Ni nanoparticles

Ni 纳米颗粒
  • 文章类型: Journal Article
    锂硫(Li-S)电池被认为是有前途的储能系统,因为它们的理论能量密度高,低成本,和生态友好。然而,诸如穿梭效应之类的问题可能导致活性材料的损失,循环性差,和快速的容量退化。通过双吸附-催化策略增强电化学性能的结构配置的利用可以克服Li-S电池的局限性。在这项研究中,集成的夹层结构,其中中空碳纤维(HCFs)用原位生成的Ni纳米颗粒改性,通过可扩展的一步碳化制备。高度分层多孔HCF充当碳骨架并提供增强离子/电子扩散的连续三维导电网络。Ni纳米粒子具有优越的锚定和催化能力,可以防止穿梭效应,提高转化率,从而促进电化学性能。这种协同效应导致100次循环后在1C下的582mAhg-1的高容量保留,提供高达3C的优异倍率性能。该新颖结构,其中Ni纳米颗粒嵌入棉花组织来源的HCFs中,提供了在高C倍率下增强电化学性能的新途径。这导致低成本,可持续,和高性能的混合材料,用于开发实用的Li-S电池。
    Lithium-sulfur (Li-S) batteries are considered promising energy-storage systems because of their high theoretical energy density, low cost, and eco-friendliness. However, problems such as the shuttle effect can result in the loss of active materials, poor cyclability, and rapid capacity degradation. The utilization of a structural configuration that enhances electrochemical performance via dual adsorption-catalysis strategies can overcome the limitations of Li-S batteries. In this study, an integrated interlayer structure, in which hollow carbon fibers (HCFs) were modified with in-situ-generated Ni nanoparticles, was prepared by scalable one-step carbonization. Highly hierarchically porous HCFs act as the carbon skeleton and provide a continuous three-dimensional conductive network that enhances ion/electron diffusion. Ni nanoparticles with superior anchoring and catalytic abilities can prevent the shuttle effect and increase the conversion rate, thereby promoting the electrochemical performance. This synergistic effect resulted in a high capacity retention of 582 mAh g-1 at 1 C after 100 cycles, providing an excellent rate capability of up to 3 C. The novel structure, wherein Ni nanoparticles are embedded in cotton-tissue-derived HCFs, provides a new avenue for enhancing electrochemical performance at high C rates. This results in a low-cost, sustainable, and high-performance hybrid material for the development of practical Li-S batteries.
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  • 文章类型: Journal Article
    金属纳米颗粒(NP)在钙钛矿氧化物上的溶出已被证明是生产催化剂-载体系统的可靠策略。传统的解决方案需要长时间的高温,限制支撑材料的选择。据报道,在室温和大气压下,NiNPs的等离子体直接溶解来自模型A位缺陷钙钛矿氧化物(La0.43Ca0.37Ni0.06Ti0.94O2.955)。使用仅He气体以及He/H2气体混合物的介质阻挡放电配置,在几分钟内(最多15分钟)内进行等离子体释放。产生小NP(<30nm直径)。为了证明解出NP的实用性,旨在评估其从合成气中甲烷化的催化性能的各种实验,CO,和CH4氧化进行。成功证明了低温和大气压等离子体溶液,并表明这种方法可能有助于基于溶液的稳定催化剂系统的实际部署。
    Exsolution of metal nanoparticles (NPs) on perovskite oxides has been demonstrated as a reliable strategy for producing catalyst-support systems. Conventional exsolution requires high temperatures for long periods of time, limiting the selection of support materials. Plasma direct exsolution is reported at room temperature and atmospheric pressure of Ni NPs from a model A-site deficient perovskite oxide (La0.43Ca0.37Ni0.06Ti0.94O2.955). Plasma exsolution is carried out within minutes (up to 15 min) using a dielectric barrier discharge configuration both with He-only gas as well as with He/H2 gas mixtures, yielding small NPs (<30 nm diameter). To prove the practical utility of exsolved NPs, various experiments aimed at assessing their catalytic performance for methanation from synthesis gas, CO, and CH4 oxidation are carried out. Low-temperature and atmospheric pressure plasma exsolution are successfully demonstrated and suggest that this approach could contribute to the practical deployment of exsolution-based stable catalyst systems.
