Nanoscale
·
2018
·Vol. 10
·期 32
·15238-15248
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IF 7.233
Qijun Che,Ningning Bai,Qing Li,Xinhong Chen,Ya Tan,Xi Xu
An enormous challenge in the development of renewable hydrogen sources for electricity-driven water-splitting systems has been the limitation of the earth-abundant and robust highly-active cathode electrocatalysts. In this work, we developed a simple sulfur-anion doping strategy to obtain the S-doped NiCo composite (S-NiCo@50) on Ni foam (NF) via a one-step electrochemical deposition. It was found that doped sulfur plays a crucial role in reducing the overpotential of hydrogen evolution by providing abundant active sites as identified by the XPS spectrum. The formed metallic Ni and Co effectively promoted electron transportation. The synergistic effects between the amorphous CoxNiyS(x+y) substance and crystalline Ni and Co metal seemed to result in enhanced HER activity. In particular, the S-NiCo@50 electrode, featuring a hierarchical morphology, showed an ultralow overpotential of 28 and 125 mV at 10 and 100 mA cm−2, respectively, in 1.0 M NaOH with a large exchange current density (j0) of 4.8 mA cm−2 as well as high conductivity and stability; its catalytic properties are superior to most of the reported alkaline electrocatalysts and are on par with commercial Pt/C. Assembled with the counter electrode (Ni–Fe/NF), the overall water splitting was proved with a low 1.55 V at 10 mA cm−2. Moreover, we built the Ni24Co6S6 cluster as the S-NiCo@50 model and revealed its intrinsic activity by density functional theory (DFT) calculations. This study shows that S-doping and component control can be an exquisite strategy for realizing high-efficiency electrochemical water reduction.
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高影响因子
JOURNAL OF NANOPARTICLE RESEARCH
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2018
·Vol. 20
·期 11
·1-10
·
IF 2.127
Duan Wanyi,Li Aoqi,Chen Yujuan,Zhuo Kelei,Liu Jianming,Wang Jianji
In this work, a facile one-pot solvothermal method is developed for fabricating hollow spherical PtCu alloy nanoparticles (with the size of 124 ± 16 nm) supported on reduced graphene oxide (PtCu/rGO), with the assistance of 1-decyl-3-methylimidazolium bromide ([C 10 MIm]Br) as the structure-directing agent and capping agent. The influence of various experimental parameters on the morphology and structure of prepared PtCu/rGO hybrids is researched. Compared with the commercial Pt/C (10 wt%) and Pt/rGO, the as-prepared PtCu/rGO hybrid exhibits a larger electrochemical active surface area, higher electrocatalytic activity, and better tolerance for methanol oxidation in acidic media. We believe that the hollow spherical PtCu alloy supported on rGO will have great potential applications for direct methanol fuel cells.
Hollow spherical PtCu alloy supported on rGO hybrid is successfully synthesized by a facile one-pot solvothermal method with the assistance of 1-decyl-3-methylimidazolium bromide. 1-Decyl-3-methylimidazolium bromide acts as both shape-controlled agent and capping agent for synthesizing PtCu/rGO. The as-prepared PtCu/rGO exhibits high electrocatalytic activity and good poisoning-resistant ability for methanol oxidation in acidic media.
