Yuqi Niu , Yan Cao , Ning Liu , Chengna Dai , Ruinian Xu , Gangqiang Yu , Ning Wang , Biaohua Chen , Yubing Xu , Hongxia Han
{"title":"高效丙烷干重整的超低负荷Pt/ ni负载CeO2催化剂:增强氧空位和金属负载相互作用,提高合成气产量","authors":"Yuqi Niu , Yan Cao , Ning Liu , Chengna Dai , Ruinian Xu , Gangqiang Yu , Ning Wang , Biaohua Chen , Yubing Xu , Hongxia Han","doi":"10.1016/j.ijhydene.2025.05.377","DOIUrl":null,"url":null,"abstract":"<div><div>Dry reforming of propane (PDR) has attracted increasing attention for syngas production due to its lower energy demand compared to methane dry reforming (DRM). In this study, a series of Pt/Ni-supported CeO<sub>2</sub>-based catalysts with ultralow metal loadings (0.2 wt% Pt and 0.6 wt% Ni) was synthesized via a one-step hydrothermal method by utilizing H<sub>2</sub> as a structure-directing agent and PEG, EG as the dispersants. The optimized catalyst of Pt<sub>0·2</sub>/Ni<sub>0.6</sub>@CeO<sub>2</sub><sup>−D</sup>-1H<sub>2</sub> demonstrates exceptional catalytic performance (C<sub>3</sub>H<sub>8</sub>, CO<sub>2</sub> conversions of 39.4 and 94.9 %; syngas productivity of both 30 mmol·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>) and reaction stability (pass through 30 h's reaction) at 600 °C. Comprehensive characterization techniques, including XRD, H<sub>2</sub>-TPR, CO<sub>2</sub>-TPD, XPS, and HRTEM, reveal that the introduction of H<sub>2</sub> and dispersants (PEG and EG) significantly enhance the oxygen vacancy concentration, which promoted CO<sub>2</sub> adsorption and activation. Moreover, they can also modulate the catalyst morphology structure, which effectively inhibits the sintering of active metals through promoting the anchoring of active metals and strengthening the interaction between Ni<sup>2+</sup> and the support. In-situ FTIR analysis suggested a plausible reaction mechanism: CO<sub>2</sub> initially adsorbs on the catalyst surface to form carbonate species, which are subsequently transformed into formate intermediates and finally decomposed into CO and OH∗ species. Generally, this study demonstrates the development of a highly efficient Pt/Ni-supported CeO<sub>2</sub> catalyst achieving superior syngas production through enhanced oxygen vacancy generation, optimized metal-support interaction, which would contribute to other highly efficient catalyst designs.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"143 ","pages":"Pages 250-264"},"PeriodicalIF":8.1000,"publicationDate":"2025-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ultralow-loading Pt/Ni-supported CeO2 catalysts for efficient propane dry reforming: Enhanced oxygen vacancies and metal-support interaction for superior syngas production\",\"authors\":\"Yuqi Niu , Yan Cao , Ning Liu , Chengna Dai , Ruinian Xu , Gangqiang Yu , Ning Wang , Biaohua Chen , Yubing Xu , Hongxia Han\",\"doi\":\"10.1016/j.ijhydene.2025.05.377\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Dry reforming of propane (PDR) has attracted increasing attention for syngas production due to its lower energy demand compared to methane dry reforming (DRM). In this study, a series of Pt/Ni-supported CeO<sub>2</sub>-based catalysts with ultralow metal loadings (0.2 wt% Pt and 0.6 wt% Ni) was synthesized via a one-step hydrothermal method by utilizing H<sub>2</sub> as a structure-directing agent and PEG, EG as the dispersants. The optimized catalyst of Pt<sub>0·2</sub>/Ni<sub>0.6</sub>@CeO<sub>2</sub><sup>−D</sup>-1H<sub>2</sub> demonstrates exceptional catalytic performance (C<sub>3</sub>H<sub>8</sub>, CO<sub>2</sub> conversions of 39.4 and 94.9 %; syngas productivity of both 30 mmol·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup>) and reaction stability (pass through 30 h's reaction) at 600 °C. Comprehensive characterization techniques, including XRD, H<sub>2</sub>-TPR, CO<sub>2</sub>-TPD, XPS, and HRTEM, reveal that the introduction of H<sub>2</sub> and dispersants (PEG and EG) significantly enhance the oxygen vacancy concentration, which promoted CO<sub>2</sub> adsorption and activation. Moreover, they can also modulate the catalyst morphology structure, which effectively inhibits the sintering of active metals through promoting the anchoring of active metals and strengthening the interaction between Ni<sup>2+</sup> and the support. In-situ FTIR analysis suggested a plausible reaction mechanism: CO<sub>2</sub> initially adsorbs on the catalyst surface to form carbonate species, which are subsequently transformed into formate intermediates and finally decomposed into CO and OH∗ species. Generally, this study demonstrates the development of a highly efficient Pt/Ni-supported CeO<sub>2</sub> catalyst achieving superior syngas production through enhanced oxygen vacancy generation, optimized metal-support interaction, which would contribute to other highly efficient catalyst designs.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":\"143 \",\"pages\":\"Pages 250-264\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2025-06-05\",\"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/S0360319925026916\",\"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/S0360319925026916","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}
Ultralow-loading Pt/Ni-supported CeO2 catalysts for efficient propane dry reforming: Enhanced oxygen vacancies and metal-support interaction for superior syngas production
Dry reforming of propane (PDR) has attracted increasing attention for syngas production due to its lower energy demand compared to methane dry reforming (DRM). In this study, a series of Pt/Ni-supported CeO2-based catalysts with ultralow metal loadings (0.2 wt% Pt and 0.6 wt% Ni) was synthesized via a one-step hydrothermal method by utilizing H2 as a structure-directing agent and PEG, EG as the dispersants. The optimized catalyst of Pt0·2/Ni0.6@CeO2−D-1H2 demonstrates exceptional catalytic performance (C3H8, CO2 conversions of 39.4 and 94.9 %; syngas productivity of both 30 mmol·gcat−1·h−1) and reaction stability (pass through 30 h's reaction) at 600 °C. Comprehensive characterization techniques, including XRD, H2-TPR, CO2-TPD, XPS, and HRTEM, reveal that the introduction of H2 and dispersants (PEG and EG) significantly enhance the oxygen vacancy concentration, which promoted CO2 adsorption and activation. Moreover, they can also modulate the catalyst morphology structure, which effectively inhibits the sintering of active metals through promoting the anchoring of active metals and strengthening the interaction between Ni2+ and the support. In-situ FTIR analysis suggested a plausible reaction mechanism: CO2 initially adsorbs on the catalyst surface to form carbonate species, which are subsequently transformed into formate intermediates and finally decomposed into CO and OH∗ species. Generally, this study demonstrates the development of a highly efficient Pt/Ni-supported CeO2 catalyst achieving superior syngas production through enhanced oxygen vacancy generation, optimized metal-support interaction, which would contribute to other highly efficient catalyst designs.
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.