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  • 文章类型: Journal Article
    镍茂的声化学分解效应,研究了在低温下容易升华的镍细颗粒的合成方法。在一水合肼和2-丙醇混合溶剂中,超声辐照促进了镍茂的还原,合成了镍细颗粒,同时排除了镍茂的升华。与常见的肼还原镍盐不同,这需要多步反应,镍茂直接还原而不形成中间体。研究了水浴温度(20-60°C)的影响,其中使用较高的水浴温度(60°C)合成较大的细颗粒。当在20°C下照射时,镍新世的还原率低,通过镍茂的还原和分解,导致镍细颗粒和有机纳米颗粒的形成。还调查了超声频率,其中使用低频超声辐照合成了细镍颗粒。高温热点的形成导致镍在镍细颗粒表面的扩散和生长;因此,合成了树莓状镍细颗粒。在这项研究中,镍新世的难以处理的性质,由于它的升华特性,很容易被超声波照射克服。热点处的瞬时和局部反应有助于抑制颗粒生长。此外,通过直接还原途径合成Ni细颗粒,这与以前的反应不同。此方法表示一个新的,无分散剂,合成Ni细颗粒的低温工艺。
    Sonochemical decomposition effects of nickelocene, which sublimates easily were investigated to synthesize dispersant-free nickel fine particles at low temperature. In a hydrazine monohydrate and 2-propanol mixed solvent, the reduction of nickelocene was promoted by ultrasound irradiation, and nickel fine particles were synthesized while precluding the sublimation of nickelocene. Unlike the common hydrazine reduction of nickel salts, which requires multiple-step reactions, nickelocene was reduced directly without forming intermediates. The effect of the water-bath temperature (20-60 °C) was investigated, where larger fine particles were synthesized using a higher water-bath temperature (60 °C). When irradiated at 20 °C, the reduction rate of nickelocene was low, leading to the formation of nickel fine particles and organic nanoparticles via the reduction and decomposition of nickelocene. The ultrasound frequency was also investigated, where fine nickel particles were synthesized using low-frequency ultrasound irradiation. The formation of high-temperature hotspots led to the diffusion and growth of nickel on the surface of the nickel fine particles; therefore, raspberry-like nickel fine particles were synthesized. In this study, the difficult-to-handle nature of nickelocene, owing to its sublimation properties, was easily overcome by ultrasound irradiation. Instantaneous and localized reactions at hotspots contributed to inhibiting particle growth. Furthermore, Ni fine particles were synthesized via a direct reduction pathway, which differs from previous reactions. This method represents a new, dispersant-free, low-temperature process for synthesizing Ni fine particles.
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  • 文章类型: Journal Article
    这项研究研究了纳米多孔La0.52Sr0.28Ti0.94Ni0.06O3钙钛矿中Ni纳米颗粒的氧化还原溶液。溶解镍纳米颗粒的特性,包括它们的尺寸,人口,通过环境扫描电子显微镜(ESEM)对表面浓度进行了深入分析,透射电子显微镜-能量色散X射线光谱(TEM-EDX)作图,和氢气程序升温还原(H2-TPR)。镍溶液早在400°C时就在氢气中触发,在500°C的还原步骤后,对低温CO氧化具有最高的催化活性,尽管只有10%的镍溶解。在具有相似化学组成(La0.65Sr0.35TiO3)以及可比的比表面积和Ni负载量的钙钛矿材料上,将溶解的纳米颗粒的活性和稳定性与其浸渍的对应物进行了比较。在800°C下进行老化步骤后,发现溶解的Ni纳米颗粒在300°C下的催化活性比浸渍的纳米颗粒高10倍,强调氧化还原溶液制备的Ni纳米颗粒的热稳定性。
    This study investigated the redox exsolution of Ni nanoparticles from a nanoporous La0.52Sr0.28Ti0.94Ni0.06O3 perovskite. The characteristics of exsolved Ni nanoparticles including their size, population, and surface concentration were deeply analyzed by environmental scanning electron microscopy (ESEM), transmission electron microscopy-energy dispersive X-ray spectroscopy (TEM-EDX) mapping, and hydrogen temperature-programmed reduction (H2-TPR). Ni exsolution was triggered in hydrogen as early as 400 °C, with the highest catalytic activity for low-temperature CO oxidation achieved after a reduction step at 500 °C, despite only a 10% fraction of Ni exsolved. The activity and stability of exsolved nanoparticles were compared with their impregnated counterparts on a perovskite material with a similar chemical composition (La0.65Sr0.35TiO3) and a comparable specific surface area and Ni loading. After an aging step at 800 °C, the catalytic activity of exsolved Ni nanoparticles at 300 °C was found to be 10 times higher than that of impregnated ones, emphasizing the thermal stability of Ni nanoparticles prepared by redox exsolution.
