{"title":"稀土氧化物包覆Co纳米颗粒催化氨分解","authors":"Hiroshi Mizoguchi, Shunqin Luo, Masato Sasase, Masaaki Kitano, Hideo Hosono","doi":"10.1021/acs.jpclett.4c03309","DOIUrl":null,"url":null,"abstract":"We fabricated Co-based catalysts by the low-temperature thermal decomposition of R–Co intermetallics (R = Y, La, or Ce) to reduce the temperature of ammonia cracking for hydrogen production. The catalysts synthesized are nanocomposites of Co/RO<sub><i>x</i></sub> with a metal-rich composition. In the Co<sub>13</sub>/LaO<sub>1.5</sub> catalyst derived from LaCo<sub>13</sub>, Co nanoparticles of 10–30 nm size are enclosed by the LaO<sub>1.5</sub> matrix. The nanocomposite exhibited superior catalytic activity (91% at 500 °C), which was attributed to dual advantages; the low workfunction of the supporter, O-deficient LaO<sub>1.5-x</sub> nanoparticles, promotes electron donation to the Co catalyst in the interface, which leads to enhanced N–H bond dissociation. Moreover, such a composite structure is effective in suppressing the grain growth of Co nanoparticles because the LaO<sub>1.5</sub> layer works as a diffusion barrier against Co. The thermal decomposition of intermetallics is a new route for the facile synthesis of catalysts having an electronically active support.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"29 1","pages":""},"PeriodicalIF":4.8000,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ammonia Decomposition Catalyzed by Co Nanoparticles Encapsulated in Rare Earth Oxide\",\"authors\":\"Hiroshi Mizoguchi, Shunqin Luo, Masato Sasase, Masaaki Kitano, Hideo Hosono\",\"doi\":\"10.1021/acs.jpclett.4c03309\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"We fabricated Co-based catalysts by the low-temperature thermal decomposition of R–Co intermetallics (R = Y, La, or Ce) to reduce the temperature of ammonia cracking for hydrogen production. The catalysts synthesized are nanocomposites of Co/RO<sub><i>x</i></sub> with a metal-rich composition. In the Co<sub>13</sub>/LaO<sub>1.5</sub> catalyst derived from LaCo<sub>13</sub>, Co nanoparticles of 10–30 nm size are enclosed by the LaO<sub>1.5</sub> matrix. The nanocomposite exhibited superior catalytic activity (91% at 500 °C), which was attributed to dual advantages; the low workfunction of the supporter, O-deficient LaO<sub>1.5-x</sub> nanoparticles, promotes electron donation to the Co catalyst in the interface, which leads to enhanced N–H bond dissociation. Moreover, such a composite structure is effective in suppressing the grain growth of Co nanoparticles because the LaO<sub>1.5</sub> layer works as a diffusion barrier against Co. The thermal decomposition of intermetallics is a new route for the facile synthesis of catalysts having an electronically active support.\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"29 1\",\"pages\":\"\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-01-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpclett.4c03309\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c03309","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Ammonia Decomposition Catalyzed by Co Nanoparticles Encapsulated in Rare Earth Oxide
We fabricated Co-based catalysts by the low-temperature thermal decomposition of R–Co intermetallics (R = Y, La, or Ce) to reduce the temperature of ammonia cracking for hydrogen production. The catalysts synthesized are nanocomposites of Co/ROx with a metal-rich composition. In the Co13/LaO1.5 catalyst derived from LaCo13, Co nanoparticles of 10–30 nm size are enclosed by the LaO1.5 matrix. The nanocomposite exhibited superior catalytic activity (91% at 500 °C), which was attributed to dual advantages; the low workfunction of the supporter, O-deficient LaO1.5-x nanoparticles, promotes electron donation to the Co catalyst in the interface, which leads to enhanced N–H bond dissociation. Moreover, such a composite structure is effective in suppressing the grain growth of Co nanoparticles because the LaO1.5 layer works as a diffusion barrier against Co. The thermal decomposition of intermetallics is a new route for the facile synthesis of catalysts having an electronically active support.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.