JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Xiaoming Wang,Qianqian Peng,Xilin Zhang,Xucheng Lv,Xin Wang,Yongzhu Fu
Refractory high-entropy alloy nanocomposites (HEA-NPs) are important class of materials with unique structure and potential applications. Although several synthetic methods have been reported, developing novel routes to prepare nanoscale HEA-based catalysts facilely is still urgently desired. This work takes advantage of confinement assisted arc and plasma shock (APS) to prepare a series of HEA-NPs by regulating the type and proportion of metal precursors. The phase constitutes and morphology of the HEA-NPs are fully characterized. The prepared refractory HEA-NPs possesses five highly dispersed metal components, including titanium (Ti), niobium (Nb), tantalum (Ta), chromium (Cr), molybdenum (Mo) and simultaneously exhibits an uniform hexagonal morphology of nanocrystals . By taking advantage of its unique corrosion resistance , TiNbTaCrMo HEA-NPs can function as a promising candidate for electrocatalytic hydrogen evolution reaction (HER) in natural seawater . And its catalytic performance after alloying is significantly enhanced compared with the elemental metal. Theoretically, the promoted HER activity can be attributed to the strong adsorption for the various metal components in HEA-NPs caused by the upshifting d -band center close to the Fermi level . Furthermore, this confinement strategy can be further extended to synthesize other HEA-NPs. Our strategy provides a novel method to synthesize various HEA-NPs for further catalytic application.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Zhen Li,Miao Gong,Mengqi Wang,Aixin Feng,Linlu Wang,Peiyong Ma,Shoujun Yuan
Hydrogen has attracted significant attention as a clean energy source. Supercritical water gasification (SCWG) technology can produce hydrogen-rich gas while also disposing of sludge. The hydrogen yield from the SCWG of sludge is greatly increased when catalyzed by AlCl 3 . In this paper, a combined catalyst based on AlCl 3 was proposed to further increase the hydrogen yield of SCWG of dewatered sewage sludge (DSS). Analysis of the products from catalytic gasified of DSS and its model compounds were used to propose a catalytic mechanism and reaction pathway of the catalytic SCWG of DSS. Among the combined catalysts used for the SCWG of DSS, 10 wt% AlCl 3 –H 2 O 2 (mass ratio 8:2) had the best hydrogen production effect, and the hydrogen yield reached 8.88 mol/kg organic matter. This was 14% higher than when catalyzed by 10 wt% AlCl 3 . During catalysis with AlCl 3 , Al 3+ reacted with OH − in water and precipitated as Al(OH) 3 , which produced an acidic environment in the liquid product. Al(OH) 3 dehydrated to form an AlO(OH) and deposited in the solid product. A small amount of H 2 O 2 promoted the steam reforming reaction of organic matter in DSS, which increased the hydrogen yield. H 2 O 2 further promoted the hydrogen yield in an acidic environment. The catalytic effect of AlCl 3 was unaffected by H 2 O 2 . The H + generated by AlCl 3 during catalysis promoted H 2 O 2 to further depolymerized organic matter (such as humic substances) in DSS, so that AlCl 3 –H 2 O 2 catalyzed the SCWG of DSS to further increase the hydrogen yield. The order of hydrogen yield catalyzed by AlCl 3 –H 2 O 2 was guaiacol > humic acid > glycerol > alanine > glucose. Compared with AlCl 3 , AlCl 3 –H 2 O 2 reduced the hydrogen yield of glucose by nearly 20% and increased the hydrogen yield of humic acid by about 17% (25.81 mol/kg feed).
