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

IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL
Yuqi Niu , Yan Cao , Ning Liu , Chengna Dai , Ruinian Xu , Gangqiang Yu , Ning Wang , Biaohua Chen , Yubing Xu , Hongxia Han
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引用次数: 0

摘要

丙烷干式重整(PDR)与甲烷干式重整(DRM)相比,其能源需求更低,在合成气生产中受到越来越多的关注。本研究以H2为结构导向剂,PEG、EG为分散剂,通过一步水热法制备了一系列Pt/Ni负载的超低金属负载(0.2 wt% Pt和0.6 wt% Ni) ceo2基催化剂。优化后的催化剂Pt0·2/Ni0.6@CeO2−D-1H2具有优异的催化性能(C3H8、CO2转化率分别为39.4%和94.9%;600℃下的合成气产率为30 mmol·gcat−1·h−1),反应稳定性为30 h。XRD、H2- tpr、CO2- tpd、XPS和HRTEM等综合表征技术表明,H2和分散剂(PEG和EG)的引入显著提高了氧空位浓度,促进了CO2的吸附和活化。此外,它们还可以调节催化剂的形态结构,通过促进活性金属的锚定和加强Ni2+与载体的相互作用,有效抑制活性金属的烧结。现场FTIR分析表明:CO2最初吸附在催化剂表面形成碳酸盐,随后转化为甲酸酯中间体,最后分解为CO和OH *。总的来说,本研究展示了一种高效Pt/ ni负载的CeO2催化剂的开发,通过增强氧空位生成,优化金属-载体相互作用,实现了卓越的合成气产量,这将有助于其他高效催化剂的设计。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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.
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来源期刊
International Journal of Hydrogen Energy
International Journal of Hydrogen Energy 工程技术-环境科学
CiteScore
13.50
自引率
25.00%
发文量
3502
审稿时长
60 days
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.
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