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晶格匹配的异质结构用于电催化水解离制氢能
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作者 宋少青 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2023年第10期31-33,共3页
氢气具有高燃烧热、无污染等特点,是替代化石燃料的理想能源.电催化水分解为高纯度氢气被认为是一种很有前途的方法.电催化分解水的关键是开发高性能、低成本的电催化剂.铂基电催化剂在酸性和碱性介质中都表现出良好的电催化活性,但经... 氢气具有高燃烧热、无污染等特点,是替代化石燃料的理想能源.电催化水分解为高纯度氢气被认为是一种很有前途的方法.电催化分解水的关键是开发高性能、低成本的电催化剂.铂基电催化剂在酸性和碱性介质中都表现出良好的电催化活性,但经济成本限制了其进一步应用.近期研究表明,由过渡金属基材料组成的异质结构电催化剂也表现出高效电催化析氢的潜力.异质结构电催化剂的晶格匹配程度影响其界面电子结构,进而决定了析氢反应的动力学和活性.因此,开发用于析氢反应的晶格匹配异质结构电催化剂的构建方法具有重要意义,也颇具挑战性.为了解决上述问题,李炫华教授课题组及合作者报道了一种梯度加热外延生长方法,采用该方法制备了晶格匹配良好的MO_(2)C-MO_(2)N异质结构电催化剂,并用于高效制氢(Angew.Chem.Int.Ed.,2022,61,e202209703).NH3状态温度图和密度泛函理论结果表明,NH3分子被吸附在MO_(2)C的(101)面上,作为MO_(2)N的成核位点.通过调节加热过程,可使吸附的NH3分子从不稳定的物理吸附转化为化学吸附,有效地调节了MO_(2)N的成核和生长过程,避免MO_(2)C和MO_(2)N之间的晶格失配,使得电导率增加2.5倍,电化学活性面积增加1.7倍.MO_(2)C-MO_(2)N晶格匹配良好的异质界面,电子从MO_(2)C传输到MO_(2)N,MO_(2)C-MO_(2)N的费米能级接近Mo位点的费米能级,电子转移到Mo活性位点,而Mo位点具有较低的氢吸附自由能,促进了H*的吸附和解吸行为.同时,考察了MO_(2)C-MO_(2)N异质结构电催化剂电催化水分解反应过程中的过渡态、吸附能、中间产物以及相应能垒下的可能反应途径.H_(2)O分解过程包括:H_(2)O首先在催化剂表面发生吸附和活化,然后解离成H*和OH*并转化为H*或OH–,最后以较低的反应吉布斯自由能实现H2析出.除了晶格匹配的异质界面电催化剂的设计外,电催化体系的构建也对电催化活性起着重要作用.典型的电催化水分解系统通常在液相水下工作,液相水具有很高的析氢传输阻力,不利于反应进行.文章作者将太阳能引入电催化系统,并以表面碳化木材、Ti泡沫、MO_(2)C-MO_(2)N、Nafion膜和IrO_(2)为原材料合理设计了光热电催化水蒸气裂解装置,实现了电催化水蒸气裂解制氢.具体过程如下:将表面碳化木材作为蒸汽发生器,在光照射下通过光热蒸腾效应将液态水转化为水蒸气,由于其强大的光收集能力和固有的多孔结构,可使太阳能蒸汽转化效率达到67.2%;将MO_(2)C-MO_(2)N和IrO_(2)作为阴极和阳极负载在Ti泡沫上,并采用Nafion膜进行阳极到阴极的质子传输.通过上述策略设计巧妙的催化装置晶格匹配良好,MO_(2)C-MO_(2)N表现出与商业Pt/C相当的催化性能,并且连续反应150 h后稳定性没有衰减.综上,文章提出了一种调节异质结构电催化剂界面晶格匹配度的新方法,为晶格匹配电催化剂的设计提供了依据;同时,作者设计的高效生产H2电催化水蒸气裂解装置为其他采用各种原位表征技术的光热辅助催化系统的开发提供了参考. 展开更多
关键词 电催化装置 水解离 产氢 异质结构 晶格匹配
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白钨矿选矿废水絮凝-电催化氧化装置应用 被引量:2
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作者 刘谊兵 《现代矿业》 CAS 2019年第2期220-221,224,共3页
针对白钨选矿废水难以沉降、分解的问题,为提高回水利用率,提出了一种利用絮凝-电催化氧化原理处理白钨矿选矿废水的方法和装置,并以西北某白钨矿选矿废水为对象进行降解试验。结果表明,絮凝-电催化氧化装置电絮凝装置沉降槽通电2 h,1~... 针对白钨选矿废水难以沉降、分解的问题,为提高回水利用率,提出了一种利用絮凝-电催化氧化原理处理白钨矿选矿废水的方法和装置,并以西北某白钨矿选矿废水为对象进行降解试验。结果表明,絮凝-电催化氧化装置电絮凝装置沉降槽通电2 h,1~#调浆槽调整废水pH值为2,电导率为900 us/cm;电催化装置电解槽通电4 h,废水COD去除率和悬浮物去除率分别高达89.0%和88.0%,净化效果明显,可提高回水利用率。 展开更多
关键词 絮凝-催化氧化装置 PH值 时间 白钨选矿废水
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电催化氧化处理市政污水的实验研究 被引量:3
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作者 潘宇 李立新 孙彩玉 《黑龙江科技大学学报》 2022年第2期198-200,209,共4页
为将市政污水厂排放标准提升至准Ⅳ类标准,以东营市某市政污水处理厂生化出水为研究对象,构建了处理量为1 m^(3)/h的电催化氧化实验装置,考察不同电流密度下其对市政污水的处理效果及运行的稳定性。研究结果表明,提高电流密度能够增强... 为将市政污水厂排放标准提升至准Ⅳ类标准,以东营市某市政污水处理厂生化出水为研究对象,构建了处理量为1 m^(3)/h的电催化氧化实验装置,考察不同电流密度下其对市政污水的处理效果及运行的稳定性。研究结果表明,提高电流密度能够增强电催化氧化处理效果。考虑运行的经济性,确定最优电流密度为5 mA/cm^(2),电催化氧化装置出水COD和NH^(+)_(4)-N的质量浓度可分别稳定在23~29 mg/L和0.8~1.4 mg/L之间。 展开更多
关键词 污水处理 催化氧化装置 化学需氧量 NH^(+)_(4)-N
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EC型压载水处理装置TRO机舱布置
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作者 肖涛 陈雄剑 《广船科技》 2023年第3期18-20,共3页
某型船的技术规格书要求:取样监测单元(TRO)需布置在安全区域机舱处所。而国内和国外没有这种布置型式,为满足市场要求,特设计此种布置。
关键词 催化型(EC)压载水处理装置 取样监测单元(TRO) 机舱布置
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Influence of Crystal Size of USY Zeolite on Performance of Hydro-upgrading Catalysts
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作者 Wang Fucun Zhu Jinling Yan Zifeng 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS 2012年第1期32-36,共5页
The effect of crystal size of USY zeolite on the performance of hydro-upgrading catalysts for treating catalytically cracked(FCC) LCO(light cycle oil) was studied.Three W-Ni catalysts supported on USY zeolites with di... The effect of crystal size of USY zeolite on the performance of hydro-upgrading catalysts for treating catalytically cracked(FCC) LCO(light cycle oil) was studied.Three W-Ni catalysts supported on USY zeolites with different crystal sizes and Al2O3 were prepared by impregnation method.The catalysts were characterized by XRD and BET methods,and evaluated in a micro-reactor using tetralin as the model compound and in an 100-mL hydrogenation test unit using FCC LCO as the feedstock.By contrast,catalyst made from smaller crystal-size USY zeolite had higher external surface area and shorter pore length,having more hydrogenation activity sites and short contact time of reactant molecules with acidity sites.The evaluation results showed that the catalyst prepared on the basis of small crystal-size USY zeolite had higher tetralin conversion and better hydro-upgrading performance for treating FCC LCO. 展开更多