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  • 文章类型: Journal Article
    对于通过水分解制氢的析氢反应(HER)和析氧反应(OER),实现高效的双功能电催化剂仍然是一个巨大的挑战。在这里,通过简单的热解策略,成功地在泡沫镍上制备了分散在嵌入碳层中的一维(1D)碳化钼微柱(Ni/Mo2C@C)上的新型混合镍纳米颗粒。在合成过程中,在H2和C2H2混合气氛下同时生成镍纳米颗粒和碳化钼,并保形地包封在碳层中。得益于独特的0D/1D异质结构以及双相Mo2C和Ni的协同作用以及碳层的保护作用,可以实现降低活化能障碍和快速催化反应动力学,在10mAcm-2的电流密度下,HER的过电位为96mV,OER的过电位为266mV,并且在1.0MKOH电解质中具有出色的耐久性。此外,使用开发的Ni/Mo2C@C作为阴极和阳极,构建的电解槽表现出1.55V的小电压,用于整个水分解。新设计的Ni/Mo2C@C可以为开发具有低成本过渡金属元素的高效双功能催化剂用于水分解提供启发。
    It remains a tremendous challenge to achieve high-efficiency bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) for hydrogen production by water splitting. Herein, a novel hybrid of 0D nickel nanoparticles dispersed on the one-dimensional (1D) molybdenum carbide micropillars embedded in the carbon layers (Ni/Mo2C@C) was successfully prepared on nickel foam by a facile pyrolysis strategy. During the synthesis process, the nickel nanoparticles and molybdenum carbide were simultaneously generated under H2 and C2H2 mixed atmospheres and conformally encapsulated in the carbon layers. Benefiting from the distinctive 0D/1D heterostructure and the synergistic effect of the biphasic Mo2C and Ni together with the protective effect of the carbon layer, the reduced activation energy barriers and fast catalytic reaction kinetics can be achieved, resulting in a small overpotential of 96 mV for the HER and 266 mV for the OER at the current density of 10 mA cm-2 together with excellent durability in 1.0 M KOH electrolyte. In addition, using the developed Ni/Mo2C@C as both the cathode and anode, the constructed electrolyzer exhibits a small voltage of 1.55 V for the overall water splitting. The novel designed Ni/Mo2C@C may give inspiration for the development of efficient bifunctional catalysts with low-cost transition metal elements for water splitting.
