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Highly Defective Dark TiO_(2) Modified with Pt: Effects of Precursor Nature and Preparation Method on Photocatalytic Properties
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作者 E.D.Fakhrutdinova O.A.Reutova +6 位作者 T.A.Bugrova I.Yu.Ovsyuk L.S.Kibis O.A.Stonkus D.B.Vasilchenko O.V.Vodyankina V.A.Svetlychnyi 《Transactions of Tianjin University》 EI CAS 2024年第2期198-209,共12页
The study focused on the modification with platinum of dark defective titania obtained via pulsed laser ablation. Both the method of Pt introduction and the nature of the Pt precursor were varied. All samples exhibite... The study focused on the modification with platinum of dark defective titania obtained via pulsed laser ablation. Both the method of Pt introduction and the nature of the Pt precursor were varied. All samples exhibited similar phase compositions, specific surface areas, and Pt contents. High-resolution transmission electron microscopy coupled with pulsed CO adsorption revealed increased dispersity when photoreduction and the hydroxonitrate complex (Me _(4) N) _(2) [Pt _(2) (OH) _(2) (NO _(3) ) _(8) ] were used. The sample featured a high content of single-atom species and subnano-sized Pt clusters. The X-ray photoelectron spectroscopy results showed that the photoreduction method facilitated the appearance of a larger number of Pt ^(2+) states, which appeared owing to the strong metal-support interaction (SMSI) eff ect of the transfer of electron density from the electron-saturated defects on the TiO _(2) surface to Pt ^(4+) . In the hydrogen evolution reaction, samples with a significant fraction of the Pt ^(2+) ionic component, capable of generating short-lived Pt^(0) single-atom sites under irradiation due to the SMSI eff ect, exhibited the highest photocatalytic activity. The 0.5Pt(C)/TiO_(2) -Ph sample exhibited the highest hydrogen yield with a quantum efficiency of 0.53, retaining its activity even after 8 h of operation. 展开更多
关键词 Dark(black)TiO_(2) Pulsed laser ablation Platinum reduction method Precursor type PHOTOCATALYSIS hydrogen evolution reaction
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Thermodynamics and kinetics of hydriding and dehydriding reactions in Mg-based hydrogen storage materials 被引量:20
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作者 Qian Li Yangfan Lu +10 位作者 Qun Luo Xiaohua Yang Yan Yang Jun Tan Zhihua Dong Jie Dang Jianbo Li Yuan Chen Bin Jiang Shuhui Sun Fusheng Pan 《Journal of Magnesium and Alloys》 SCIE EI CAS CSCD 2021年第6期1922-1941,共20页
Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamic... Mg-based materials are one of the most promising hydrogen storage candidates due to their high hydrogen storage capacity,environmental benignity,and high Clarke number characteristics.However,the limited thermodynamics and kinetic properties pose major challenges for their engineering applications.Herein,we review the recent progress in improving their thermodynamics and kinetics,with an emphasis on the models and the influence of various parameters in the calculated models.Subsequently,the impact of alloying,composite,and nanocrystallization on both thermodynamics and dynamics are discussed in detail.In particular,the correlation between various modification strategies and the hydrogen capacity,dehydrogenation enthalpy and temperature,hydriding/dehydriding rates are summarized.In addition,the mechanism of hydrogen storage processes of Mg-based materials is discussed from the aspect of classical kinetic theories and microscope hydrogen transferring behavior.This review concludes with an outlook on the remaining challenge issues and prospects. 展开更多
