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钯/二氧化铈锆三元催化剂中稀土掺杂对金属-载体相互作用的抑制作用

Inhibition of Metal-Support Interactions by Rare-Earth Doping in Palladium/Ceria Zirconia Three-Way Catalysts.

作者信息

Costley-Wood Lucy, Flores-González Nicolás A, Wilson Claire, Thompson Paul, Day Sarah, Celorrio Veronica, Decarolis Donato, Morris Ruby, Schuster Manfred E, Marchbank Huw, Hyde Timothy I, Kolpin Amy, Thompsett Dave, Gibson Emma K

机构信息

University of Glasgow, Glasgow G12 8QQ, U.K.

University College London, London WC1H 0AJ, U.K.

出版信息

Chem Mater. 2025 Aug 29;37(18):7214-7226. doi: 10.1021/acs.chemmater.5c01417. eCollection 2025 Sep 23.

DOI:10.1021/acs.chemmater.5c01417
PMID:41019949
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12461787/
Abstract

The impact of rare-earth (RE) doping in ceria-zirconiacritical for enhancing thermal stability and optimizing redox propertieson surface palladium (Pd) behavior has been investigated. RE doping was found to weaken metal-support interactions, leading to increased Pd mobility, with notable effects on oxygen storage capacity and light-off performance under model exhaust conditions. The mobility and redox characteristics of Pd were assessed through in situ thermal experiments using X-ray absorption spectroscopy at the Pd K-edge and synchrotron powder diffraction. Complementary Ce K-edge EXAFS and Rietveld refinements confirmed the structure and composition of the doped ceria-zirconia material. Deactivation studies and lifetime prediction are essential for commercial catalysts, particularly for three-way catalysts (TWCs) designed for decade-long operation. To probe long-term stability, in situ thermal treatments were conducted to induce separation of the metastable ceria-zirconia solid solution. These accelerated thermal aging treatments were then compared with a prolonged, seven week aging protocol, and regular in situ synchrotron PXRD measurements provided insights into the phase separation process. The influence of thermal aging on metal-support interactions was further assessed through catalytic performance testing.

摘要

研究了稀土（RE）掺杂氧化铈-氧化锆（这对于提高热稳定性和优化氧化还原性能至关重要）对表面钯（Pd）行为的影响。发现稀土掺杂会削弱金属-载体相互作用，导致钯的迁移率增加，在模拟排气条件下对储氧能力和起燃性能有显著影响。通过在钯K边使用X射线吸收光谱和同步加速器粉末衍射进行原位热实验，评估了钯的迁移率和氧化还原特性。补充的铈K边扩展X射线吸收精细结构（EXAFS）和Rietveld精修证实了掺杂氧化铈-氧化锆材料的结构和组成。失活研究和寿命预测对于商业催化剂至关重要，特别是对于设计用于长达十年运行的三元催化剂（TWC）。为了探究长期稳定性，进行了原位热处理以诱导亚稳氧化铈-氧化锆固溶体的分离。然后将这些加速热老化处理与延长的七周老化方案进行比较，定期的原位同步加速器粉末X射线衍射（PXRD）测量提供了对相分离过程的见解。通过催化性能测试进一步评估了热老化对金属-载体相互作用的影响。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/d4eeb247e3d1/cm5c01417_0009.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/d4eeb247e3d1/cm5c01417_0009.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/4310d3144a16/cm5c01417_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/95ffb83ad215/cm5c01417_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/ebc20e86aa34/cm5c01417_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/7477ad97fe95/cm5c01417_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/7d19a579b349/cm5c01417_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/27845f297a06/cm5c01417_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/918f/12461787/d4eeb247e3d1/cm5c01417_0009.jpg

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