Authors
Meiyang Cui, Xiangru Wei, Moon Young Yang, Grayson Johnson, Perrin Godbold, Yizhen Chen, Maoyu Wang, Yugang Zhang, Chang Liu, Shengsong Yang, Brian Lee, Sooyeon Hwang, Farzad Bastani, Mingyang Liu, Petra Reinke, Lu Ma, Hua Zhou, Christopher B Murray, William A Goddard, Sen Zhang
Published in
Proceedings of the National Academy of Sciences of the United States of America. Volume 123. Issue 42. Pages e2617489123. Oct 20, 2026. Epub Oct 12, 2026.
Abstract
Single-crystal materials are essential for fundamental catalysis studies and advanced technologies; however, synthesizing single crystals that simultaneously integrate mesoporosity, tunable size, and well-defined surfaces remains challenging. Here, we report a wet-chemical, template-free strategy to synthesize mesoporous quasi-single-crystal CeO2 superparticles (SPs). Operando wide- and small-angle X-ray scattering combined with theoretical modeling reveal a nonclassical growth mechanism driven by the oriented attachment of nanocluster building blocks. This process yields high-surface-area quasi-single crystals that preferentially expose energetically favorable (111) facets on both the external surfaces and internal pore walls, thereby enhancing the stabilization of active sites when used as heterogeneous catalyst supports. Using this approach, we demonstrate broad applicability by synthesizing highly dispersed precious metal-loaded CeO2 (M/CeO2, M = Pd, Pt, Rh, or Ir) and metal-doped CeO2 (Cu-CeO2) SPs. Moreover, Pd/CeO2 SPs exhibit effective stabilization of Pd clusters in CO2 hydrogenation to methanol, delivering a high methanol selectivity of 85% and markedly improved durability compared with conventional supports.
PMID:
42863066
Bibliographic data and abstract were imported from PubMed on 13 Oct 2026.
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