关键词 Magnesium-based hydrogen storage materials Hydriding/dehydriding reactions THERMODYNAMICS Kinetic models Analysis methods
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稠环化合物脱氢反应的热力学计算
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作者 巩洪旭 刘涛 戴立顺 《石油炼制与化工》 CAS CSCD 北大核心 2024年第6期99-106,共8页
采用Benson基团贡献法对菲(PH)、芘(PY)及2-甲基菲(2-MP)加氢反应网络中欠缺的化合物标准摩尔生成焓、绝对熵和定压摩尔热容进行估算;并以物性数据为基础,计算PH,PY,2-MP加氢反应网络中各反应的反应焓变、反应吉布斯自由能变、平衡常数... 采用Benson基团贡献法对菲(PH)、芘(PY)及2-甲基菲(2-MP)加氢反应网络中欠缺的化合物标准摩尔生成焓、绝对熵和定压摩尔热容进行估算;并以物性数据为基础,计算PH,PY,2-MP加氢反应网络中各反应的反应焓变、反应吉布斯自由能变、平衡常数和转化率。计算结果表明:PH,PY,2-MP加氢反应网络中的脱氢反应均为吸热反应;PH,PY,2-MP加氢反应网络中脱氢反应的平衡转化率均存在反应温度敏感区,调节反应温度可以使各脱氢反应的平衡转化率均趋近于100%;对于加氢程度相同的稠环芳烃加氢产物,甲基支链的存在使得脱氢反应更容易进行;对于加氢程度和甲基支链数相同的稠环芳烃加氢产物,芳环数量越多,脱氢反应越容易进行;在0~2 MPa和300~800 K的反应条件下,高温低压有利于PH,PY,2-MP加氢反应网络中脱氢反应的进行。 展开更多
关键词 催化裂化油浆 2-甲基菲 加氢反应网络 Benson基团贡献法 热力学计算
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一种高效稳定的高熵合金电催化剂用于析氢反应
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作者 赵贵 路宽 +8 位作者 李玉楠 卢发贵 高朋 南兵 李丽娜 张熠霄 徐鹏涛 刘晰 陈立桅 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第7期156-165,共10页
水分解是一种利用可再生能源驱动的绿色制氢方法,零碳排放特性使其成为解决氢能源生产的重要途径.在电化学水分解中,制备高活性和稳定性的催化剂至关重要.高熵合金(HEAs)由于独特的结构和性能使其成为理想的催化剂材料,其多元成分和可... 水分解是一种利用可再生能源驱动的绿色制氢方法,零碳排放特性使其成为解决氢能源生产的重要途径.在电化学水分解中,制备高活性和稳定性的催化剂至关重要.高熵合金(HEAs)由于独特的结构和性能使其成为理想的催化剂材料,其多元成分和可调组成提供了丰富的表面活性位点和灵活的催化特性,有望提高水分解的效率并降低成本.然而,简易高效地制备HEAs仍面临挑战,且目前对HEA催化剂的结构-活性关系的了解存在不足.因此,探索一种简便有效的方法用以制备高性能HEAs催化剂,并深入理解其在水分解反应中的作用机制和结构演变,能够为未来绿色制氢技术的发展提供重要的科学基础和技术支持.本文采用了电化学测量、CuK-边和PtL3-边的原位同步辐射X射线吸收光谱(XAS)测试以及密度泛函理论(DFT)计算相结合的方法,系统地研究了高熵合金电催化剂PtPdRhRuCu/C的析氢反应(HER)活性、反应机制以及结构演变规律.PtPdRhRuCu HEAs纳米颗粒由简便的一步溶剂热法制备,直径约为6.7±0.6 nm,其合金结构和元素分布通过多种表征手段(扫描透射电子显微镜、X射线衍射和能量色散X射线光谱等)得到确认.XAS对Cu K-边和PtL3-边的分析结果显示,HEAs纳米颗粒表面的少量铜氧化物在HER过程中被还原至金属态.扩展X射线吸收精细结构的拟合结果表明,HEAs在工况HER中保持了金属态和无序的原子排列,没有新的分离相形成.电化学测试结果表明,得益于多金属活性位点,PtPdRhRuCu/C催化剂在酸性和碱性条件下均表现出较好的HER活性和耐久性.在10 m Acm^(-2)的电流密度下,该催化剂在1molL^(-1)KOH中具有23.3 m V的极低过电位,优于商业Pt/C催化剂(50.3 m V),其质量活性是Pt/C的7.9倍,达到3.0 Amg^(-1)Pt.PtPdRhRuCu的高熵效应显著提升了催化剂在HER中的长期稳定性,在稳定性测试中,PtPdRhRuCu/C催化剂在10000次循环伏安测试后几乎无性能衰减,而Pt/C的过电位增加了约24 m V.在-55 m V过电位下的30 h的HER测试中,PtPdRhRuCu/C保持95.7%的初始电流密度,而Pt/C衰减了53.6%.在酸性条件下,PtPdRhRuCu/C的循环稳定性和耐久性也优于Pt/C.DFT计算结果表明,PtPdRhRuCu/C较好的HER性能和稳定性归因于高熵合金的协同效应,多金属成分提供了多样的活性位点,优化了HER反应路径,特别是在Volmer步骤中降低了水裂解的反应能垒.PtPdRhRuCu/C上的HER过程遵循Volmer-Tafel机理,水分子优先吸附在Ru位点,促进HO-H键的解离,解离出的质子迁移到Pt上,而OH通过Ru和Rh的桥接作用而稳定,最终在Cu上释放H2.综上,本文展示了高熵合金在HER中较好的性能,并通过详细的表征深入理解了其构-效关系.研究成果为高熵合金催化剂的合理设计和应用提供理论支持,为未来高效、耐久和低成本的绿色制氢技术提供重要的科学依据和技术支持. 展开更多
关键词 析氢反应 高熵合金 原位X射线吸收光谱 一步溶剂热法 低过电位
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Lattice Boltzmann Simulation of a Gas-to-Solid Reaction and Precipitation Process in a Circular Tube
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作者 Matthew D.Lindemer Suresh G.Advani Ajay K.Prasad 《Computer Modeling in Engineering & Sciences》 SCIE EI 2018年第12期527-553,共27页
