Efficient conversion and carbon deposition inhibit strategy of photothermal-driven methane reforming on Ni@SrTiO3 catalyst
马旭杨卫卫
MA Xu;YANG Weiwei
西安交通大学能源与动力工程学院
深入探索了甲烷与二氧化碳在光热异质催化剂体系中的高效反应特性,旨在为甲烷干重整反应提供一种更具潜力的催化解决方案。为达成此目标,选取了Ni@CaAlxOy、Ni@SrTiO3和Ni@Sr0.5Ba0.5TiO3三种催化剂,并在400~800℃的宽泛温度范围内对其性能进行了全面评估。实验结果显示,Ni@SrTiO3催化剂展现出了最高的稳定性和催化活性,尤其在800℃时,其甲烷转化率峰值高达89.12%,显著优于其他2种催化剂。这一表现不仅表现了Ni@SrTiO3在甲烷干重整反应中的应用潜力,也凸显了光热驱动技术在提升催化性能方面的显著优势。本研究还综合运用了氢气程序升温还原(H2-TPR)、二氧化碳程序升温脱附(CO2-TPD)及电子顺磁共振(EPR)等先进表征技术,深入揭示了Ni@SrTiO3催化剂良好性能的内在机制。通过上述表征技术发现,Ni@SrTiO3的优异性能主要源于其独特的表面缺陷结构、丰富的碱性中心以及高浓度的氧空位。这些特性不仅促进了反应物的吸附和活化,还优化了氧迁移机制,从而提升了催化效率。此外,Ni@SrTiO3还表现出了强大的抗积碳性能,这得益于其优化的三元催化界面,有效抑制了甲烷干重整副反应,进一步保障了催化剂的稳定性和耐用性。这些发现不仅为甲烷干重整反应提供了一种更具潜力的催化解决方案,也为催化剂的设计和优化提供了重要的理论指导和实践依据。未来研究将进一步优化Ni@SrTiO3催化剂的组成和结构,以期实现更高效、更可持续的甲烷转化与氢气制备过程。
This study delves into the exploration of efficient reaction characteristics of methane and carbon dioxide in a photothermalheterogeneous catalyst system, aiming to provide a more promising catalytic solution for methane dry reforming. To achieve this objective,three catalysts: Ni@CaAlxOy, Ni@SrTiO3, and Ni@Sr0.5Ba0.5TiO3 were selected and comprehensively evaluated for their performancewithin a broad temperature range of 400~800 ℃. The experimental results demonstrated that the Ni@SrTiO3 catalyst exhibited the higheststability and catalytic activity, particularly at 800 ℃, where its methane conversion peaked at 89.12%, significantly outperforming the othertwo catalysts. This performance not only underscores the potential application of Ni@SrTiO3 in methane dry reforming but also highlightsthe significant advantages of photothermal drive technology in enhancing catalytic performance. Furthermore, this study employedadvanced characterization techniques, including hydrogen temperature-programmed reduction (H2-TPR), carbon dioxide temperature-programmed desorption (CO2-TPD), and electron paramagnetic resonance (EPR), to delve into the underlying mechanisms ofNi@SrTiO3’s superior performance. Through these characterization techniques, it was found that Ni@SrTiO3’s exceptional performance is primarily attributed to its unique surface defect structure, abundant alkaline centers, and high concentrations of oxygen vacancies. Thesecharacteristics not only facilitate the adsorption and activation of reactants but also optimize the oxygen migration mechanism, therebyenhancing catalytic efficiency. Additionally, Ni@SrTiO3 demonstrated robust anti-coking performance, benefiting from its optimizedternary catalytic interface, which effectively inhibits side reactions in methane dry reforming, further ensuring the stability and durabilityof the catalyst. These findings not only provide a more promising catalytic solution for methane dry reforming but also offer importanttheoretical guidance and practical basis for the design and optimization of catalysts. Future research will further optimize the compositionand structure of the Ni@SrTiO3 catalyst to achieve more efficient and sustainable methane conversion and hydrogen production processes.
光热耦合甲烷重整积碳氧传输机制催化活性
photothermal coupling;methane reforming;carbon deposition;oxygen transport mechanism;catalytic activity
主办单位:煤炭科学研究总院有限公司 中国煤炭学会学术期刊工作委员会