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COMPOSITES COMMUNICATIONS
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2018
·
IF 0
Ziqian Wu,Yunru Yu,Minhan Zou,Yuxiao Liu,Feika Bian,Yuanjin Zhao
With numerous unique properties, anisotropic particles which have non-spherical morphologies have intriguing great attention in recent years. Here, anisotropic microparticles with the shape of peanuts were fabricated through a novel microfluidic strategy, including microfluidic generation of droplet-containing fiber matrices and deformation of the droplets induced by stretching the fiber matrices. Droplets were emulsified in the microfluidic device system, in which flow rates were precisely controlled to determine droplet size and structure. Through stretching the elastic fibers, encapsulated droplets were able to be deformed into peanut-like shapes, with their interconnected cores well-aligned in correspondence to the stretching direction. Magnetic peanut-shaped particles could be obtained by incorporating magnetic nanoparticles , and showed extraordinary controllable ability under a changing magnetic field. In addition, the microparticles containing platinum and magnetic nanoparticles were generated and found being able to work as microstirrers. These features strongly attested the versatility and promising values of the peanut-inspired anisotropic microparticles in a broad range of application fields.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Jia-Hong Wu,Fang-Qi Shao,Shi-Yi Han,Song Bai,Jiu-Ju Feng,Zhengquan Li,Ai-Jun Wang
Photocatalytic degradation of environmental pollutants by using semiconductor-based photocatalysts offers great potential for remediation of toxic chemicals. For an economical and eco-friendly method to eliminate hexavalent chromium (Cr(VI)), favourable catalysts own high efficiency, stability and capability of harvesting light. Combination of metal with semiconductor is a promising route to improve the photocatalytic performance for Cr(VI) reduction. Herein, well-dispersed platinum (Pt) nanocubes (NCs) were synthesized by a facile one-step hydrothermal method with poly- l -lysine (PLL) as the growth-directing agent, followed by their uniform dispersion on graphitic carbon nitride (g-C 3 N 4 ). Their morphology, crystal structure, chemical composition , and formation mechanism were mainly characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). The hybrid nanocomposite was further explored for photocatalytic reduction of Cr(VI) to trivalent chromium (Cr(III)) under visible light at room temperature , by using formic acid (HCOOH) as a reducing agent, showing great improvement in photocatalytic activity and reusability, outperforming the referenced g-C 3 N 4 and home-made Pt black/g-C 3 N 4 catalysts. The effects of various experimental parameters and the proposed mechanism are discussed in detail.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Guoqiang Liu,Cuijiao Zhao,Guozhong Wang,Yunxia Zhang,Haimin Zhang
We investigate the possibility of utilizing benzyl alcohol oxidation reaction to replace sluggish oxygen evolution reaction (OER) for the charging process in a rechargeable zinc-air battery , catalyzed by NiCo alloy nanoparticles supported on activated carbon (NiCo/AC) with the multifunctional electrocatalytic activities of the oxygen reduction , oxygen evolution and benzyl alcohol oxidation reactions. As an electrocatalyst for the oxygen reduction reaction (OER), NiCo/AC exhibits superior catalytic activity with an onset potential of 0.85 V ( vs. RHE), a half-wave potential of 0.74 V ( vs. RHE) and a large limiting current density of 4.65 mA cm −2 at 0.2 V ( vs. RHE). Moreover, NiCo/AC also demonstrates the electrocatalytic oxidation activities toward water and benzyl alcohol, moreover, the benzyl alcohol oxidation reaction is more thermodynamically and kinetically favourable with 254 mV smaller overpotential than water oxidation at 10 mA cm −2 . Owing to these advantages, NiCo/AC as air cathode material is assembled into a home-made rechargeable zinc-air battery, resulting an almost 200 mV lower charging voltage at the current density of 50 mA cm −2 in the presence of 0.1 M benzyl alcohol compared to the battery without benzyl alcohol, consequently obtaining 10.5% energy saving at the charging current density of 50 mA cm −2 with high durability.
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高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 22
·13770-13776
·
IF 10.733
Yu Ding,Bo-Qiang Miao,Yu-Cheng Jiang,Hong-Chang Yao,Xi-Fei Li,Yu Chen
The hydrogen evolution reaction (HER) is an important half-reaction in water electrolysis. According to the Nernst equation, increasing the interfacial proton concentration may be an effective strategy for reducing the overpotential of HER. Herein, based on the interface engineering strategy, we successfully synthesized polyethyleneimine (PEI)-modified nickel phosphide (NiP2) nanosheets on carbon cloth (CC) nanohybrids (denoted as PEI@NiP2-CC). Multiple physical characterizations proved that the PEI molecules are firmly anchored on the NiP2 surface due to strong N–Ni interactions. In both acidic and neutral media, the solution protons increased at the PEI@NiP2-CC/electrolyte interface due to the protonation of the –NH2 groups in the PEI molecules. The effect of the molecular weight (MW) of PEI on the HER activity was explored in detail. The MW-optimized PEI@NiP2-CC nanohybrids showed only 44 and 100 mV overpotentials for HER in acidic and neutral media, respectively, and were much better than un-modified NiP2-CC nanohybrids. This work provides a strong basis for determining the correlativity between surface modification and catalytic activity.