The lattice Boltzmann method(LBM)is used to simulate the growth of a solid-deposit on the walls of a circular tube resulting from a gas-to-solid reaction and precipitation process.This process is of particular interes... The lattice Boltzmann method(LBM)is used to simulate the growth of a solid-deposit on the walls of a circular tube resulting from a gas-to-solid reaction and precipitation process.This process is of particular interest for the design of reactors for the production of hydrogen by the heterogeneous hydrolysis of steam with Zn vapor in the Zn/ZnO thermochemical cycle.The solid deposit of ZnO product on the tube wall evolves in time according to the temporally-and axially-varying convective-diffusive transport and reaction of Zn vapor with steam on the solid surface.The LBM is wellsuited to solving problems with coupled flow,heat and mass transfer in a time-evolving domain.Here,a D2Q9 axisymmetric multiple-relaxation-time(MRT)lattice Boltzmann scheme is used to simulate incompressible fluid transport while a D2Q5 axisymmetric MRT lattice Boltzmann scheme is used to simulate the convective-diffusive transport of Zn vapor.The model is first validated against several analytical solutions,followed by a parametric study to understand the effect of Reynolds,Schmidt,and Damk?hler numbers on the time evolution of the ZnO deposition profile along the tube axis.The axial location of the fastest deposition is found to increase with increasing Peclet number,and decrease with increasing Damk?hler number,with no independent effect from the Schmidt number.When the reaction kinetics are assumed to increase along the tube axis due to nonisothermal tube wall temperature,a second peak in the deposition profile can be observed for sufficiently low values of Da/Pe. 展开更多
关键词 LATTICE BOLTZMANN methods REACTIVE flow heterogeneous reaction PRECIPITATION solar hydrogen production.
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电沉积法制备碱性电解水镍基析氧电极的研究进展 被引量:1
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作者 张静 贺业亨 +6 位作者 王晶晶 夏博文 赵秦峰 王延飞 余颖龙 邵晨熠 龙川 《化工进展》 EI CAS CSCD 北大核心 2023年第12期6239-6250,共12页
在“碳达峰、碳中和”的目标下,绿氢成为极具前景的清洁能源。碱性电解水制取绿氢技术商业化程度最高,但由于析氧反应(OER)动力学过程缓慢且需要较高的过电位,成为制约电解水电极效率的主要瓶颈。商业电解槽中广泛使用的镍网或泡沫镍电... 在“碳达峰、碳中和”的目标下,绿氢成为极具前景的清洁能源。碱性电解水制取绿氢技术商业化程度最高,但由于析氧反应(OER)动力学过程缓慢且需要较高的过电位,成为制约电解水电极效率的主要瓶颈。商业电解槽中广泛使用的镍网或泡沫镍电极的OER性能仍有很大提升空间,在其上复合镍基催化功能层,开发新型高活性的析氧电极有利于提高电极效率,降低制氢成本。电沉积技术具有工艺简单、条件温和、利于放大生产自支撑电极的优势,成为工业化生产OER电极的理想工艺之一。本文综述了近年来利用电沉积技术制备的镍基析氧电极并用于碱性电解水的研究进展。采用电沉积技术在镍网或泡沫镍基底上制备镍(氢)氧化物、双金属及多元金属以及非金属掺杂的镍基催化剂作为催化功能层,通过增强催化功能层的电导率及金属间的协同作用、增加活性位点数量、减小扩散路径以及改变表面原子构型等方式提高镍基自支撑电极的OER性能。最后,展望了镍基自支撑电极在电解水领域的应用,同时指出了电沉积法制备电极材料存在的挑战。 展开更多
关键词 电解 制氢 催化剂 镍基自支撑电极 析氧反应 电沉积法
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镍基磷化物结构调控及电催化性能
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作者 范爱玲 郭亚奇 +1 位作者 李瑞廷 刘一楠 《北京工业大学学报》 CAS CSCD 北大核心 2023年第9期980-989,共10页
为探究不同掺杂对镍基磷化物催化性能的影响,采用水热法制备4种不同掺杂(Fe、Co、Mo、W)的镍基前驱体,然后通过化学气相沉积法对不同前驱体磷化,得到相应的4种镍基磷化物。经SEM分析发现,不同前驱体的结构存在较大差异。磷化后,仅有NiMo... 为探究不同掺杂对镍基磷化物催化性能的影响,采用水热法制备4种不同掺杂(Fe、Co、Mo、W)的镍基前驱体,然后通过化学气相沉积法对不同前驱体磷化,得到相应的4种镍基磷化物。经SEM分析发现,不同前驱体的结构存在较大差异。磷化后,仅有NiMoP较好地保留了其前驱体的原有形貌,展示出最佳的结构稳定性。XPS分析表明:4种镍基磷化物表现出不同价态结构,Fe、Co掺杂镍基磷化物具有相似低价态结构,而Mo、W掺杂镍基磷化物具有高价电子态结构。进一步电化学析氢测试表明,NiMoP在10 mA/cm^(2)的电流密度下过电位仅为97 mV,与贵金属Pt的83 mV相近,远低于其他3种样品的过电位。同时,在长期的稳定性测试中,NiMoP也表现出比其他3种磷化物更为优良的稳定性能,表明其良好的析氢催化活性。 展开更多
