxidation. Herein, ternary PdPtCu NAs were synthesized through the solvothermal method using ethylene glycol as the solvent and reducing agent. The morphology and composition of PdPtCu NAs can be effectively controlled via selecting suitable surfactants and adjusting the proportion of precursors. The three-dimensional (3D) PdPtCu NAs with spiny rambutan-like morphology were obtained using the triblock copolymer Pluronic F-127 (PF-127) as the surfactant and adding three precursors with an equal molar ratio. The unique structure of PdPtCu NAs and the synergistic effect between the components significantly improved the electrocatalytic activity toward ethanol oxidation. Compared with different atomic ratio binary or ternary nanomaterials, 3D PdPtCu NAs manifested the best electrocatalytic performance.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Zonghua Pu,Tingting Liu,Weiyue Zhao,Xiudong Shi,Yanchen Liu,Gaixia Zhang,Weihua Hu,Shuhui Sun,Shijun Liao
Highly active catalyst for the hydrogen oxidation/evolution reactions (HOR and HER) plays an essential role for the water-to-hydrogen reversible conversion. Currently, increasing attention has been concentrated on developing low-cost, high-activity, and long-life catalytic materials, especially for acid media due to the promise of proton exchange membrane (PEM)-based electrolyzers and polymer electrolyte fuel cells. Although non-precious-metal phosphide (NPMP) catalysts have been widely researched, their electrocatalytic activity toward HER is still not satisfactory compared to that of Pt catalysts. Herein, a series of precious-metal phosphides (PMPs) supported on graphene (rGO), including IrP2-rGO, Rh2P-rGO, RuP-rGO, and Pd3P-rGO, are prepared by a simple, facile, eco-friendly, and scalable approach. As an example, the resultant IrP2-rGO displays better HER electrocatalytic performance and longer durability than the benchmark materials of commercial Pt/C under acidic, neutral, and basic electrolytes. To attain a current density of 10 mA cm–2, IrP2-rGO shows overpotentials of 8, 51, and 13 mV in 0.5 M dilute sulfuric acid, 1.0 M phosphate-buffered saline (PBS), and 1.0 M potassium hydroxide solutions, respectively. Additionally, IrP2-rGO also exhibits exceptional HOR performance in the 0.1 M HClO4 medium. Therefore, this work offers a vital addition to the development of a number of PMPs with excellent activity toward HOR and HER.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
·
IF 3.807
Jianpeng Li,Xianfeng Li,Hongyan Chen,Dingshu Xiao,Jiajia Li,Dekang Xu
In this paper, we present a facile and one-step way for synthesizing Fe, N dual doped highly porous graphitic biomass carbon (FeNC) by using K 2 FeO 4 to fulfill the activated process and catalytic graphitization of straws. The FeNC demonstrates hierarchically porous structure with large surface area of 1034 m 2 g −1 , Fe, N dual doping with certain amount of Fe-N x , and graphitic structure. With these favorable features, the electrocatalytic activity for oxygen reduction reaction (ORR) reveals that the FeNC exhibits positively onset potential with highly comparable limiting current density when comparing with the sample using conventional KOH activated agent. In additional, the assembled Zn-air battery using FeNC as air-cathode catalyst delivers a maximal power density of 128.4 mW cm −2 . Considering the abundance of straws on the earth and the low-cost and green prepared process, the present FeNC materials are highly promising in application in ORR catalysts for Zn-air battery and other energy-related fields.
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JOURNAL OF CATALYSIS
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2020
·
IF 7.888
Lei Lei,Danlian Huang,Chen Zhang,Rui Deng,Sha Chen,Zhihao Li
As a member of the transition metal sulfide family, cobalt sulfides (CoS x ) are considered as highly-activity, cost-effectively, as well as stable electrocatalysts with huge potential for the application of water splitting. Combining experiments and theoretical calculations, we demonstrated that F dopants could activate the Co and S sites of CoS 2 in CoS 2 @NF composites prepared via one-step hydrothermal method and contribute to enhance the intrinsic electrical conductivity, achieving a significantly improved activity of water splitting. The improved surface wettability in F-doped CoS 2 @NF composites ensures rapid electrolyte penetration and accelerates migration of hydroxyl as well as oxygen release. Furthermore, the F-doped CoS 2 @NF composites exhibit remarkable electrocatalytic activity and excellent long-term operational stability for overall water splitting in alkaline and neutral media. Predominantly, our work could be explored to enhance and understand the catalytic properties of other transition metal sulfides, and be also expected for further progress achieved with other nonmetal element dopants.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Ying Gao,Hanwei He,Wenyu Tan,Yizhi Peng,Xiaomei Dai,Yihui Wu
Exploring efficient, abundant, low-cost and stable materials for hydrogen evolution reaction (HER) is highly desired but still a challenging task. Herein, Ni–Se–Mo electrocatalysts supported on nickel foam (NF) substrate were synthesized by a facile one-step electrodeposition method. The Ni–Se–Mo film presents high electrocatalytic activity and stability toward HER, with a low overpotential of 101 mV to afford a current density of 10 mA cm −2 in 1.0 M KOH medium. Such excellent HER performance of Ni–Se–Mo film induced by the synergistic effects from Mo-doped Ni–Se film leads to the fast electron transfer . This work provides the validity of interface engineering strategy in preparing highly efficient transition metal chalcogenides based HER electrocatalysts.
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Journal of Energy Chemistry
·
2020
·
IF 7.216
Yuzhi Li,Siwei Li,Jing Hu,Yuanyuan Zhang,Yuchen Du,Xijiang Han,Xi Liu,Ping Xu
Designing readily available and highly active electrocatalysts for water splitting is essential for renewable energy technologies. Here we present the construction of FeCo-FeCoP@C hollow nanocubes encapsulated in nitrogen-doped carbon nanocages (FeCo-FeCoP@C@NCCs) through controlled carbonization and subsequent phosphorization of a Prussian blue analogue. With stronger electronic interaction and hollow structure, the as-obtained FeCo-FeCoP@C@NCCs material requires small overpotentials of 91 mV and 280 mV to deliver 10 mA cm −2 in 1 M KOH toward hydrogen and oxygen evolution, respectively. More importantly, applying this material for overall water splitting, it only requires 1.64 V to afford 10 mA cm −2 and exhibits impressively durability over 40 h without obvious performance decay. The present approach inspires potentials for the controllable synthesis of multi-component catalysts for practical applications.
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