Blocking the <i>Operando</i> Formation of Single‐Atom Spectators by Interfacial Engineering
Aside from activity and selectivity, catalyst stability is a key focus in heterogeneous catalysis research. Although sintering of metal species has been considered the primary cause for deactivation of metal catalysts, our study reveals that the loss of activity at low reaction temperatures in the CeO<sub>2</sub>-supported Pt (Pt/CeO<sub>2</sub>) catalyst in complete propane oxidation is due to the dispersion of Pt ensemble sites (nanoclusters) and their subsequent operando conversion into Pt single atoms under reaction conditions. These Pt single-atom species exhibit low reactivity and act as spectators in the low-temperature reaction region. To address this issue, we engineered the surface of CeO<sub>2</sub> by introducing NbO<sub>x</sub>, which does not directly interact with Pt. Instead, NbO<sub>x</sub> blocks the strong binding sites for Pt on CeO<sub>2</sub>, thereby preventing Pt redispersion/fragmentation and preserving reactive Pt ensembles. This strategy led to a remarkable 37-fold increase in the reaction rate compared to the Pt/CeO<sub>2</sub> catalyst. Our findings emphasize the importance of suppressing the formation of noble metal single-atom spectators through innovative surface engineering strategy. These mechanistic insights not only advance the understanding of the materials science of Pt/CeO<sub>2</sub> but also extend to critical technological fields such as energy conversion systems and environmental remediation technologies.
Authors
- Lihui Zhou (ORCID: https://orcid.org/0000-0003-1434-8799)
- Junzhong Xie (ORCID: https://orcid.org/0000-0002-9457-9572)
- Mi Peng (ORCID: https://orcid.org/0000-0001-7713-4398)
- Sheng Dai (ORCID: https://orcid.org/0000-0001-5787-0179)
- Yun Guo (ORCID: https://orcid.org/0000-0003-4778-6007)
- Bingqing Yao (ORCID: https://orcid.org/0000-0002-7769-021X)
- Qian He (ORCID: https://orcid.org/0000-0003-4891-3581)
- Ding Ma (ORCID: https://orcid.org/0000-0002-3341-2998)
- Geng Sun (ORCID: https://orcid.org/0000-0003-2123-7464)
- Bingjun Xu (ORCID: https://orcid.org/0000-0002-2303-257X)
- Yanglong Guo (ORCID: https://orcid.org/0000-0003-0021-9128)
- Shasha Ge (ORCID: https://orcid.org/0009-0005-0636-8185)
- Li Wang (ORCID: https://orcid.org/0000-0002-2469-8007)
- Wangcheng Zhan (ORCID: https://orcid.org/0000-0002-0712-4917)
- Yao Xü (ORCID: https://orcid.org/0000-0003-0602-898X)
- Jie Zhang (ORCID: https://orcid.org/0000-0002-9976-3942)
- Zhaohua Wang (ORCID: https://orcid.org/0000-0001-9878-8382)
- Xuan Tang (ORCID: https://orcid.org/0000-0003-2604-4178)
- Yao Lv
Institutions
- King University (US)
- East China University of Science and Technology (CN)
- Chongqing University (CN)
- National University of Singapore (SG)
- Peking University (CN)
- Beijing National Laboratory for Molecular Sciences (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-04-03
- DOI
- https://doi.org/10.1002/anie.202505507
- Citations
- 12
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 6.21
Funders
- Tencent
- National Natural Science Foundation of China
- East China University of Science and Technology
- Science and Technology Commission of Shanghai Municipality
- National Key Research and Development Program of China
- Fundamental Research Funds for the Central Universities