关键词 镍基磷化物 价态调控 析氢反应 电解水 水热法 磷化
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二硫化钼在电催化析氢反应中的应用进展 被引量:2
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作者 张红涛 韩乔 杨占旭 《化工新型材料》 CAS CSCD 北大核心 2023年第5期49-54,共6页
氢气因清洁和可再生等优点,被认为是一种具有发展前景的清洁能源,在未来替代传统化石燃料的可再生能源体系中具有重要地位。电化学分解水是一种高效且环境友好的制氢途径,在电解水制氢技术的发展中,高效电催化析氢催化剂的作用显得尤为... 氢气因清洁和可再生等优点,被认为是一种具有发展前景的清洁能源,在未来替代传统化石燃料的可再生能源体系中具有重要地位。电化学分解水是一种高效且环境友好的制氢途径,在电解水制氢技术的发展中,高效电催化析氢催化剂的作用显得尤为重要。二硫化钼(MoS_(2))具有较低的析氢吉布斯自由能及耐酸碱腐蚀等优点,因此,MoS_(2)作为高效的电催化析氢催化剂一直是研究热点。阐述了MoS_(2)的电催化析氢机理,综述了不同形貌MoS_(2)在电催化析氢中的应用,通过对MoS_(2)电催化剂进行改性来优化其催化活性。研究表明通过改善MoS_(2)边缘位点的催化活性、增加活性位点的数量等方法能够极大地改善MoS_(2)电化学析氢过程中的催化活性。 展开更多
关键词 二硫化钼 电催化剂 活性位点 合成方法 析氢反应
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Rare earth alloy nanomaterials in electrocatalysis 被引量:1
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作者 Yifei Li Xilin Yuan +5 位作者 Ping Wang Lulin Tang Miao He Pangen Li Jiang Li Zhenxing Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期574-594,I0014,共22页
With the rapid development of society and economy, the excessive consumption of fossil energy has led to the global energy and environment crisis. In order to explore the sustainable development of new energy, researc... With the rapid development of society and economy, the excessive consumption of fossil energy has led to the global energy and environment crisis. In order to explore the sustainable development of new energy, research based on electrocatalysis has attracted extensive attention in the academic circle. The main challenge in this field is to develop nano-catalysts with excellent electrocatalytic activity and selectivity for target products. The state of the active site in catalyst plays a decisive role in the activity and selectivity of the reaction. In order to design efficient and excellent catalysts, it is an effective means to adjust the electronic structure of catalysts. Electronic effects are also called ligand effects. By alloying with rare earth(RE) elements, electrons can be redistributed between RE elements and transition metal elements, achieving accurate design of the electronic structure of the active site in the alloy. Because of the unique electronic structure of RE, it has been paid attention in the field of catalysis. The outermost shell structure of RE elements is basically the same as that of the lower shell, except that the number of electrons in the 4f orbital is different, but the energy level is similar, so their properties are very similar. When RE elements form compounds, both the f electrons in the outermost shell and the d electrons in the lower outer shell can participate in bonding. In addition, part of the 4f electrons in the third outer shell can also participate in bonding.In order to improve the performance of metal catalysts, alloying provides an effective method to design advanced functional materials. RE alloys can integrate the unique electronic structure and catalytic behavior of RE elements into metal materials, which not only provides an opportunity to adjust the electronic structure and catalytic activity of the active component, but also enhances the structural stability of the alloy and is expected to significantly improve the catalytic performance of the catalyst. From the perspective of electronic and catalytic activity, RE