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NANO
·
2021
·
IF 1.556
Naiyuan Cui,Sizhan Wang,Lu Wang
It is of great significance to prepare electrochemical glucose sensors with high selectivity and stability via effective and rapid methods. In this work, the self-support electrode with copper and nickel-based oxide is prepared by chemical-etching reaction which occurred under the property of electrochemical potential difference. In this processing, nickel foam is etched selectively by Cu 2 + ions and they not only act as self-supporting electrode substrate, but also as nickel ions precursor of NiO. Moreover, the reaction can be completely satisfied on 30 min at room temperature. As a self-supporting electrode nonenzymic glucose electrochemical sensor, the electrode exhibited a wide linear range (0.04–3.00 mM), low detection limit (0.02 mM) with high sensitivity of 1096 μ A ⋅ mM − 1 ⋅ cm − 2 and good selectivity, repeatability and stability. Furthermore, the application of the prepared sensor provides an avenue for the application of the transition metal materials in the field of electrochemical sensing.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Ya-Nan Zhou,Fu-Li Wang,Shu-Yue Dou,Zhuo-Ning Shi,Bin Dong,Wen-Li Yu,Hui-Ying Zhao,Feng-Ge Wang,Jian-Feng Yu,Yong-Ming Chai
High-valence Nb has been proved to be promising to enhance oxygen evolution reaction (OER). However, how to realize the atomic doping of larger-radii Nb is challenging. Herein, an elaborate molten salt method is applied to rapidly incorporate Nb into NiFe-layered double hydroxides (Nb-NiFe-LDH). The fabricated Nb-NiFe-LDH is featured with nano pompons composed of cross-linked hollow nanotubes, which ensures maximum exposure of active sites. Meanwhile, the generated lattice defects can adjust electron density and absorption property of intermediates on the surface, facilitating oxygen evolution. As validation, the obtained Nb-NiFe-LDH exhibits motivated OER activity with overpotential of 242 mV at 50 mA cm −2 and small Tafel slope of 31.3 mV dec −1 as well as long-term stability of 73 h. DFT reveals that such superior OER performance benefits from the fine-tuned surface adsorption ability for reaction intermediates and electron transfer capability as well as optimized oxidation cycle of active metals by synergistic Nb and defects. This work is expected to provide deep insights into the advanced catalysts development via high-valence metal doping achieved by molten salt method.
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JOM
·
2021
·Vol. 73
·期 11
·3451-3459
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IF 2.474
Chen Ben,Li Zhi-Bo,Zhang Guo-Hua,Chou Kuo-Chih
To improve the performance of Mo-based cermets, Mo-(Ni)-Al 2 O 3 cermets were prepared with raw materials of nano-sized Al 2 O 3 powder. The effects of Al 2 O 3 and Ni additions on the densification behavior, microstructure, bending strength, and hardness of the Mo-(Ni)-Al 2 O 3 cermets were experimentally analyzed. The results showed the content of Al 2 O 3 had a great influence on the degree of densification of Mo-Al 2 O 3 cermets at the sintering temperature of 1600°C. In addition, the Al 2 O 3 particles were distributed evenly in the matrix of Mo-based cermets, which refined the grains of Mo and increased the hardness of cermets. Because of the weak interfacial bonding strength between Al 2 O 3 ceramic phase and Mo metal phase, the bending strength decreased continuously with increasing Al 2 O 3 content. However, Ni addition improved the wetting and adhesion of Al 2 O 3 and Mo. With the addition of Ni, the relative density increased, and thus hardness and bending strength were improved.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2021
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IF 8.067
Lianbo Wang,Shilong Xing,Zizhen Shen,Huabing Liu,Chuanhai Jiang,Vincent Ji,Yuantao Zhao
In current work, Ni-Ti-CeO 2 nanocomposite coatings were achieved by co-adding Ti microparticles and CeO 2 nanoparticles. Designed experiments and COMSOL computer simulation were applied to reveal the synergistic role of Ti microparticles and CeO 2 nanoparticles in tailoring the spatial microstructures and properties of Ni-Ti-CeO 2 nanocomposite coating. Unilaterally, the conductive Ti microparticles conducted the growth behavior of Ni grains by current density concentration, distorting electronic field lines and heterogeneous nucleation. Individual domains consisting of inner nanograins and outer radial columnar grains surrounded Ti microparticles, where Ti microparticles acted as seeds. Ti microparticles tended to be