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用于氨分解的镍镁铝水滑石衍生催化剂——从前体到有效催化剂

Ni-Mg-Al Hydrotalcite-Derived Catalysts for Ammonia Decomposition-From Precursor to Effective Catalyst.

作者信息

Kowalczyk Andrzej, Zaryczny Martyna, Piwowarska Zofia, Chmielarz Lucjan

机构信息

Faculty of Chemistry, Jagiellonian University, Gronostajowa 2, 30-387 Kraków, Poland.

出版信息

Molecules. 2025 Feb 25;30(5):1052. doi: 10.3390/molecules30051052.

Abstract

A series of Ni-Mg-Al hydrotalcite-derived mixed metal oxides with different Ni/Mg ratios were prepared by the coprecipitation method followed by calcination at 600 °C. The hydrotalcite-like materials, as well as their calcined forms, were characterized with respect to structure (XRD, UV-Vis DRS), chemical composition (ICP-OES), textural parameters (low-temperature N sorption), dispersion of nickel species (H-chemisorption) and nickel species reducibility (H-TPR). Moreover, the process of hydrotalcite-like materials' thermal transformation to mixed metal oxide systems in air and argon flow was studied by the TG-DTA method. The activity of the studied catalysts in the reaction of ammonia decomposition increased with an increase in nickel content in the samples. It was shown that nickel species incorporated into the Mg-Al oxide matrix segregated under conditions of reduction in a flow of H/Ar mixture with the formation of metallic nickel crystallites of the average size of about 10 nm. The size of nickel crystallites was practically no change in the subsequent reduction cycles and resulted in increased catalytic activity in comparison to larger crystallites of metallic nickel (20.2-23.6 nm) deposited on AlO and MgO.

摘要

通过共沉淀法制备了一系列具有不同镍/镁比的镍-镁-铝水滑石衍生的混合金属氧化物,并在600℃下煅烧。对类水滑石材料及其煅烧形式进行了结构(XRD、紫外-可见漫反射光谱)、化学成分(电感耦合等离子体发射光谱)、织构参数(低温氮吸附)、镍物种分散度(氢化学吸附)和镍物种还原度(氢程序升温还原)等方面的表征。此外,采用热重-差示热分析方法研究了类水滑石材料在空气和氩气流中热转化为混合金属氧化物体系的过程。所研究催化剂在氨分解反应中的活性随样品中镍含量的增加而提高。结果表明,掺入镁-铝氧化物基体中的镍物种在氢/氩混合气流还原条件下发生偏析,形成平均尺寸约为10nm的金属镍微晶。镍微晶的尺寸在随后的还原循环中基本不变,与沉积在氧化铝和氧化镁上的较大金属镍微晶(20.2-23.6nm)相比,催化活性有所提高。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c1ed/11901857/2d144830f0a0/molecules-30-01052-g001.jpg

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