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  • 文章类型: Journal Article
    电催化还原CO2(ECR)为抑制碳排放和完成碳循环提供了一种有前途的方法。然而,在中性或碱性电解质中不可避免地产生碳酸盐和有限的CO2利用效率导致能源效率低,碳损失及其广泛的商业利用。在酸性条件下减少CO2的进步为其商业利用提供了一种有前途的方法,但是抑制析氢反应和催化剂的腐蚀仍然具有挑战性。在这里,通过简单的混合加热和冷冻干燥方法成功制备了包裹在N掺杂碳纳米管(NixNC-a)中的Ni纳米颗粒(NPs)。Ni100NC-a在pH通用条件下对CO实现了接近100%的高法拉第效率(FE),再加上有希望的CO电流密度(>100mAcm-2)。尤其是在酸性条件下,Ni100NC-a表现出出色的ECR性能,在-1.44V时的高FECO为97.4%,在-1.74V时的转换频率(TOF)为11kh-1,电流密度为288.24mAcm-2。这种优异的性能归因于NiNPs和N掺杂碳壳的协同作用,保护NiNPs免受蚀刻,促进CO2吸附和调节局部pH。此外,Ni100NC-a可以驱动可逆Zn-CO2电池,具有4.68mWcm-2的高功率密度和出色的稳定性(98h)。这项研究为有效的pH通用CO2电还原和Zn-CO2电池提供了有希望的候选者。
    Electrocatalytic reduction of CO2 (ECR) offers a promising approach to curbed carbon emissions and complete carbon cycles. However, the inevitable creation of carbonates and limited CO2 utilization efficiency in neutral or alkaline electrolytes result in low energy efficiency, carbon losses and its widespread commercial utilization. The advancement of CO2 reduction under acidic conditions offers a promising approach for their commercial utilization, but the inhibition of hydrogen evolution reaction and the corrosion of catalysts are still challenging. Herein, Ni nanoparticles (NPs) wrapped in N-doped carbon nanotubes (NixNC-a) are successfully prepared by a facile mixed-heating and freeze-drying method. Ni100NC-a achieves a high Faraday efficiency (FE) of near 100 % for CO under pH-universal conditions, coupled with a promising current density of CO (>100 mA cm-2). Especially in acidic conditions, Ni100NC-a exhibits an exceptional ECR performance with the high FECO of 97.4 % at -1.44 V and the turnover frequency (TOF) of 11 k h-1 at -1.74 V with a current density of 288.24 mA cm-2. This excellent performance is attributed to the synergistic effect of Ni NPs and N-doped carbon shells, which protects Ni NPs from etching, promotes CO2 adsorption and regulates local pH. Moreover, Ni100NC-a could drive the reversible Zn-CO2 battery with a high power-density of 4.68 mW cm-2 and a superior stability (98 h). This study presents a promising candidate for efficient pH-universal CO2 electroreduction and Zn-CO2 battery.
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  • 文章类型: Journal Article
    设计催化剂以沿着所需的反应途径进行催化反应,例如,CO2甲烷化,受到了很多关注,但仍然是一个巨大的挑战。这项工作报告了一种Ru1Ni单原子合金(SAA)催化剂(Ru1Ni/SiO2),该催化剂是通过RuCl3和Ni纳米颗粒(NP)之间的电置换反应制备的,该反应源自Ni页硅酸盐(Ni-ph)的还原。Ru1Ni/SiO2对CO2加氢为CH4的选择性和催化活性(周转频率(TOF)值:40.00×10-3s-1)大大提高,远高于Ni/SiO2(TOF值:4.40×10-3s-1)和大多数报道的Ni基催化剂(TOF值:1.03×10-3-11.00×10-3s-1)。实验研究证明,Ru单原子通过Ru1-Ni配位固定在NiNPs表面上,并伴随着从Ru1到Ni的电子转移。原位实验和理论计算都证实Ru1Ni-SAA的界面位点是内在活性位点,这促进了CO2的直接离解,降低了CO*中间体加氢的能障,从而引导和增强CO2氢化为CH4。
    Designing catalysts to proceed with catalytic reactions along the desired reaction pathways, e.g., CO2 methanation, has received much attention but remains a huge challenge. This work reports one Ru1Ni single-atom alloy (SAA) catalyst (Ru1Ni/SiO2) prepared via a galvanic replacement reaction between RuCl3 and Ni nanoparticles (NPs) derived from the reduction of Ni phyllosilicate (Ni-ph). Ru1Ni/SiO2 achieved much improved selectivity toward hydrogenation of CO2 to CH4 and catalytic activity (Turnover frequency (TOF) value: 40.00 × 10-3 s-1), much higher than those of Ni/SiO2 (TOF value: 4.40 × 10-3 s-1) and most reported Ni-based catalysts (TOF value: 1.03 × 10-3-11.00 × 10-3 s-1). Experimental studies verify that Ru single atoms are anchored onto the Ni NPs surface via the Ru1-Ni coordination accompanied by electron transfer from Ru1 to Ni. Both in situ experiments and theoretical calculations confirm that the interface sites of Ru1Ni-SAA are the intrinsic active sites, which promote the direct dissociation of CO2 and lower the energy barrier for the hydrogenation of CO* intermediate, thereby directing and enhancing the CO2 hydrogenation to CH4.