elements have unique electronic configuration and lanthanide shrinkage effect. Alloying with RE elements will make the alloy have more abundant electronic structure, activity, and spatial arrangement, effectively adjusting the reaction kinetics of the electrochemical process of the catalyst. In this paper, the composition,structure, synthesis of RE alloys and their applications in the field of electrocatalysis are summarized, including the hydrogen evolution reaction, the oxygen evolution reaction, the oxygen reduction reaction, the methanol oxidation reaction, the ethanol oxidation reaction, and other catalytic reactions. At the same time, the present challenges of RE alloy electrocatalytic materials are summarized and their future development direction is pointed out. In the field of electrocatalysis, the cost of catalyst is too high and the stability is not strong. Therefore, the testing process should be related to the actual application, and the test method should be standardized, so as to carry forward the field of electrocatalysis. 展开更多
关键词 Rare earth Alloy nanomaterials ELECTROCATALYSIS Preparation methods hydrogen evolution reaction Oxygen reduction reaction Methanol oxidation reaction Ethanol oxidation reaction
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金属相二硫化钼催化剂的液相制备及其析氢性能研究
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作者 任浩文 陈世宏 +2 位作者 罗春晖 赵强 闫康平 《电子元件与材料》 CAS 北大核心 2023年第6期653-658,共6页
电解水产氢被认为是未来实现可持续、清洁能源供应的一种重要方式。为了实现这一目标,开发高效、廉价的电催化剂是至关重要的。二硫化钼(MoS_(2))是一种被认为可以替代贵金属的催化剂,其具有配位不饱和的边缘活性位点和接近铂(Pt)的氢... 电解水产氢被认为是未来实现可持续、清洁能源供应的一种重要方式。为了实现这一目标,开发高效、廉价的电催化剂是至关重要的。二硫化钼(MoS_(2))是一种被认为可以替代贵金属的催化剂,其具有配位不饱和的边缘活性位点和接近铂(Pt)的氢吸附自由能。然而,由于半导体相(2H-MoS_(2))受限于自身的导电能力较差及活性位点数目较低,因此具有不同配位结构的金属相(1T-MoS_(2))被认为是更理想的电解水析氢材料,因为它表现出类似于金属的导电能力且能提供更多的催化活性位点。本研究通过简单的水热法和退火法,使用不同的酸性溶剂合成出了高达76%1T相占比的二硫化钼(MoS_(2)-A)。在电解水产氢实验中,MoS_(2)-A在0.5 mol/L的硫酸中表现出优异的电催化析氢性能,其在10 mA/cm^(2)处的过电位为324 mV,Tafel斜率为95 mV/dec。值得一提的是,在合成过程中添加了乙酸,可以在一定程度上减缓二硫化钼纳米片的团聚并促使其垂直排列,从而得到尺寸更小、能够暴露更多活性位点、具有优异电子传输能力的催化剂。这些发现表明,MoS_(2)-A在电催化析氢领域有很大的潜力,可以作为一种廉价、高效的电催化剂来降低电解水产氢的成本,并促进其商业化应用。 展开更多
关键词 析氢反应 水热法 金属相二硫化钼 电催化 电解水
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镍基磷化物在碱性电解水析氢反应中的研究进展 被引量:1
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作者 项俊欣 马昕霞 +5 位作者 吴江 许伟 戚瑜敏 郭成杰 俞金磊 刘健 《应用化工》 CAS CSCD 北大核心 2023年第9期2627-2631,共5页
主要对镍基磷化物析氢反应的催化机理和活性来源进行了探究,介绍了在不同电解液环境中的析氢反应机理以及Tafel斜率与反应过程中动力学的关系,并阐述了P原子的引入以及磷化程度对镍基磷化物活性位点和吸附能的影响;概括了镍基磷化物常... 主要对镍基磷化物析氢反应的催化机理和活性来源进行了探究,介绍了在不同电解液环境中的析氢反应机理以及Tafel斜率与反应过程中动力学的关系,并阐述了P原子的引入以及磷化程度对镍基磷化物活性位点和吸附能的影响;概括了镍基磷化物常见的合成方法和磷源,以及对形貌调控、掺杂、界面工程等不同改性方法进行了论述,深入分析了镍基磷化物改性后具有良好析氢性能的原因,最后根据镍基磷化物目前在析氢反应中存在的问题提出了发展方向。 展开更多
关键词 镍基磷化物 碱性电解水 改性方法 析氢反应
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HER单原子电催化剂的载体构建与性能研究进展 被引量:1
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作者 薛莲 孙豪 +2 位作者 程薇 陈效贤 姚伟峰 《中国材料进展》 CAS CSCD 北大核心 2023年第3期249-259,共11页
单原子催化剂(single atom catalysts,SACs)由于其高催化活性、良好稳定性等优点,在电化学领域得到广泛研究。单原子催化剂不仅提供了研究催化反应机理的新见解与思路,还在均相与非均相催化反应连接方面起到了重要的作用。为了减少单原... 单原子催化剂(single atom catalysts,SACs)由于其高催化活性、良好稳定性等优点,在电化学领域得到广泛研究。单原子催化剂不仅提供了研究催化反应机理的新见解与思路,还在均相与非均相催化反应连接方面起到了重要的作用。为了减少单原子催化剂在合成过程中出现聚集、原子利用率低等问题,总结和归纳了单原子催化剂的载体并介绍了单原子催化剂的合成方法;介绍了电催化析氢反应(hydrogen evolution reaction,HER)的机理;对于电催化析氢反应,重点介绍了Pt、Pd、Ru、Co、Mo、Ni金属单原子,单原子合金和非金属单原子在内的单原子催化剂的催化活性,并分析了其电催化性能提高的原因。结果表明,单原子催化剂的制备已经实现了从贵金属单原子催化剂向非贵金属单原子催化剂的演变。最后,还对单原子催化剂研究存在的问题进行了分析,并对单原子催化剂的发展前景做了展望。 展开更多