关键词 crystal size USY hydro-upgrading catalyst
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Electron Beam Application for Regeneration of Catalysts Used in Refinery Cracking Units
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作者 Femando Mantovani Kondo Celina Lopes Duarte +2 位作者 Ivone Mulako Sato Vera Lucia Ribeiro Salvador Wilson Aparecido Parejo Calvo 《Journal of Physical Science and Application》 2016年第3期11-19,共9页
A catalyst is a substance that alters the rate of a reaction. The process of catalysis is essential to the modem day manufacturing industry, mainly in FCC (Fluid Catalytic Cracking) process units. However, long-term... A catalyst is a substance that alters the rate of a reaction. The process of catalysis is essential to the modem day manufacturing industry, mainly in FCC (Fluid Catalytic Cracking) process units. However, long-term exploitation of oil and gas processing catalysts leads to formation of carbon- and sulfur-containing structures of coke and dense products on the catalyst surface. They block reactive catalyst sites and reduce the catalytic activity. The main advantage of radiation processing by EB (electron beam) and gamma rays is chain cracking reaction in crude oil. Otherwise, under exposure to ionize radiation, considerable structure modification of equilibrium silica-alumina catalyst from FCC process may occur, in addition to the removal of impurities. The conditions applied in the irradiation range (20-150 kGy) of gamma rays and EB were not sufficient to alter the structure of the catalyst, whether for removal of the contaminant nickel, a major contaminant of the FCC catalyst, either to rupture of the crystalline structure either for the future reutilization of chemical elements. ATR-FTIR (Attenuated Total Reflectance-Fourier Transform Infrared Spectroscopy and EDXRFS (Energy Dispersive X-Ray Fluorescence Spectrometry) analysis were used to characterize and evaluate effects of radiation processing on equilibrium catalysts purification. To evaluate and comprehend the reactive catalyst sites, SEM (Scanning Electron Microscopy) and particle size distribution analyses were carried out. 展开更多
关键词 EB gamma rays FCC process regeneration of catalysts silica-alumina catalyst.
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Electrochemical water oxidation by photo-deposited cobalt-based catalyst on a nano-structured TiO_(2) electrode 被引量:1
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作者 LI Lin SUN LiCheng 《Science China Chemistry》 SCIE EI CAS 2012年第9期1976-1981,共6页
A cobalt-based catalyst was directly photo-deposited on the surface of a widely used n-type nano-structured semiconductor(TiO_(2)).Different thicknesses of the TiO 2 films as well as different time of photo-deposition... A cobalt-based catalyst was directly photo-deposited on the surface of a widely used n-type nano-structured semiconductor(TiO_(2)).Different thicknesses of the TiO 2 films as well as different time of photo-deposition of the Co-based catalyst on TiO_(2) films have been optimized.It was found that the electrode with 3 layers of TiO_(2) film(in 8 m thickness) and 1 hour photo-deposition of the cobalt-based catalyst by light irradiation from a 500 W Xenon lamp gave the highest current density(~5 mA/cm^(2)).Using this cobalt-modified TiO_(2) film as a working electrode in an electrochemical device,highly efficient water oxidation has been demonstrated in a pH 7.0 aqueous solution with low overpotential. 展开更多
关键词 artificial photosynthesis electrochemical water oxidation cobalt-based catalyst photo-deposition water splitting
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