aggregated, leading to spatial heterogeneity of microstructures. Ni deposits buried the Ti microparticles in forms of “covering model”, contributing to the formation of inside voids and rough surface and aggregation of Ti microparticles; on the other hand, the non-conductive CeO 2 microparticles hardly changed the distribution of current density and electronic field lines on the cathode surface. Ni deposits buried the CeO 2 microparticle in forms of “stacking model”, avoiding the inside voids and aggregation of particles. The incorporation of CeO 2 microparticle brought in microstructure evolutions only on its top side without disturbing the growth behavior of Ni grains on its lateral side or bottom, suggesting the limited effects. This was correlated with the presence of current concentration above the CeO 2 microparticle at the last stage of burying CeO 2 microparticle. The co-addition of Ti microparticles and CeO 2 nanoparticles into Ni deposits exploited the complementary action of the two particles, which gave birth to satisfied spatial microstructures and improved hardness. Ti microparticles took major responsibility for microstructure evolutions, while the CeO 2 nanoparticles were mainly in charge of the microstructure homogeneity.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Yanhong Wang,Nannan Chen,Xiaoqiang Du,Xinghua Han,Xiaoshuang Zhang
Electrolysis of water is an environmentally friendly and promising hydrogen generation technology, which is one of the best ways to deal with the global energy crisis and environmental pollution. However, the slow anode reaction of water electrolysis is the bottleneck of limiting the efficient hydrogen production. Therefore, it is a key problem to explore an efficient and economical electrocatalyst to assist the anode reaction. Herein, a series of self-supporting M-NiCo 2 S 4 /Ni 3 S 2 (M=Mn, Fe, Cu, Zn) nanostructures grown on a nickel foam (NF) skeleton were prepared through one-step hydrothermal strategy. In this process, doping engineering is employed to adjust the electronic structure of catalyst and improve the performance of the catalyst. Among them, the introduction of Fe not only greatly changed the morphology, but also provided rich active sites. Specifically, the Fe-NiCo 2 S 4 /Ni 3 S 2 electrode can achieve current densities of 50 and 100 mA cm −2 at overpotential of 159 and 210 mV in alkaline media for oxygen evolution reaction (OER). In addition, driving current densities of 50 and 100 mA cm −2 in 1.0 M KOH with 0.5 M urea only requires the ultra-small voltage of 1.37 and 1.39 V (vs. RHE) for urea oxidation reaction (UOR), indicating that UOR can well replace OER to reduce electrical energy consumption. The experimental results and density functional theory calculations (DFT) demonstrate that the superior activity of the catalyst can be attributed to the optimal water adsorption energy, faster electron transfer rate, more active site exposure and good electrical conductivity . This work extends the application of doping engineering in water electrolysis and provides a novel preparation method of efficient catalyst for OER and UOR.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Manigandan Ramadoss,Yuanfu Chen,Xin Chen,Zhe Su,Marimuthu Karpuraranjith,Dongxu Yang,Manzoor Ahmad Pandit,Krishnamurthi Muralidharan
Rational construction of self-template catalysts for efficient electrolytic water splitting reactions is being a challenging prospect in sustainable energy production. For the first time, owing to these aims, we report a self-template representation of self-assembled iron-modulated cobalt-nickel phosphide (Fe-CoNiP) grown on 3D-nickel foam (NF) using a facile amine hydrolysis-approached synergetic phosphorylation strategy. Due to its unique vertically standing self-template hierarchical nanoarrays and atomic modulated multicomponent system, these Fe-CoNiP nanoarchitectures exhibit excellent electrocatalytic hydrogen and oxygen evolution reactions with very low applied overpotentials of 110 and 280 mV to obtain 10 mA cm–2, respectively, and an overpotential value of 390 mV (J10) obtained for overall water splitting overtakes most precious-metal/phosphide-based electrocatalysts in an alkaline medium. Moreover, the rationally cocrystallized Fe-CoNiP binder-free electrocatalyst as a multifunctional electrode has robust physicochemical stability above 2 days with very little degradation during alkaline electrolysis. These demonstrated results may lead to new insights into constructing an alternative electrocatalyst with hierarchical nanoarchitecture to boost the overall water splitting.