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JOURNAL OF CATALYSIS
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2019
·
IF 7.723
Zuohui Wang,Nannan Heng,Xiaobing Wang,Jinling He,Yong Zhao
The original active site units and morphologies structure on catalyst surface is highly important to promote the rate of chemical reaction, while less concern is paid on their dynamic change during reaction process. Understanding these reconstructions in reactions is essential to illustrate the correlations between the structure and reactivity of catalyst, as well as the rational design of efficient catalyst. Here, single metal phophide materials are adopted as model electrocatalysts to show the structure evolution in the process of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). After both OER and HER operation, the core-shell structured metal-hydroxide/oxyhydroxide@metal-phosphide catalysts are generated, resulting in the high but decreased activity. To overcome the activity deterioration of metal phosphide induced by morphology reconstruction, binary heterostructure metal phosphides catalysts are designed and show the better OER and HER activity and stability compared to those of single phosphides. The work illustrates the structure-performance relationship of catalyst surface dynamics on catalytic performance, which will provide the guidance for designing high performance electrocatalysts, photocatalysts, and thermal catalysts.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yuancai Ge,Hang Chu,Jiyi Chen,Peiyuan Zhuang,Qianyi Feng,William R. Smith,Pei Dong,Mingxin Ye,Jianfeng Shen
Constructing regularly catalytic arrays is essential for electrochemical catalysis, especially for hydrogen evolution reaction (HER). In this work, two-dimensional zeolitic imidazolate framework (ZIF) arrays were chosen as templates to construct few-layer MoS2-decorated hollow CoP. By coupling MoS2 nanosheets arrays and two-dimensional ZIF-67 derived CoP, the advantages of the active sites of MoS2 nanosheets edges and CoP are combined for efficient HER, which can drive a current density of 100 mA/cm2 in both acid (91 mV) and alkaline (135 mV) solutions for 10 h. Furthermore, the prepared catalyst can reach a current density of 10 mA/cm2 with overpotentials of only 53 and 77 mV in 0.5 M H2SO4 and 1 M KOH, respectively. Most importantly, we believe replacing ZIF-67 powders with 2D ZIF-67 arrays can boost the electrochemical activities for HER and this method can provide us a guideline for the future application of two-dimensional ZIF-67 arrays to construct efficient electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Wenxin Zhu,Tianshu Zhang,Yi Zhang,Zhihao Yue,Yinge Li,Rong Wang,Yanwei Ji,Xuping Sun,Jianlong Wang
Although NiFe-based (oxy)hydroxides have been recognized as the most promising anode materials for industrial water splitting, the existed synthetic methods are difficult to fabricate NiFe-based (oxy)hydroxides simultaneously fulfilling the requirements of low-cost and ambient synthetic process, high performance, and easier realization of large-scale production. In this work, a simple while effective strategy was proposed to fabricate well-aligned Ni-Fe hydroxide nanosheets array on Ni foam (NiFe-OH NS/NF) by the ambient spontaneous redox reaction between Ni foam and Fe 3+ and accompanied hydrolysis co-deposition of the generated Ni 2+ , Fe 2+ /Fe 3+ , and OH − . The tailored highly-oriented amorphous and nanoporous nanosheets structure as well as the strong electronic interaction between Ni and Fe species endow this NiFe-OH NS/NF with excellent OER activity that a large current density of 500 mA cm −2 could be well afforded at a low overpotential of 292 mV. Importantly, the manufacturing and raw-materials cost to synthesize the NiFe-OH NS/NF by this strategy is estimated to be just $0.0165 per cm 2 , much lower than those for other reported self-supported Fe-containing catalyst materials. Also, this ambient means not only could be applicable to the large-scale production of size-tunable NiFe-OH NS/NF with stable nanoarray structure, but also could be easily used for the synthesis of NiCo NS/NF and NiCoFe NS/NF for applications.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Yihui Wu,Hanwei He
Designing and synthesizing of efficient and inexpensive bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is one of the current research topics. In this study, Ni Fe C Mo film in nickel mesh substrate is prepared by one-step direct-current electrodeposition method. The obtained Ni Fe C Mo film shows the excellent electrocatalytic activity , which only requires overpotentials of 254 mV for HER and 256 mV for OER to drive current density of 10 mA cm −2 , with corresponding Tafel slopes of 163.9 and 60.3 mV·dec −1 in 30% KOH medium, respectively. Moreover, Ni Fe C Mo film only needs a low cell voltage of 1.61 V to drive current density of 10 mA cm −2 in an alkaline electrolyzer . Such remarkably HER and OER properties of Ni Fe C Mo alloy is attributed to the increased effective electrochemically active surface area and the synergy effect among Ni, Fe, C and Mo.