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  • 文章类型: Journal Article
    在制备过程中以及在超临界2-丙醇(250°C,70bar)使用原位电子自旋共振。原位电子自旋共振已用于研究催化剂钝化和随后在气流中还原氧化物层的过程。在超临界2-丙醇中已检测到钝化Ni纳米颗粒表面上NiO层的还原,这与动力学建模数据一致。已经发现,与氢气流量的还原相比,超临界2-丙醇中氧化镍层的还原发生在较低的温度下,根据原位电子自旋共振研究。
    Highly dispersed Ni-TiO2 catalyst has been studied in the process of preparation and under catalytic transfer hydrogenation reaction conditions in supercritical 2-propanol (250°C, 70 bar) using electron spin resonance in situ. Electron spin resonance in situ has been used to study the process of the catalyst passivation and subsequent reduction of the oxide layer in the gas flow. Reduction of the NiO layer on the surface of passivated Ni nanoparticles has been detected in supercritical 2-propanol, which is in agreement with kinetic modeling data. It has been found that the reduction of the nickel oxide layer in supercritical 2-propanol occurs at a lower temperature compared with the reduction in hydrogen flow, according to in situ electron spin resonance study.
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  • 文章类型: Journal Article
    这项研究的目的是使用氯化镍盐和称为DPMN的席夫碱配体产生稳定的镍纳米颗粒。合成过程涉及两步相转移程序。使用诸如UV-可见光和FT-IR的光谱技术来确认配体稳定的镍纳米颗粒(DPMN-NiNP)的形成。要分析大小,表面形态,和DPMN-NiNPs的质量,利用SEM和TEM技术。进行了体外研究,以研究合成化合物对三种不同癌细胞系和一种正常细胞系的潜在抗癌活性。并将结果与顺铂的结果进行了比较。研究人员还进行了测试,以确定DPMN-NiNPs结合CT-DNA的能力,使用各种技术,如电子吸收,荧光,测粘度,和循环伏安法。结果表明,合成的DPMN-NiNPs具有良好的DNA结合能力,通过使用热和声化学方法对DNA进行变性进一步验证。研究人员还研究了DPMN-NiNPs的抗菌和抗氧化活性,表现出比单独的DPMN更好的生物活性。此外,发现合成的纳米化合物选择性地损伤癌细胞系,而不伤害正常细胞系。最后,研究人员通过使用紫外可见光谱法测试DPMN-NiNPs分解甲基红染料的能力,研究了DPMN-NiNPs作为染料降解催化剂的潜力。由RamaswamyH.Sarma沟通。
    合成具有头基团和尾基团的生物活性有机席夫碱配体头基团相互作用并稳定镍纳米颗粒Ni纳米颗粒的平均尺寸为45nm固体并制备稳定的镍纳米颗粒。镍纳米颗粒具有良好的生物性能和催化性能。
    The objective of this research was to create stable nickel nanoparticles using nickel chloride salt and a Schiff base ligand called DPMN. The synthesis process involved a two-step phase transfer procedure. Spectroscopic techniques such as UV-Visible and FT-IR were used to confirm the formation of ligand-stabilized nickel nanoparticles (DPMN-NiNPs). To analyze the size, surface morphology, and quality of DPMN-NiNPs, SEM and TEM techniques were utilized. In vitro studies were performed to investigate the potential anticancer activity of the synthesized compounds against three different cancer cell lines and one normal cell line, and the results were compared to those of cis-platin. The researchers also conducted tests to determine the ability of DPMN-NiNPs to bind to CT-DNA using various techniques such as electronic absorption, fluorescence, viscometric, and cyclic voltammetric. The results showed that the synthesized DPMN-NiNPs exhibited good DNA binding ability, which was further validated by denaturation of DNA using thermal and sonochemical methods. The researchers also investigated the antimicrobial and antioxidant activities of DPMN-NiNPs, which demonstrated better biological activities than DPMN alone. Furthermore, the synthesized nano compounds were found to selectively damage cancer cell lines without harming normal cell lines. Finally, the researchers examined the potential of DPMN-NiNPs as a catalyst in dye degradation by testing its ability to decompose methyl red dye using UV-Visible spectroscopy.Communicated by Ramaswamy H. Sarma.
