Shu Liu , Yujia Han , Teng Zong , Chaojie Wang , Ming Tian , Lin Li , Wansheng Zhang , Wentao Wang , Xiaodong Wang
{"title":"Pt催化剂催化分解硝酸羟铵配位数依赖性研究","authors":"Shu Liu , Yujia Han , Teng Zong , Chaojie Wang , Ming Tian , Lin Li , Wansheng Zhang , Wentao Wang , Xiaodong Wang","doi":"10.1016/j.apcata.2025.120457","DOIUrl":null,"url":null,"abstract":"<div><div>To uncover the relation between active metals structure and the adsorption, activation as well as its decomposition performance of hydroxylamine nitrate (HAN) that has been considered to be a promising low-toxicity monopropellant for spacecrafts, the performance of xPt/Al<sub>2</sub>O<sub>3</sub> with various Pt loadings (x = 0.1, 0.5, 1 and 2, indicates the mass percentage of Pt) was evaluated in the aqueous HAN (10 wt%) decomposition. It was found that the both the NH<sub>3</sub>OH<sup>+</sup> conversion and the turnover frequency (TOF) enhanced as Pt loadings increased while NO<sub>3</sub><sup>-</sup> was hardly converted at the temperature of lower than 120 ℃ for xPt/Al<sub>2</sub>O<sub>3</sub>, and 2Pt/Al<sub>2</sub>O<sub>3</sub> exhibited the best activity with almost 100 % NH<sub>3</sub>OH<sup>+</sup> conversion, 20 % NH<sub>4</sub><sup>+</sup> selectivity and 80 % N<sub>2</sub>O selectivity at around 120 ℃, respectively. This originated from the increased Pt coordinated number of active sites with sufficiently continuous Pt sites caused by its enhanced particle size with loadings, which was beneficial to the cracking of N-O, O-H and N-H bonds together thus the activation and conversion of NH<sub>3</sub>OH<sup>+</sup> to NH<sub>4</sub><sup>+</sup> and N<sub>2</sub>O.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"705 ","pages":"Article 120457"},"PeriodicalIF":4.8000,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Coordination number dependence of Pt catalysts for catalytic decomposition of aqueous hydroxylammonium nitrate (HAN)\",\"authors\":\"Shu Liu , Yujia Han , Teng Zong , Chaojie Wang , Ming Tian , Lin Li , Wansheng Zhang , Wentao Wang , Xiaodong Wang\",\"doi\":\"10.1016/j.apcata.2025.120457\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>To uncover the relation between active metals structure and the adsorption, activation as well as its decomposition performance of hydroxylamine nitrate (HAN) that has been considered to be a promising low-toxicity monopropellant for spacecrafts, the performance of xPt/Al<sub>2</sub>O<sub>3</sub> with various Pt loadings (x = 0.1, 0.5, 1 and 2, indicates the mass percentage of Pt) was evaluated in the aqueous HAN (10 wt%) decomposition. It was found that the both the NH<sub>3</sub>OH<sup>+</sup> conversion and the turnover frequency (TOF) enhanced as Pt loadings increased while NO<sub>3</sub><sup>-</sup> was hardly converted at the temperature of lower than 120 ℃ for xPt/Al<sub>2</sub>O<sub>3</sub>, and 2Pt/Al<sub>2</sub>O<sub>3</sub> exhibited the best activity with almost 100 % NH<sub>3</sub>OH<sup>+</sup> conversion, 20 % NH<sub>4</sub><sup>+</sup> selectivity and 80 % N<sub>2</sub>O selectivity at around 120 ℃, respectively. This originated from the increased Pt coordinated number of active sites with sufficiently continuous Pt sites caused by its enhanced particle size with loadings, which was beneficial to the cracking of N-O, O-H and N-H bonds together thus the activation and conversion of NH<sub>3</sub>OH<sup>+</sup> to NH<sub>4</sub><sup>+</sup> and N<sub>2</sub>O.</div></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":\"705 \",\"pages\":\"Article 120457\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-07-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X25003588\",\"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":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X25003588","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Coordination number dependence of Pt catalysts for catalytic decomposition of aqueous hydroxylammonium nitrate (HAN)
To uncover the relation between active metals structure and the adsorption, activation as well as its decomposition performance of hydroxylamine nitrate (HAN) that has been considered to be a promising low-toxicity monopropellant for spacecrafts, the performance of xPt/Al2O3 with various Pt loadings (x = 0.1, 0.5, 1 and 2, indicates the mass percentage of Pt) was evaluated in the aqueous HAN (10 wt%) decomposition. It was found that the both the NH3OH+ conversion and the turnover frequency (TOF) enhanced as Pt loadings increased while NO3- was hardly converted at the temperature of lower than 120 ℃ for xPt/Al2O3, and 2Pt/Al2O3 exhibited the best activity with almost 100 % NH3OH+ conversion, 20 % NH4+ selectivity and 80 % N2O selectivity at around 120 ℃, respectively. This originated from the increased Pt coordinated number of active sites with sufficiently continuous Pt sites caused by its enhanced particle size with loadings, which was beneficial to the cracking of N-O, O-H and N-H bonds together thus the activation and conversion of NH3OH+ to NH4+ and N2O.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.