Yan Li , Haohao Chang , Jia Wang , Kun Jiang , Yun-Quan Liu , Xinchang Pang
{"title":"一种高效的rh基La2Ce2O7柴油蒸汽重整催化剂:催化剂结构对其性能的影响","authors":"Yan Li , Haohao Chang , Jia Wang , Kun Jiang , Yun-Quan Liu , Xinchang Pang","doi":"10.1016/j.ijhydene.2025.150591","DOIUrl":null,"url":null,"abstract":"<div><div>The development of high-performance catalysts with good coking resistance and sulfur tolerance for diesel reforming has been a big challenge. Generally, the strong metal-support interaction (SMSI) plays a pivotal role in determining the catalytic performance. This study investigated comparatively a supported-type (Rh/La<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub>) and an embedded-type (La<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7</sub>) catalyst, and revealed that lattice-embedding strategy for active metals significantly enhances SMSI and improves catalytic activity. The activity tests demonstrated that the embedded-type catalyst La<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7</sub> exhibited a better low-temperature activity, achieving a nearly-complete diesel conversion (∼100 %) at 650 °C, whereas the supported-type catalyst only reached ∼85 % conversion at 750 °C. Stability tests in 650–850 °C further confirmed the high stability of La<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7</sub>, with a H<sub>2</sub> production rate of 70.4 % at 850 °C. Characterization of the catalysts confirmed that the embedded type, in which Rh<sup>3+</sup> was implemented with partially substituted Ce<sup>4+</sup>, triggered a strong SMSI effect, inducing electronic reconstruction within the support, i.e. promoting Ce<sup>4+</sup> to Ce<sup>3+</sup>, thus creating a high concentration of oxygen vacancies. Additionally, the highly dispersed Rh nanoclusters (with average size 2.5 nm, dispersity 44.0 %) were formed. All these structural features had collectively resulted in a catalyst of exceptional anti-coking and sulfur-tolerance properties. In summary, this study provided a good example for the oriented regulation of SMSI through lattice-embedding, which offered a useful guidance for the development of high-performance catalysts for on-board hydrogen production from diesel.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"159 ","pages":"Article 150591"},"PeriodicalIF":8.3000,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A highly-efficient Rh-based La2Ce2O7 catalyst for steam reforming of diesel: Effect of catalyst structure on performance\",\"authors\":\"Yan Li , Haohao Chang , Jia Wang , Kun Jiang , Yun-Quan Liu , Xinchang Pang\",\"doi\":\"10.1016/j.ijhydene.2025.150591\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The development of high-performance catalysts with good coking resistance and sulfur tolerance for diesel reforming has been a big challenge. Generally, the strong metal-support interaction (SMSI) plays a pivotal role in determining the catalytic performance. This study investigated comparatively a supported-type (Rh/La<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub>) and an embedded-type (La<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7</sub>) catalyst, and revealed that lattice-embedding strategy for active metals significantly enhances SMSI and improves catalytic activity. The activity tests demonstrated that the embedded-type catalyst La<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7</sub> exhibited a better low-temperature activity, achieving a nearly-complete diesel conversion (∼100 %) at 650 °C, whereas the supported-type catalyst only reached ∼85 % conversion at 750 °C. Stability tests in 650–850 °C further confirmed the high stability of La<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7</sub>, with a H<sub>2</sub> production rate of 70.4 % at 850 °C. Characterization of the catalysts confirmed that the embedded type, in which Rh<sup>3+</sup> was implemented with partially substituted Ce<sup>4+</sup>, triggered a strong SMSI effect, inducing electronic reconstruction within the support, i.e. promoting Ce<sup>4+</sup> to Ce<sup>3+</sup>, thus creating a high concentration of oxygen vacancies. Additionally, the highly dispersed Rh nanoclusters (with average size 2.5 nm, dispersity 44.0 %) were formed. All these structural features had collectively resulted in a catalyst of exceptional anti-coking and sulfur-tolerance properties. In summary, this study provided a good example for the oriented regulation of SMSI through lattice-embedding, which offered a useful guidance for the development of high-performance catalysts for on-board hydrogen production from diesel.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":\"159 \",\"pages\":\"Article 150591\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2025-07-22\",\"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/S0360319925035906\",\"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/S0360319925035906","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}
A highly-efficient Rh-based La2Ce2O7 catalyst for steam reforming of diesel: Effect of catalyst structure on performance
The development of high-performance catalysts with good coking resistance and sulfur tolerance for diesel reforming has been a big challenge. Generally, the strong metal-support interaction (SMSI) plays a pivotal role in determining the catalytic performance. This study investigated comparatively a supported-type (Rh/La2Ce2O7) and an embedded-type (La2Ce1.89Rh0.11O7) catalyst, and revealed that lattice-embedding strategy for active metals significantly enhances SMSI and improves catalytic activity. The activity tests demonstrated that the embedded-type catalyst La2Ce1.89Rh0.11O7 exhibited a better low-temperature activity, achieving a nearly-complete diesel conversion (∼100 %) at 650 °C, whereas the supported-type catalyst only reached ∼85 % conversion at 750 °C. Stability tests in 650–850 °C further confirmed the high stability of La2Ce1.89Rh0.11O7, with a H2 production rate of 70.4 % at 850 °C. Characterization of the catalysts confirmed that the embedded type, in which Rh3+ was implemented with partially substituted Ce4+, triggered a strong SMSI effect, inducing electronic reconstruction within the support, i.e. promoting Ce4+ to Ce3+, thus creating a high concentration of oxygen vacancies. Additionally, the highly dispersed Rh nanoclusters (with average size 2.5 nm, dispersity 44.0 %) were formed. All these structural features had collectively resulted in a catalyst of exceptional anti-coking and sulfur-tolerance properties. In summary, this study provided a good example for the oriented regulation of SMSI through lattice-embedding, which offered a useful guidance for the development of high-performance catalysts for on-board hydrogen production from diesel.
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.