锆酸钇负载镍基催化剂催化氨分解制氢研究

IF 8.3 2区 工程技术 Q1 CHEMISTRY, PHYSICAL
Mauricio Musso, Santiago Veiga, Angie Quevedo, Juan Bussi
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引用次数: 0

摘要

氨(NH3)分解生成氢(H2)似乎是解决氢储存和运输相关挑战的一个有希望的替代方案。尽管如此,还需要基于非贵金属的高活性催化剂来将其转化为H2和N2。本文采用溶胶-凝胶法制备了一系列以锆酸钇为载体的镍基催化剂,采用x射线衍射、N2吸附-解吸等温线、热重分析、扫描电镜、程序升温还原、循环伏安法和傅里叶变换红外光谱等技术对催化剂进行了表征,并在350-700℃的氨分解反应中进行了测试。计算了NH3和H2的表观活化能和反应级数。Ni含量(10%、15%和20%)和支架上的Y:Zr比(1:1和2:1)也是实验变量。对于Y:Zr比为1:1的催化剂,其催化性能随Ni含量的增加而提高,但表观活化能没有明显变化。当Y:Zr比由1:1增加到2:1时,由于抑制了NH3在较致密和较大体积结构上的吸附,表观活化能略高。另一方面,Y:Zr比的增加也提高了对H2中毒的抵抗力,因为氧空位数量增加,并且减轻了活性相烧结效应。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Hydrogen production through catalytic ammonia decomposition using Ni-based catalysts supported on yttrium zirconate
Ammonia (NH3) decomposition to produce hydrogen (H2) appears as a promising alternative to address the challenges linked to hydrogen storage and transportation. Nonetheless, highly active catalysts based on non-noble metals for its reconversion into H2 and N2 are also needed. In this work, a series of Ni-based catalysts supported on yttrium zirconate were prepared by a sol-gel technique, characterized by several techniques (X-ray diffraction, N2 adsorption-desorption isotherms, thermogravimetric analysis, scanning electron microscopy, temperature programmed reduction and cyclic voltammetry and Fourier-transform infrared spectroscopy) and tested in the ammonia decomposition reaction in the range of 350–700 °C. Apparent activation energies and reaction orders for NH3 and H2 were calculated. Ni content (10 %, 15 % and 20 %) and the Y:Zr ratio on the support (1:1 and 2:1) were also experimental variables. For the catalysts with Y:Zr ratio equal 1:1, the catalytic performance rises with the Ni content without significant changes in the apparent activation energy. An increase in the Y:Zr ratio from 1:1 to 2:1 leads to a slightly higher apparent activation energy due to an inhibition of the NH3 adsorption on the denser and bulkier structure. On the other hand, the increase in the Y:Zr ratio also improves the resistance towards H2 poisoning, due to a higher number of oxygen vacancies, and mitigates the active phase sintering effect.
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来源期刊
International Journal of Hydrogen Energy
International Journal of Hydrogen Energy 工程技术-环境科学
CiteScore
13.50
自引率
25.00%
发文量
3502
审稿时长
60 days
期刊介绍: The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc. The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.
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