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Materials Research Express
·
2019
·Vol. 7
·期 1
·015007
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IF 1.449
Pengdong Feng,Mao Zhong,Weiwei Zhao
Next generation wearable electronics require stretchable dielectrics. There has been significant effort to characterize and improve the components of dielectric composites for use in these devices. In this work, a new stretchable dielectric material, composited by silver nanoparticles (Ag NPs), nickel nanoparticles (Ni NPs), and polydimethylsiloxane (PDMS), is prepared and characterized. The alternating arrays of Ag NPs groups and Ni NPs groups in the three-dimensional matrix of PDMS function as micro capacitors and prevent current percolation. Compared with PDMS alone, the alternating arrays exhibit a dielectric constant (k) that is increased by 1146% and can reach 35.13, with dielectric loss as low as 0.009. Slightly lower k and larger dielectric loss appear at high frequencies. The material exhibits negative temperature dependence, and the composition ratio affects the dielectric properties. The strain at break is 139.68% and the elastic modulus is as low as 3.57 kPa. By controlling the type, size and dispersion of metal nanoparticles in PDMS matrix, a parallel-plate capacitor with constant capacitance is achieved, demonstrating the dependence of the dielectric constant on the applied strain. Moreover, by replacing the parallel plates with cylindrical fibers, a capacitive strain sensor was demonstrated. After hundreds of stretching-releasing cycles, the dielectrics work normally. The excellent properties of this material suggest its significant potential for use in wearable electronics.
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CHEMOSPHERE
·
2019
·
IF 5.108
Xinying Zhang,Chang Su,Xiaoyan Liu,Zhenguo Liu,Xia Liang,Yanming Zhang,Yuwei Feng
The aim of this study was to investigate whether the plant-growth-promoting rhizobacteria (PGPR) could enhance phytoremediation efficiency of Scirpus triqueter ( S.triqueter ) in the pyrene-Ni co-contaminated soil. We also expected to reveal the possible mechanism for the affected phytoremediation efficiency induced by PGPR. We used three kinds of contaminated soils (Ni-contaminated soil, pyrene-contaminated soil and pyrene-Ni co-contaminated soil) to conduct this pot study. After harvest, plants growth indicators, polyphenol oxidase (PPO) activity and soil microbial community structure of each treatment were investigated to explain the different dissipation rates of pyrene and removal rates of Ni between treatments with and without PGPR. The results showed that PGPR-inoculated S. triqueter increased dissipation rates of pyrene and removal rates of Ni in all three contaminated soils, among which Ni removal rates in Ni single contaminated soil was elevated most significantly, from 0.895‰ to 8.8‰, increasing nearly 9 folds. However, Ni removal rate efficiency in co-contaminated soil was weakened because more toxic and complicated co-contaminated soil restrained plant growth and Ni absorption. We also observed that co-contamination harmed the soil microbial community more severely than that in single pyrene or Ni contaminated soil through phospholipid fatty acids analysis. Furthermore, dissipation rates of pyrene and removal rates of Ni were found positively correlated to the PPO activity and the abundance of branched and saturated fatty acids reflected by Pearson correlation analysis.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 10
·9480-9489
·
IF 2.914
Dai Shijin,Zheng Yilin,Zhao Youcai,Li Qiang,Niu Dongjie
