Fabrication and Mechanism Study of Clustered Au/CeO2 Catalyst for the CO Oxidation Reaction★

doi:10.6023/A23040174

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (8): 874-883.DOI: 10.6023/A23040174 Previous Articles Next Articles

Special Issue: 庆祝《化学学报》创刊90周年合辑

Article

团簇Au/CeO₂的制备及其催化CO氧化反应构效关系的研究^★

付信朴^a, 王秀玲^a, 王伟伟^a, 司锐^b, 贾春江^a^,^*()

a 山东大学化学与化工学院胶体与界面化学重点实验室特种聚合材料重点实验室济南 250100
b 中山大学材料学院广东深圳 518107

投稿日期:2023-04-28 发布日期:2023-09-14
作者简介:
^★庆祝《化学学报》创刊90周年.
基金资助:
项目受国家重点研发项目(2021YFA1501103); 国家杰出青年基金项目(22225110); 国家自然科学基金(22075166); 国家自然科学基金(22271177); 山东大学未来学者项目资助

Fabrication and Mechanism Study of Clustered Au/CeO₂ Catalyst for the CO Oxidation Reaction^★

Xinpu Fu^a, Xiuling Wang^a, Weiwei Wang^a, Rui Si^b, Chunjiang Jia^a()

a Key Laboratory of Special Aggregated Materials, Key Laboratory for Colloid and Interface Chemistry, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100
b School of Materials, Sun Yat-Sen University, Shenzhen, Guangdong 518107

Received:2023-04-28 Published:2023-09-14
Contact: *E-mail: jiacj@sdu.edu.cn
About author:
^★Dedicated to the 90th anniversary of Acta Chimica Sinica.
Supported by:
National Key Research and Development Program of China(2021YFA1501103); National Science Fund for Distinguished Young Scholars of China(22225110); National Natural Science Foundation of China(22075166); National Natural Science Foundation of China(22271177); Young Scholars Program of Shandong University

Supported Au-based catalysts have been attracting continuous attention owing to their outstanding performance in various catalytic applications. However, the complicated environment on the catalyst surface severely hampered the unambiguous illustration of the structural-function relationship for Au-based catalysts. In this work, we developed a facile strategy to fabricate various Au species [Auⁿ^＋ (n>1), Au^δ^＋ (0<n<1) and Au⁰] onto the CeO₂ support, which the Au/CeO₂interaction was distinctively modulated by the CeO₂-x with different calcination temperatures. As-prepared Au/CeO₂-x were valued as catalysts for CO oxidation reaction, which is important for both environmental application and model catalysis. The as-formed clustered Au with δ＋ oxidation state on CeO₂-400 demonstrates the best catalytic performance at 50 ℃, while the Au nanoparticles with dominant Au⁰ atoms are superior for catalyzing CO oxidation at room temperature. However, the monodispersed Auⁿ^＋ single-sites with the highest dispersion are almost inactive for CO oxidation below 50 ℃. On the basis of structural characterizations and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results, we reasonably speculated that the electronic state of Au species plays a predominant role at room temperature for catalytic performance owing to the differentiated CO adsorption ability. This speculation is well in line with our former research finding that the Auⁿ^＋ sites are weak in capturing CO molecules and Au⁰ is favorable for CO adsorption. The surficial O atoms, especially the lattice O atoms, play a minor role in catalyzing CO oxidation for the Au particles within Au/CeO₂-700, implying that the reactant molecules might prefer a L-H pathway at room temperature. In contrast, the clustered Au^δ^＋ with moderate CO adsorption ability and abundant interfacial site was apt to participate in the surface reaction with a MvK pathway, in which the reaction between surficial lattice O atoms and adsorbed CO molecules significantly contribute to the catalytic activity. Therefore, the Au/CeO₂-400 catalyst coupling with moderate CO adsorption ability and abundant active O atoms displayed the best catalytic efficiency at elevated temperatures. These findings in this work provided a facile route for the fabrication efficient Au/CeO₂ catalyst, and shed light on the molecular understanding of the reaction path over various Au sites.

Key words: supported gold catalyst, ceria-based material, CO oxidation, in-situ characterizations, reaction mechanism

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Xinpu Fu, Xiuling Wang, Weiwei Wang, Rui Si, Chunjiang Jia. Fabrication and Mechanism Study of Clustered Au/CeO₂ Catalyst for the CO Oxidation Reaction^★[J]. Acta Chimica Sinica, 2023, 81(8): 874-883.

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Fig. & Tab. 10

Figure 1. (a) The XRD patterns of CeO2-x samples, (b) ATR-FTIR spectra of CeO2-x samples, (c) the XRD patterns of Au/CeO2-x samples and (d) H2-TPR profile of Au/CeO2-x samples

Figure 2. TEM images of (a, b) Au/CeO2-UC, (c, d) Au/CeO2-400 and (e, f) Au/CeO2-700

Figure 3. The BET areas of Au/CeO2-x samples

Figure 4. (a) XANES spectra of Au/CeO2-x samples; EXAFS spectra of (b) Au/CeO2-400 and (c) Au/CeO2-700, where the solid line is data and dash line is fitting result; (d) fitting results

Figure 5. Catalytic performance of Au/CeO2-x samples: (a) light-off test, (b) steady test at 50 ℃. Other reaction conditions: 1%CO/20%O2/N2, GHSV=97, 500 mL?g－1?h－1

Figure 6. In-situ DRIFTS spectra of CO adsorption for (a) Au/CeO2-UC, (b) Au/CeO2-400, (c) Au/CeO2-700

Figure 7. (a) XANES spectra of Au/CeO2-x used samples; EXAFS spectra of (b) Au/CeO2-400-used and (c) Au/CeO2-700-used, where the solid line is data and dash line is fitting results; (d) fitting results

Figure 8. In-situ DRIFTS spectra collected under various conditions: saturated CO adsorption (solid line); N2 purging for 2 min after CO adsorption (green dash line); O2 purging for 2 min after CO adsorption (blue dash line). (a) Au/CeO2-UC, (b) Au/CeO2-400 and (c) Au/CeO2-700, (d) summarized illustration of infrared absorption spectroscopy (IR) signal intensity for CO and CO2 species collected under switch mode

Figure 9. In-situ DRIFTS spectra collected under reaction condition: (a) 1950~2450 cm－1 and (b) 1000~1800 cm－1

Figure 10. CO-TPR profile of (a) Au/CeO2-UC, (b) Au/CeO2-400 and (c) Au/CeO2-700

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团簇Au/CeO₂的制备及其催化CO氧化反应构效关系的研究^★

Fabrication and Mechanism Study of Clustered Au/CeO₂ Catalyst for the CO Oxidation Reaction^★

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团簇Au/CeO2的制备及其催化CO氧化反应构效关系的研究★