关键词 单原子催化剂 载体 合成方法 析氢反应机理 电催化
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MoS_(2)/CNTs电催化析氢性能探究
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作者 段孟言 窦生艳 +2 位作者 魏清渤 昝灵兴 张红玲 《化学工程师》 CAS 2023年第2期13-16,共4页
本文通过一步水热法成功实现了二硫化钼(MoS_(2))在碳纳米管(CNTs)内外壁的原位生长,形成了限域和非限域的MoS_(2)/CNTs复合纳米材料,并探究了其对电化学析氢反应(HER)的催化活性。研究结果表明,在碳纳米管内外壁均原位生长出二维片状Mo... 本文通过一步水热法成功实现了二硫化钼(MoS_(2))在碳纳米管(CNTs)内外壁的原位生长,形成了限域和非限域的MoS_(2)/CNTs复合纳米材料,并探究了其对电化学析氢反应(HER)的催化活性。研究结果表明,在碳纳米管内外壁均原位生长出二维片状MoS_(2)纳米材料,形成部分限域的MoS_(2)/CNTs纳米材料。此外,电催化析氢性能测试显示,MoS_(2)生长在适量的CNTs(~25mg)时,形成的MoS_(2)/CNTs复合纳米材料表现出较强的HER活性和稳定性。在10mA·cm^(-2)时,HER的过电位为440mV。Tafel斜率为117mV·dec^(-1)。 展开更多
关键词 水热法 限域 纳米材料 电催化 析氢反应
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One-pot molten salt method for constructing CdS/C_(3)N_(4) nanojunctions with highly enhanced photocatalytic performance for hydrogen evolution reaction 被引量:3
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作者 Weijia Zhao Hongyun Niu +3 位作者 Yongliang Yang Hongzhou Lv Jungang Lv Yaqi Cai 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2022年第2期244-257,共14页
The construction of heterojunction photocatalysts for efficiently utilizing solar energy has attracted considerable attention to solve the energy crisis and reduce environmental pollution.In this study,we use the ener... The construction of heterojunction photocatalysts for efficiently utilizing solar energy has attracted considerable attention to solve the energy crisis and reduce environmental pollution.In this study,we use the energy released from an easily-occurred exothermic chemical reaction to serve as the drive force to trigger the formation of Cd S and C_(3)N_(4) nanocomposites which are successfully fabricated with cadmium nitrate and thiourea without addition of any solvents and protection of inert gas at initial temperature,a little higher than the melting point of thiourea.The as-prepared Cd S/C_(3)N_(4) materials exhibit high efficiency for photocatalytic hydrogen evolution reaction(HER)with the HER rate as high as 15,866μmol/(g·hr)under visible light irradiation(λ>420 nm),which is 89 and 9 times those of pristine C_(3)N_(4) and Cd S,respectively.Also,the apparent quantum efficiency(AQE)of Cd S/C_(3)N_(4)–1:2–200–2(Cd S/C_(3)N_(4)–1:2–200–2 means the ratio of Cd to S is 1:2 and the reaction temperature is set at 200℃ for two hours)reaches 3.25%atλ=420±15 nm.After irradiated for more than 24 hr,the HER efficiencies of Cd S/C_(3)N_(4) do not exhibit any attenuation.The DFT calculation suggests that the charge difference causes an internal electric field from C_(3)N_(4) pointing to Cd S,which can more effectively promote the transfer of photogenerated electrons from Cd S to C_(3)N_(4).Therefore,most HER should occur on C_(3)N_(4) surface where photogenerated electrons accumulate,which largely protects Cd S from photo-corrosion. 展开更多
关键词 One-pot molten salt method Cd S/C_(3)N_(4)nanojunctions Photocatalytic hydrogen evolution reaction Anti-photo-corrosion DFT calculation
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碳化钼基析氢反应电催化剂的制备及改性研究进展
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作者 许邵帅 崔文静 +2 位作者 白杰 李春萍 孙兴伟 《功能材料》 CAS CSCD 北大核心 2023年第12期12056-12067,共12页