Chlorine-containing organic waste (COWs) is a big threat for the waste incineration because of the dioxin generation and equipment corrosion. Recently, dechlorination and detoxification of COWs is emergent in order to lower the environmental risk and treatment costs. In this study, base-catalyzed decomposition processes with different hydroxides, hydrogen donors, and catalysts were conducted for pre-treatment of COWs to reduce organic chlorine content, with the TCB as a model compound and industrial rectification residues for verification. Results showed that maximum chlorine retention efficiency (CRE) of four alkalis followed the order of KOH > NaOH–KOH > NaOH > Mg(OH) 2 , which were 98.3%, 93.4%, 97.2%, and 1.5%, respectively, and could be expressed as an apparent first-order reaction. The differences were resulted from the varying ionic potentials of the metal cations. Hydrogen donors (glycol, glycerol, paraffin oil, and PEG 200) acted as effective dechlorination regents follow the order of PEG > glycol > paraffin oil > glycerol. In addition, Fe, Ni, Cu, and activated carbon catalysts increased the CRE by 68.9% to 92.4%, 91.9%, 89.2%, and 73.3%, respectively. Residue analysis through X-ray diffraction and Fourier transform infrared spectroscopy revealed that KCl, sodium oxalate, and phenol were the main products and a plausible stepwise dechlorination pathway was proposed. The effectiveness of three optimized combinations including NaOH/PEG, KOH/PEG, and NaOH–KOH/PEG (with the Fe catalyst) was confirmed by using them for dechlorinating rectification residues, and they restrained 98.2%, 91.2%, and 94.6% of the chlorine, respectively. The organochlorine content decreased from 19.2 to 1.8% within 180 min, while inorganic chorine content increased from 1.5 to 18.9%, indicating the potential for COWs dechlorination.
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ACS Catalysis
·
2019
·
IF 12.221
Xiaoqiang Zhang,Peifang Yan,Bin Zhao,Kairui Liu,Mayfair C. Kung,Harold H. Kung,Shanyong Chen,Z. Conrad Zhang
The catalytic properties of physical mixtures of Ni particles (100–200 nm) with nanoparticles of anatase TiO2 (TiO2-A), ZrO2, Al2O3, rutile TiO2 (TiO2-R), and CeO2 were investigated for the hydrodeoxygenation (HDO) of guaiacol. High selectivities to phenolics were obtained only for Ni mixed with anatase TiO2 (Ni and TiO2-A), while saturated hydrocarbons were the main products for the mixtures with other supports. By thermal treatment in hydrogen gas only at 300 °C or higher and subsequently separating the large Ni particles from the TiO2-A particles with a magnet, it was further discovered that there was migration of TiO2 from TiO2-A onto the large Ni particles, resulting in an amorphous TiO2 overlayer on the Ni particles as evidenced by high-resolution TEM, and vice versa, migration of Ni onto TiO2-A. The TiO2 overlayer rendered the Ni particles completely inactive as a hydrogenation/hydrodeoxygenation catalyst. Conversely, the small amounts of Ni (<1.5 wt %) migrated onto TiO2-A formed highly dispersed Ni, undetectable by high-resolution TEM (<2 nm), that were remarkably highly active for HDO of guaiacol, producing selectively phenolics. Such highly selective HDO catalysts could also be formed by incipient wetness impregnation of Ni in loadings above 2 wt % onto the TiO2-A, but it was essential to pretreat the sample in H2 at 300 °C or higher. Pretreatment in H2 at 200 °C generated catalysts that produced saturated ring products. The activity of the impregnated catalysts, as measured by guaiacol conversion, increased linearly with Ni loading below 0.5 wt %. The activity continued to increase with Ni loading but more slowly up to 2 wt %, beyond which there was little further change. The results suggested that two types of Ni species existed on the TiO2-A surface. One type consisted of a cluster of Ni atoms that were dominant on larger Ni particles that were active in aromatic ring hydrogenation and hydrodeoxygenation. They were readily covered by reducible TiO2-A at 300 °C or higher due to the traditional strong metal support interaction (SMSI) effect and became inactive. Another type was clusters of a very small number of Ni atoms, perhaps one atom, that were present as highly dispersed Ni clusters interacting strongly with the defect sites of TiO2-A. The strong interaction of this type of Ni with the TiO2 defect deterred TiOx migration allowing surface exposed Ni atoms to catalyze the HDO of guaiacol with very high selectivities that were not characteristic of typical Ni particles.
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危险品化学品经营许可证（带存储）