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SEPARATION SCIENCE AND TECHNOLOGY
·
2018
·
IF 1.2
Yan Yan,Qi Wang,Zeyang Xiang,Yanzhao Yang
A reasonable project was presented for the extraction and separation of Pt(IV), Pd(II), Ru(III), and Rh(III) from the mixed imidazolium-based ionic liquids (ILs) [C6mim]Cl, [C6mim][NTf2], and [C6mim][DDTC]. Pt(IV) was first separated from other three platinum group metals with a mixture of [C6mim]Cl and [C6mim][NTf2]. Then, separation of Pd(II) and Ru(III) from Rh(III) was realized by changing the concentration of [C6mim][DDTC]. Back-extraction of Pt(IV), Pd(II), and Ru(III) from loaded hydrophobic phase and the recovery of Rh(III) in aqueous phase were also investigated. Mechanisms between Pd(II)/Ru(III) and [C6mim][DDTC] were further explored using ultraviolet spectrophotometry (UV-Vis), infrared spectrophotometry (FTIR), the method of continuous variations, ab initio quantum chemical studies, and X-ray crystallographic analysis. The results afford more directions for extracting and separating metals by introducing devisable functionalized group into ILs.
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高影响因子
CARBON
·
2018
·
IF 7.082
Guang Li,Qingfeng Yi,Xiaokun Yang,Yao Chen,Xiulin Zhou,Gang Xie
Ni-Co-N doped honeycomb carbon (HC) nano-composites Ni 3 Co 1 -N/HC (Ni 3 Co 1 -N/HC-20, Ni 3 Co 1 -N/HC-30 and Ni 3 Co 1 -N/HC-40 with respective metal mass percentage of 20%, 30% and 40%) with a regular hexagonal structure have been fabricated by using the simple polymethylmethacrylate (PMMA) emulsion template method . The side length of the carbon hexagon is ca. 100 nm for the honeycomb carbon (HC). For the Ni 3 Co 1 -N/HC catalysts, the NiCo nanoparticles and the nanocarbon tubes derived from dicyandiamide are uniformly dispersed on HCs. The as-synthesized Ni 3 Co 1 -N/HC catalysts exhibit efficient electroactivity for oxygen reduction reaction (ORR) in alkaline medium and possess excellent tolerance to the alcohols (ethanol, n -propanol and iso -propanol). Based on these results, a membrane-less direct alcohol fuel cell has been assembled with the Ni 3 Co 1 -N/HC as the cathodic catalyst, the ternary Pd 7 Ag 2 Sn 2 /CNT as the anodic catalyst and alcohol (ethanol, n -propanol or iso -propanol) as the fuel. The fuel cell with the Ni 3 Co 1 -N/HC-40 as the cathodic catalyst displays the open circuit voltage of 0.79 V and maximum power density of 42.2 mW cm −2 for the ethanol fuel , 0.60 V and 33.3 mW cm −2 for the n -propanol fuel, and 0.43 V and 14.4 mW cm −2 for the iso -propanol fuel. The membrane-less fuel cell also presents stable discharge performance at different discharging current densities.
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