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<p>Diesel reforming is a promising technology for onboard hydrogen supply. However, developing effective catalysts that are highly resistant to coking and sulfur poisoning remains a significant challenge. In this study, a series of A<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7−δ</sub> (A = Y, Pr, Sm) catalysts with a defective fluorite structure were synthesized. The investigation revealed that the catalyst with Sm as the A-site metal exhibited a porous honeycomb-like structure. This structure effectively promotes rapid mass transfer and reduces the occurrence of side reactions. Characterization results revealed that the catalyst possesses a significant number of surface oxygen vacancies. XPS analysis indicated that these abundant oxygen vacancies lead to a strong interaction between Rh and Sm<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub>. This interaction causes electron transfer from Rh to Sm<sub>2</sub>Ce<sub>2</sub>O<sub>7</sub>, resulting in electron-deficient Rh. This electron-deficient state suppresses the adsorption of sulfur on the active metal Rh, thereby enhancing sulfur tolerance. Additionally, the abundant oxygen vacancies and strong metal-support interaction contribute to the highest Rh dispersion (65.4%) and the smallest Rh particle size (1.7&#xa0;nm) among the catalysts studied. These factors significantly increase the number of active sites. Experimental results demonstrated that the Sm<sub>2</sub>Ce<sub>1.89</sub>Rh<sub>0.11</sub>O<sub>7−δ</sub> catalyst with abundant oxygen vacancies exhibited superior catalytic performance. It achieved nearly 100% conversion of n-hexadecane (containing 50 ppm sulfur) and produced a hydrogen composition of approximately 68% in the reforming products. Moreover, the catalyst maintained excellent stability over 30&#xa0;h of continuous operation, with no signs of sintering, carbon deposition, or sulfur poisoning.</p> Graphical Abstract <p></p>

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Constructing Highly Efficient A2Ce1.89Rh0.11O7−δ (A = Y, Pr, Sm) Compounds with Defective Cubic Fluorite Phase for Diesel Reforming

  • 期刊论文

  • 发表日期：

    2025年6月3日

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  • Yan Li,
  • Yi Song,
  • Hengda Zhang,
  • Haohao Chang

摘要

Diesel reforming is a promising technology for onboard hydrogen supply. However, developing effective catalysts that are highly resistant to coking and sulfur poisoning remains a significant challenge. In this study, a series of A2Ce1.89Rh0.11O7−δ (A = Y, Pr, Sm) catalysts with a defective fluorite structure were synthesized. The investigation revealed that the catalyst with Sm as the A-site metal exhibited a porous honeycomb-like structure. This structure effectively promotes rapid mass transfer and reduces the occurrence of side reactions. Characterization results revealed that the catalyst possesses a significant number of surface oxygen vacancies. XPS analysis indicated that these abundant oxygen vacancies lead to a strong interaction between Rh and Sm2Ce2O7. This interaction causes electron transfer from Rh to Sm2Ce2O7, resulting in electron-deficient Rh. This electron-deficient state suppresses the adsorption of sulfur on the active metal Rh, thereby enhancing sulfur tolerance. Additionally, the abundant oxygen vacancies and strong metal-support interaction contribute to the highest Rh dispersion (65.4%) and the smallest Rh particle size (1.7 nm) among the catalysts studied. These factors significantly increase the number of active sites. Experimental results demonstrated that the Sm2Ce1.89Rh0.11O7−δ catalyst with abundant oxygen vacancies exhibited superior catalytic performance. It achieved nearly 100% conversion of n-hexadecane (containing 50 ppm sulfur) and produced a hydrogen composition of approximately 68% in the reforming products. Moreover, the catalyst maintained excellent stability over 30 h of continuous operation, with no signs of sintering, carbon deposition, or sulfur poisoning.

Graphical Abstract