    Bioactive organic Schiff-base ligand having head group and tail group was synthesizedHead group interacted and stabilized the nickel nanoparticlesAverage size of the Ni nanoparticles is 45 nmSolid and stable nickel nanoparticles were prepared.Nickel nanoparticles have good biological properties as well as catalytical properties.
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  • 文章类型: Journal Article
    催化甲烷分解(CMD)已经成为从天然气大规模生产H2和碳纳米结构的有吸引力的技术。由于CMD过程是轻度吸热的,在低温条件下应用集中的可再生能源,例如太阳能,可能代表CMD工艺操作的一种有希望的方法。在这里,Ni/Al2O3-La2O3蛋黄壳催化剂是使用简单的单步水热方法制备的,并测试了它们在光热CMD中的性能。我们表明,所得材料的形态,Ni纳米颗粒的分散性和还原性,金属-载体相互作用的性质可以通过添加不同量的La来调节。值得注意的是,与基础Ni/Al2O3材料相比,添加最佳量的La(Ni/Al-20La)提高了H2产率和催化剂稳定性,同时也有利于碳纳米纤维的基本生长。此外,我们首次展示了CMD中的光热效应,通过在500°C的恒定本体温度下引入3个太阳的光照射,相对于黑暗中的速率,催化剂的H2产率可逆地增加了约1.2倍,伴随着表观活化能从41.6kJmol-1降低到32.5kJmol-1。光照射进一步抑制了在低温下不期望的CO共同产生。我们的工作揭示了光热催化作为CMD的有前途的途径,同时提供了对改性剂在Al2O3基催化剂上富集甲烷活化位点的作用的深刻理解。
    Catalytic methane decomposition (CMD) has emerged as an appealing technology for large-scale production of H2 and carbon nanostructures from natural gas. As the CMD process is mildly endothermic, the application of concentrated renewable energy sources such as solar energy under a low-temperature regime could potentially represent a promising approach towards CMD process operation. Herein, Ni/Al2O3-La2O3 yolk-shell catalysts are fabricated using a straightforward single-step hydrothermal approach and tested for their performance in photothermal CMD. We show that the morphology of the resulting materials, dispersion and reducibility of Ni nanoparticles, and nature of metal-support interactions can be tuned by addition of varying amounts of La. Notably, the addition of an optimal amount of La (Ni/Al-20La) improved the H2 yield and catalyst stability relative to the base Ni/Al2O3 material, while also favoring base growth of carbon nanofibers. Additionally, we show for the first time a photothermal effect in CMD, whereby the introduction of 3 suns light irradiation at a constant bulk temperature of 500 °C reversibly increased the H2 yield of catalyst by about 1.2 times relative to the rate in the dark, accompanied by a decrease in apparent activation energy from 41.6 kJ mol-1 to 32.5 kJ mol-1. The light irradiation further suppressed undesirable CO co-production at low temperatures. Our work reveals photothermal catalysis as a promising route for CMD while providing an insightful understanding of the roles of modifier in enriching methane activation sites on Al2O3-based catalysts.
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