碳化钼(Mo_(2)C)因其与铂(Pt)相似的d带电子结构、宽pH适用性、易于合成、低成本等优势,成为一种很有前途的电催化剂。然而,纯Mo_(2)C存在导电性差、界面反应动力学慢、Mo-H结合能太强等缺陷。近年来,许多研究报道了改性Mo_(2)C基催化... 碳化钼(Mo_(2)C)因其与铂(Pt)相似的d带电子结构、宽pH适用性、易于合成、低成本等优势,成为一种很有前途的电催化剂。然而,纯Mo_(2)C存在导电性差、界面反应动力学慢、Mo-H结合能太强等缺陷。近年来,许多研究报道了改性Mo_(2)C基催化剂来提升其电催化析氢性能,基于此,综述了Mo_(2)C常用的制备工艺以及提高Mo_(2)C析氢性能的各种不同改性策略,深入分析了不同改性方式对Mo_(2)C析氢性能提高的内在原因。最后,提出了Mo_(2)C基电催化剂目前面临的挑战和未来的发展方向。 展开更多
关键词 碳化钼 制备工艺 改性策略 电催化 析氢反应
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铂/铜合金催化剂的制备及其电解水析氢性能研究
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作者 李艳 杨振峰 +1 位作者 樊月瑶 张小婷 《人工晶体学报》 CAS 北大核心 2023年第8期1500-1508,共9页
面对化石能源危机问题,清洁高效的氢能源受到人们的广泛关注,电解水制氢成为新的研究热点。本文主要围绕铂/铜合金催化剂的合成、表征及其电解水析氢催化应用展开研究。采用溶剂热法合成铂/铜合金,通过XRD、SEM、TEM、EDS、XPS等表征铂... 面对化石能源危机问题,清洁高效的氢能源受到人们的广泛关注,电解水制氢成为新的研究热点。本文主要围绕铂/铜合金催化剂的合成、表征及其电解水析氢催化应用展开研究。采用溶剂热法合成铂/铜合金,通过XRD、SEM、TEM、EDS、XPS等表征铂/铜合金的组成结构和微观形貌,对铂/铜合金的构效关系进行探索。利用电化学测试系统测得铂/铜合金不同条件下的析氢催化性能。在0.5 mol/L H_(2)SO_(4)中,铂/铜合金的起始过电位为20.3 mV(10 mA·cm^(-2)时),塔菲尔斜率为37.56 mV·dec^(-1);在1 mol/L磷酸缓冲盐溶液(PBS)中,铂/铜合金的起始过电位为35.0 mV(10 mA·cm^(-2)时),塔菲尔斜率为52.12 mV·dec^(-1);在1 mol/L KOH中,铂/铜合金的起始过电位为25.3 mV(10 mA·cm^(-2)时),塔菲尔斜率为36.82 mV·dec^(-1)。对比发现,铂/铜合金在酸性电解质中展现出更为优异的催化性能。而且,进一步实验表明铂/铜合金催化剂在酸性电解质中具有高的电催化活性面积(30.83 cm^(2))和良好的循环稳定性。 展开更多
关键词 催化剂 铂/铜合金 溶剂热法 电解水 析氢反应
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Anchoring Ru clusters to highly defective N-doped carbon nanotubes via a thermal-shock strategy for stable industrial hydrogen evolution
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作者 Zhiming Li Xinyu Li +5 位作者 Haiqing Ma Chenliang Ye Hongan Yu Long Nie Meng Zheng Jin Wang 《Nano Research》 SCIE EI CSCD 2024年第6期5261-5269,共9页
Non-Pt or low-Pt catalysts capable for stable generation of hydrogen via water electrolysis at an industrial level of current density are highly demanded.Construction of strong metal-support connection is beneficial t... Non-Pt or low-Pt catalysts capable for stable generation of hydrogen via water electrolysis at an industrial level of current density are highly demanded.Construction of strong metal-support connection is beneficial to improve the performance stability of electrocatalysts.Here we employed highly defective N-doped carbon nanotubes(d-N-CNT)as the support to achieve uniform and firm anchoring of Ru clusters(~1.9 nm)via a thermal-shock strategy.The as-prepared Ru/d-N-CNT catalyst shows excellent catalytic activity for hydrogen evolution reaction(HER)in alkaline media and requires an overpotential(ƞ)of 12 mV at 10 mA·cm^(−2)and 116 mV at 200 mA·cm^(−2)with a Ru loading of 0.025 mg·cm^(−2).Impressively,Ru/d-N-CNT presents robust stability for HER at both low current density(stable for at least 1000 h at 10 mA·cm^(−2))and the industrial level of current density(stable for at least 100 h at 1000 mA·cm^(−2)),remarkably outperforming commercial Pt/C and Ru/C.The highly defective nature of the N-CNT support endowed the as-prepared Ru/d-N-CNT catalyst with strong metal-support adhesion that efficiently suppressed agglomeration as well as obscission of Ru clusters.Meanwhile,the rich defects increased the surface energy of the N-CNT support and resulted in improved hydrophilicity as evidenced by the liquid contact angle measurement and the bubble evolution process,which also played an important role in stabilizing the HER performance especially at large current density. 展开更多
