纳米晶纯和掺Li2O CoO/Mn2O3体系的表面和催化性能

G. El-Shobaky, M. Shouman, S. M. Ibrahim
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引用次数: 2

摘要

采用x射线衍射(XRD)研究了煅烧温度(350 ~ 700℃)和掺杂Li2O (0.75 ~ 4.5 mol%)对CoO/Mn2O3固-固相互作用、表面和催化性能的影响,在-196℃进行了N2吸附,在180 ~ 280℃进行了异丙醇转化。结果表明,从350℃开始,纯固体和掺杂固体之间发生固-固相互作用,生成钴锰氧化物(Co,Mn) (Co,Mn)2O4相。随着煅烧温度的升高,所得相的结晶度和晶粒尺寸逐渐增大,但仍为15 ~ 33 nm的纳米晶相。所研究的体系中掺杂Li2O使所制相的晶粒尺寸减小。掺杂过程降低了体系的比表面积,在500℃和700℃煅烧的固体中,当Li2O浓度为4.5 mol%时,体系的比表面积分别降低了33%和32%。Li2O的掺入有效地增加了总孔体积,其中掺入4.5 mol%的Li2O后,在500℃和700℃煅烧后,总孔体积分别增加了57%和27%。纯体系的孔体积分布较宽,而掺杂固体的孔体积分布曲线呈多模态。纯固体和各种掺杂固体作为脱氢催化剂只产生丙酮。当煅烧温度从350℃增加到400℃时,活性增加,超过该温度后活性降低。在500°C和700°C下进行的掺杂过程大大提高了催化活性。在280°C时,当Li2O浓度为4.5 mol%时,500°C和700°C煅烧的固体的催化活性分别提高了45%和94%。在350°C和700°C范围内提高煅烧温度以及掺杂不同量的Li2O都没有改变催化反应的机理。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Surface and Catalytic Properties of Nanocrystalline Pure and Li2O - Doped CoO/Mn2O3 System
The effects of calcination temperature (350 - 700°C) and Li2O - doping (0.75 - 4.5 mol%) on solid - solid inter- action, surface and catalytic properties of CoO/Mn2O3 were investigated using XRD, N2 adsorption at -196oC and isopro- panol conversion carried out at 180 - 280°C using a flow method. The results obtained revealed that solid - solid interac- tion between pure and doped - solids took place at temperatures starting from 350°C to yield cobalt manganese oxide (Co, Mn) (Co,Mn)2O4 phase. The degree of crystallinity and crystallite size of the produced phase increased progressively as a function of calcination temperature but still remained as nanocrystalline phase 15 - 33 nm. Li2O - doping of the system in- vestigated decreased the crystallite size of the produced phase. The doping process decreased the specific surface area of the system investigated, the decrease attained 33% and 32% in presence of 4.5 mol% Li2O in solids calcined at 500 and 700oC, respectively. Li2O - doping exerted an effective increase in total pore volume, the increase reached 57% and 27% by doping with 4.5 mol% Li2O followed by calcination at 500 and 700, respectively. Pure system showed a broad pore volume distribution while the doped solids exhibited multimodal pore volume distribution curves. Pure and variously doped solids acted as dehydrogenation catalysts yielding only acetone. The activity increased by increasing the calcina- tions temperature from 350°C to 400°C, then decreased upon increasing the calcinations temperature above this limit. The doping process carried out at 500°C and 700°C much increased the catalytic activity. The maximum increase in the cata- lytic activity, measured at 280°C, in presence of 4.5 mol% Li2O attained 45 and 94% for the solids calcined at 500°C and 700°C, respectively. The increase in calcination temperature within 350°C and 700°C and doping with different amounts of Li2O did not change the mechanism of the catalyzed reaction.
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