Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion

Yang, Weiwei; Polo‐Garzon, Felipe; Zhou, Hua; Huang, Zhennan; Chi, Miaofang; Meyer, Harry M.; Yu, Xinbin; Li, Yuanyuan; Wu, Zili

doi:10.1002/ange.202217323

Cited by 4 publications

(3 citation statements)

References 41 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…For a catalyst loaded with Pd single atoms, the binding energy of Pd 3d (Figure 4g) can be fitted to four peaks, the 3d 5/2 characteristic peak of the Pd δ+ state (0< δ <2) is located at 336.23–336.46 eV, and the 3d 3/2 characteristic peak is located at 341.45–341.7 eV (purple), [ 21 ] while 337.56–337.7 eV corresponds to the 3d 5/2 of the Pd 2+ state. The peak at 342.82–343 eV corresponds to the 3d 3/2 of the Pd 2+ state (orange).…”

Section: Resultsmentioning

confidence: 99%

Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

Zheng,

Zhang,

Jiang

et al. 2024

Small

View full text Add to dashboard Cite

Single‐atom catalysts (SACs) exhibit remarkable catalytic activity at each metal site. However, conventionally synthesized single‐atom catalysts often possess low metal loading, thereby constraining their overall catalytic performance. Here, a flame spray pyrolysis (FSP) method for the synthesis of a single‐atom catalyst with a high loading capacity of up to 1.4 wt.% in practice is reported. CeZrO2 acts as a carrier and provides a large number of anchoring sites, which promotes the high‐density generation of Pd, and the strong interaction between the metal and the support avoids atom aggregation. Pd‐CeZrO2 series catalysts have excellent CO oxidation performance. When 0.97 wt.% Pd is added, the catalytic activity is the highest, and the temperature can be reduced to 120 °C. This work presented here demonstrates that FSP, as an inherently scalable technique, allows for elevating the single‐atom loading to achieve an increase in its catalytic performance. The method presented here more options for the preparation of SACs.

show abstract

Section: Resultsmentioning

confidence: 99%

Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

Zheng,

Zhang,

Jiang

et al. 2024

Small

View full text Add to dashboard Cite

show abstract

“…Supported Pd-based catalysts are widely used in the oxidation reactions with the preeminent catalytic activity; − however, they are prone to cause the deep oxidation of organic compounds, resulting in the low product selectivity. Take the selective oxidation of alcohols for example, supported Pd-based catalysts exhibit high activity for alcohol oxidation whereas tend to cause deep oxidation to CO 2 at the elevated temperature. , The selectivity and yield of the selective oxidation products could be greatly decreased at high conversion of alcohol at high temperature.…”

Section: Introductionmentioning

confidence: 99%

Highly Selective Activation of C–H Bond and Inhibition of C–C Bond Cleavage by Tuning Strong Oxidative Pd Sites

Guo,

Ma,

Wei

et al. 2023

J. Am. Chem. Soc.

View full text Add to dashboard Cite

Improving the product selectivity meanwhile restraining deep oxidation still remains a great challenge over the supported Pd-based catalysts. Herein, we demonstrate a universal strategy where the surface strong oxidative Pd sites are partially covered by the transition metal (e. g., Cu, Co, Ni, and Mn) oxide through thermal treatment of alloys. It could effectively inhibit the deep oxidation of isopropanol and achieve the ultrahigh selectivity (>98%) to the target product acetone in a wide temperature range of 50–200 °C, even at 150–200 °C with almost 100% isopropanol conversion over PdCu1.2/Al2O3, while an obvious decline in acetone selectivity is observed from 150 °C over Pd/Al2O3. Furthermore, it greatly improves the low-temperature catalytic activity (acetone formation rate at 110 °C over PdCu1.2/Al2O3, 34.1 times higher than that over Pd/Al2O3). The decrease of surface Pd site exposure weakens the cleavage for the C–C bond, while the introduction of proper CuO shifts the d-band center (εd) of Pd upward and strengthens the adsorption and activation of reactants, providing more reactive oxygen species, especially the key super oxygen species (O2 –) for selective oxidation, and significantly reducing the barrier of O–H and β-C–H bond scission. The molecular-level understanding of the C–H and C–C bond scission mechanism will guide the regulation of strong oxidative noble metal sites with relatively inert metal oxide for the other selective catalytic oxidation reactions.

show abstract

“…The big challenge is that H 2 O (typical concentration = 5-15 vol%) and SO 2 (typical concentration = 1-30 ppm) in the exhaust gas results in severe deactivation of the catalysts that decrease the CH 4 removal efficiency. Many available supports have been reported, such as Al 2 O 3 [17][18][19][20][21][22][23], CeO 2 [24][25][26][27], Ce 1−x Zr x O 2 solid solutions [28][29][30], and SnO 2 [31][32][33][34]. Zeolites with various additives have also been used in methane combustion.…”

Section: Introductionmentioning

confidence: 99%

Methane Combustion over Zeolite-Supported Palladium-Based Catalysts

Tao,

Liu,

Deng

et al. 2023

Catalysts

View full text Add to dashboard Cite

The emission of methane leads to the increase in the methane concentration in the atmosphere, which not only wastes resources but also intensifies the greenhouse effect and brings about serious environmental problems. Catalytic combustion can completely convert methane into carbon dioxide and water at low temperatures. However, the catalytic activities of the conventional supported palladium catalysts (e.g., Pd/Al2O3 and Pd/ZrO2) are easy to decrease or the two catalysts can even be deactivated under actual harsh reaction conditions (high temperatures, steam- and sulfur dioxide-containing atmospheres, etc.). Recently, noble metal catalysts supported on zeolites with ordered pores and good thermal stability have attracted much attention. This review article summarizes the recent progress on the development and characteristics of zeolite-supported noble metal catalysts for the combustion of methane. The effects of framework structures, silica/alumina ratios, acidity, doping of alkali metals or transition metals, particle sizes and distributions, and their locations of/in the zeolites on methane combustion activity are discussed. The importance of developing high-performance catalysts under realistic operation conditions is highlighted. In addition, the related research work on catalytic methane combustion in the future is also envisioned.

show abstract

Boosting the Activity of Pd Single Atoms by Tuning Their Local Environment on Ceria for Methane Combustion

Cited by 4 publications

References 41 publications

Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

Pd Single‐Atom Loaded Ce‐Zr Solid Solution Catalysts Prepared by Flame Spray Pyrolysis for Efficient CO Catalytic Oxidation

Highly Selective Activation of C–H Bond and Inhibition of C–C Bond Cleavage by Tuning Strong Oxidative Pd Sites

Methane Combustion over Zeolite-Supported Palladium-Based Catalysts

Contact Info

Product

Resources

About