关键词 thermal-shock method hydrogen evolution reaction large-current-density Ru cluster
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Enhanced hydrogen evolution performance by 3D ordered macroporous Ru-CoP@NC electrocatalysts
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作者 Chen-Chen Zhang Sheng Wei +6 位作者 Li-Xian Sun Yi-Fang Ouyang Fen Xu Hai-Liang Chu Hong-GePan Li-Xin Chen Xue-Zhang Xiao 《Rare Metals》 SCIE EI CAS CSCD 2024年第3期1095-1107,共13页
Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel cells.However,the main challenge is... Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel cells.However,the main challenge is to develop high performance,low cost and chemically stable electrocatalysts to decline the energy barriers and enhance the sluggish kinetics of hydrogen evolution reaction(HER).Herein,a three-dimensional hierarchically ordered macroporous Ru-CoP@NC electrocatalyst(3DOM Ru-CoP@NC)derived from ordered macro-microporous metal-organic frameworks has been prepared using the precursor@template and double-solvent methods.The prepared 3DOM Ru-CoP@NC catalyst exhibits an overpotential of 15 mV(j=10 mA·cm^(-2))and a reaction Tafel slope of 38 mV·dec^(-1)in alkaline electrolyte,which are superior to commercial Pt@C catalyst.Additionally,the overpotential and reaction Tafel slope of this catalyst in acidic media are 45 mV and 50 mV·dec^(-1),respectively.The outstanding HER activities of 3DOM Ru-CoP@NC catalysts are ascribed to the 3D highly interconnectedreticular nanospaces that can increase effective reaction active sites.The N dope d carbon framework improves the electronic properties and conductivity.Moreover,the strong interaction of Ru and CoP nanoparticles also boosts the HER process.These results indicate that 3DOM Ru-CoP@NC catalysts with high catalytic activities have a broad application prospect in the future. 展开更多
关键词 hydrogen evolution reaction Template method 3D ordered macroporous Ru-CoP@NC
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综合实验设计:NiFe LDH/TiO_(2)的制备及电解水性能测试
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作者 杜晓航 刘桂华 +3 位作者 刘晓静 李天航 武兰兰 李敬德 《广州化工》 CAS 2023年第2期296-300,共5页
设计介绍了一个包括NiFe LDH/TiO_(2)纳米片制备及其析氢、析氧反应电催化活性评价的综合性电化学实验。通过开展本实验,学生能够学习利用电化学沉积方法制备电催化剂的技术;初步掌握利用循环伏安、塔菲尔曲线等电化学测试技术对析氧、... 设计介绍了一个包括NiFe LDH/TiO_(2)纳米片制备及其析氢、析氧反应电催化活性评价的综合性电化学实验。通过开展本实验,学生能够学习利用电化学沉积方法制备电催化剂的技术;初步掌握利用循环伏安、塔菲尔曲线等电化学测试技术对析氧、析氢反应活性进行评价的方法;理解电解水制氢过程中涉及到的基本理论知识。本实验将引导学生关注绿色可再生能源的开发及应用,提升学生分析解决科研问题的能力和基本素养。 展开更多
关键词 析氢反应 析氧反应 电化学沉积法 电化学测试 实验设计
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NiO/NF纳米催化电极的组织结构与析氢性能
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作者 刘雪华 伍浩轩 李学发 《厦门理工学院学报》 2023年第1期72-77,共6页
为研究不同制备方法对NiO/NF(nickle foam,泡沫镍)电极组织结构和电催化析氢性能的影响规律,分别采用水热法、热分解法和微乳液法,成功制备出不同形貌特征的NiO/NF电催化析氢电极,对其组织结构进行XRD和SEM表征,并采用电化学方法研究其... 为研究不同制备方法对NiO/NF(nickle foam,泡沫镍)电极组织结构和电催化析氢性能的影响规律,分别采用水热法、热分解法和微乳液法,成功制备出不同形貌特征的NiO/NF电催化析氢电极,对其组织结构进行XRD和SEM表征,并采用电化学方法研究其电催化性能。实验结果表明:3种方法所制备产物的相组成物均为泡沫镍基底Ni和NiO;不同制备方法所获得产物的微观几何结构有较大差别,水热法所制备的NiO为纳米棒状,微乳液法制备的NiO呈现褶皱薄膜状,热分解法制备的则为不规则薄膜。相应地,3种方法制备试样的电化学性能也不同。其中,性能最佳试样由微乳液法制备,其显微形貌呈现均匀的褶皱薄膜状,提供了更多的活性位点。表明不同方法可获得不同组织结构的NiO/NF电极,几何结构优良的电极具有更大的比表面积,可提供较多的活性位点,故具备更佳的电催化析氢性能。 展开更多
关键词 NiO/NF电极 电催化析氢 制备方法 构效关系
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