Mauricio Musso, Santiago Veiga, Angie Quevedo, Juan Bussi
{"title":"锆酸钇负载镍基催化剂催化氨分解制氢研究","authors":"Mauricio Musso, Santiago Veiga, Angie Quevedo, Juan Bussi","doi":"10.1016/j.ijhydene.2025.150599","DOIUrl":null,"url":null,"abstract":"<div><div>Ammonia (NH<sub>3</sub>) decomposition to produce hydrogen (H<sub>2</sub>) 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 H<sub>2</sub> and N<sub>2</sub> 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, N<sub>2</sub> 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 NH<sub>3</sub> and H<sub>2</sub> 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 NH<sub>3</sub> adsorption on the denser and bulkier structure. On the other hand, the increase in the Y:Zr ratio also improves the resistance towards H<sub>2</sub> poisoning, due to a higher number of oxygen vacancies, and mitigates the active phase sintering effect.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"159 ","pages":""},"PeriodicalIF":8.3000,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydrogen production through catalytic ammonia decomposition using Ni-based catalysts supported on yttrium zirconate\",\"authors\":\"Mauricio Musso, Santiago Veiga, Angie Quevedo, Juan Bussi\",\"doi\":\"10.1016/j.ijhydene.2025.150599\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Ammonia (NH<sub>3</sub>) decomposition to produce hydrogen (H<sub>2</sub>) 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 H<sub>2</sub> and N<sub>2</sub> 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, N<sub>2</sub> 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 NH<sub>3</sub> and H<sub>2</sub> 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 NH<sub>3</sub> adsorption on the denser and bulkier structure. On the other hand, the increase in the Y:Zr ratio also improves the resistance towards H<sub>2</sub> poisoning, due to a higher number of oxygen vacancies, and mitigates the active phase sintering effect.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":\"159 \",\"pages\":\"\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2025-07-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Hydrogen Energy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0360319925035980\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Hydrogen Energy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0360319925035980","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
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.
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.