Abstract

Hollow multishelled structures (HoMSs) are a family of hierarchical porous materials featuring multiple independent shells and corresponding in-between cavities. A ‘Cambrian explosion’ of HoMS materials has been witnessed in the past decade owing to breakthroughs in synthetic methods. The precise regulation of structural parameters such as shell numbers, shell porosity, and intershell spacings has enabled the customization of HoMSs for specific applications. With the help of advanced characterizations techniques, in-depth studies of the physical and chemical properties of HoMSs from electronic states, orbital occupation, and lattice structures reveal influences of electron–orbital–lattice interactions in HoMSs on structure–performance correlations, which open myriad opportunities for further exploration of the structural advantages of HoMSs. Hollow multishelled structures (HoMSs), an emergent solid-state material family featuring multiple shells separated by internal cavities, are gaining intensive interest in applications exercising their temporal–spatial ordering or dynamic smart behavior. Although the assembled shell structures and tailored building blocks on the nanometer/micrometer (nano/micro) scale have been extensively studied, understanding of the interplay among the different degrees of freedom (i.e., charge, spin, orbital, and lattice) in HoMSs remains in its infancy. In this review, the new trend in HoMS chemistry regarding the influence of interactions among electron–orbital–lattice on the attractive physicochemical properties of HoMSs is investigated. By demonstrating pioneering work regulating the optical, electronic, catalytic, and magnetic properties of HoMSs, we uncover performance enhancements from an atomic perspective. Hopefully, the new research outlook in HoMSs inspires innovative prospects for the rational design of HoMS materials by using alternative degrees of freedom and/or tailoring their mutual interactions. Hollow multishelled structures (HoMSs), an emergent solid-state material family featuring multiple shells separated by internal cavities, are gaining intensive interest in applications exercising their temporal–spatial ordering or dynamic smart behavior. Although the assembled shell structures and tailored building blocks on the nanometer/micrometer (nano/micro) scale have been extensively studied, understanding of the interplay among the different degrees of freedom (i.e., charge, spin, orbital, and lattice) in HoMSs remains in its infancy. In this review, the new trend in HoMS chemistry regarding the influence of interactions among electron–orbital–lattice on the attractive physicochemical properties of HoMSs is investigated. By demonstrating pioneering work regulating the optical, electronic, catalytic, and magnetic properties of HoMSs, we uncover performance enhancements from an atomic perspective. Hopefully, the new research outlook in HoMSs inspires innovative prospects for the rational design of HoMS materials by using alternative degrees of freedom and/or tailoring their mutual interactions. a synthetic route to produce HoMS materials, followed by a reductive treatment; several processes, including (i) accumulation of precursors in templates by adsorption, (ii) removal of templates by calcination, and (iii) treatment of HoMSs with a reducing agent. an independent physical parameter in the formal description of the state of a physical system. It is used to describe the states of electron, lattice, and orbital in this review, which includes atom/ions with different charges, electrons with different spin states, and orbital moments. essentially the number of different states at a particular energy level that electrons are allowed to occupy (i.e., the number of electron states per unit volume per unit energy). refers to the dynamic response between electrons and lattice vibration in electronically excited condensed matter, which is often accompanied by orbital coupling in correlated materials. here, mainly describes repulsion of the transferred electron by the electrons in the target orbital, which is caused by the Coulombic interaction between electrons. describes the configuration distortion of the electron cloud of coordination of transition metal ions with multiple degenerate states in the ground state in certain situations. focused on the orbital degrees of freedom caused by the lattice change (e.g., perturbations, defects, substitutions), which usually results in varied orbital ordering. a universal and controllable synthetic method to fabricate HoMSs, which starts with the preparation of templates and their precursor enrichment and ends with the removal of templates rich in precursors. Templates in STA play a role in ‘multiple and sequential templating’ to form multishells. a relativistic effect, which describes the interaction between the intrinsic angular momentum and orbital angular momentum of grains. regarded as the intrinsic nature of HoMS materials, which means that matter/energy must sequentially cross every shell of HoMSs in a strict inside-out or outside-in order.

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