General synthesis of 2D rare-earth oxide single crystals with tailorable facets

Abstract Two-dimensional (2D) rare-earth oxides (REOs) are a large family of materials with various intriguing applications and precise facet control is essential for investigating new properties in the 2D limit. However, a bottleneck remains with regard to obtaining their 2D single crystals with specific facets because of the intrinsic non-layered structure and disparate thermodynamic stability of different facets. Herein, for the first time, we achieve the synthesis of a wide variety of high-quality 2D REO single crystals with tailorable facets via designing a hard-soft-acid-base couple for controlling the 2D nucleation of the predetermined facets and adjusting the growth mode and direction of crystals. Also, the facet-related magnetic properties of 2D REO single crystals were revealed. Our approach provides a foundation for further exploring other facet-dependent properties and various applications of 2D REO, as well as inspiration for the precise growth of other non-layered 2D materials.

[1]  Wei Han,et al.  Recent Advances in 2D Rare Earth Materials , 2020, Advanced Functional Materials.

[2]  N. López,et al.  Dynamic charge and oxidation state of Pt/CeO2 single-atom catalysts , 2019, Nature Materials.

[3]  Chunhua Yan,et al.  Ultrathin 2D Rare‐Earth Nanomaterials: Compositions, Syntheses, and Applications , 2019, Advanced materials.

[4]  Thibault Cheisson,et al.  Rare earth elements: Mendeleev’s bane, modern marvels , 2019, Science.

[5]  K. Fichthorn,et al.  Revisiting the Polyol Synthesis of Silver Nanostructures: Role of Chloride in Nanocube Formation. , 2019, ACS nano.

[6]  Fu-Sheng Guo,et al.  Magnetic hysteresis up to 80 kelvin in a dysprosium metallocene single-molecule magnet , 2018, Science.

[7]  L. Manna,et al.  The Many “Facets” of Halide Ions in the Chemistry of Colloidal Inorganic Nanocrystals , 2018, Chemical reviews.

[8]  Yong Wang,et al.  Activation of surface lattice oxygen in single-atom Pt/CeO2 for low-temperature CO oxidation , 2017, Science.

[9]  J. Paier,et al.  O2 Activation on Ceria Catalysts-The Importance of Substrate Crystallographic Orientation. , 2017, Angewandte Chemie.

[10]  J. Rupp,et al.  Design of Oxygen Vacancy Configuration for Memristive Systems. , 2017, ACS nano.

[11]  C. Monroe,et al.  Observation of a many-body dynamical phase transition with a 53-qubit quantum simulator , 2017, Nature.

[12]  P. W. Hess,et al.  Observation of a discrete time crystal , 2016, Nature.

[13]  Chengjie Sun,et al.  Water bridge coordination on the metal-rich facets of Gd2O3 nanoplates confers high T1 relaxivity. , 2016, Nanoscale.

[14]  Woong Kim,et al.  Generic Synthetic Route to Monodisperse Sub-10 nm Lanthanide Oxide Nanodisks: A Modified Digestive Ripening Process , 2016 .

[15]  Younan Xia,et al.  Shape-Controlled Synthesis of Colloidal Metal Nanocrystals: Thermodynamic versus Kinetic Products. , 2015, Journal of the American Chemical Society.

[16]  Donghai Mei,et al.  Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles , 2015, Nature Communications.

[17]  W. Xu,et al.  Does the 4f-shell contribute to bonding in tetravalent lanthanide halides? , 2014, The Journal of chemical physics.

[18]  Xingjiu Huang,et al.  Sub-20 nm-Fe3O4 square and circular nanoplates: synthesis and facet-dependent magnetic and electrochemical properties. , 2014, Chemical communications.

[19]  F. Krumeich,et al.  Opposite face sensitivity of CeO₂ in hydrogenation and oxidation catalysis. , 2014, Angewandte Chemie.

[20]  Konstantin M. Neyman,et al.  Maximum noble-metal efficiency in catalytic materials: atomically dispersed surface platinum. , 2014, Angewandte Chemie.

[21]  C. Murray,et al.  Mineralizer-Assisted Shape-Control of Rare Earth Oxide Nanoplates , 2014 .

[22]  A. Rogach,et al.  Hierarchical SnO2 Nanostructures: Recent Advances in Design, Synthesis, and Applications , 2014 .

[23]  Yong Jiang,et al.  Pits confined in ultrathin cerium(IV) oxide for studying catalytic centers in carbon monoxide oxidation , 2013, Nature Communications.

[24]  M. Batzill,et al.  Growth of a two-dimensional dielectric monolayer on quasi-freestanding graphene. , 2012, Nature nanotechnology.

[25]  钟业腾,et al.  Controlled synthesis of ultrathin lamellar Eu2O3 nanocrystals: self-assembly of 1D nanowires to 2D nanosheets , 2013 .

[26]  B. Yan,et al.  Salt-effect-based synthesis and anomalous magnetic properties of rare-earth oxide nanosheets with sub-1 nm thickness. , 2012, Chemistry.

[27]  Zhiyu Wang,et al.  Shape Evolution of Highly Crystalline Anatase TiO2 Nanobipyramids , 2011 .

[28]  R. Gorte,et al.  Synthesis and oxygen storage capacity of two-dimensional ceria nanocrystals. , 2011, Angewandte Chemie.

[29]  Younan Xia,et al.  Aqueous-phase synthesis of single-crystal ceria nanosheets. , 2010, Angewandte Chemie.

[30]  M. Ge,et al.  On the origin of ferromagnetism in CeO2 nanocubes , 2008 .

[31]  S. Maensiri,et al.  Egg White Synthesis and Photoluminescence of Platelike Clusters of CeO2 Nanoparticles , 2007 .

[32]  K. Hermansson,et al.  Atomic and electronic structure of unreduced and reduced CeO2 surfaces: a first-principles study. , 2004, The Journal of chemical physics.

[33]  Younan Xia,et al.  Shape-Controlled Synthesis of Gold and Silver Nanoparticles , 2002, Science.

[34]  K. Binnemans,et al.  Narrow band photoluminescence of europium-doped liquid crystals , 2002 .

[35]  Hong,et al.  Epitaxial cubic gadolinium oxide as a dielectric for gallium arsenide passivation , 1999, Science.

[36]  N. Imanaka,et al.  The Binary Rare Earth Oxides. , 1998, Chemical reviews.

[37]  E. Buck,et al.  The chemistry of the light rare‐earth elements as determined by electron energy loss spectroscopy , 1996 .

[38]  G. Ingo,et al.  X‐ray induced reduction effects at CeO2 surfaces: An x‐ray photoelectron spectroscopy study , 1991 .

[39]  G. Thornton,et al.  Satellite structure in the X-ray photoelectron spectra of some binary and mixed oxides of lanthanum and cerium , 1976 .

[40]  A. Relman.  What are acids and bases? , 1954, The American journal of medicine.