Multishell Hollow Metal/Nitrogen/Carbon Dodecahedrons with Precisely Controlled Architectures and Synergistically Enhanced Catalytic Properties

Abstract

Multishell hollow nanoarchitectures are one of the most important branches in the nanomaterial field due to their enormous potential in many fields, but synthesizing them in a well-controlled manner remains challenging. Herein, we present a general strategy for the construction of multishell hollow metal/nitrogen/carbon dodecahedrons (metal@NC) with well-defined and precisely controlled architectures. This strategy is based on the pyrolysis of multilayer solid ZIFs prepared by a step-by-step crystal growth approach, which enables precise control over the shell number and composition of the resultant hollow metal@NC. Impressively, our strategy can be further extended to the synthesis of yolk@multishell hollow structures or multishell hollow structures that are assembled by carbon nanotubes. The multishell hollow structures can efficiently facilitate the mass diffusion, which together with the high dispersity and increased surface area are responsible for their significantly enhanced catalytic performances for the selective hydrogenation of biomass-derived furfural to cyclopentanol when compared with their solid and single-shell counterparts. We anticipate that our general strategy would shed light on the rational design and accurate construction of other complex multishell hollow materials for various important yet challenging applications.

Heat Diffusion‐Induced Gradient Energy Level in Multishell Bisulfides for Highly Efficient Photocatalytic Hydrogen Production

“…[ 5,6,17 ] Among them, precisely designed hollow multishell structures possess attractive characteristics for photocatalysis, including efficient light harvesting, improved charge transfer, and high specific surface area. [ 17,21,27–32 ] Single/multishell hollow spheres, [ 18,33,34 ] hollow cubes, [ 35–37 ] egg yolk shells, [ 27,36,38 ] and other shaped hollow spheres have been reported. [ 19,28,39–41 ] In general, the preparation and synthesis of multishell structured photocatalysts can be divided into three methods according to the template used: hard templating, soft templating, and self‐templating method.…”

“…[ 19,28,39–41 ] In general, the preparation and synthesis of multishell structured photocatalysts can be divided into three methods according to the template used: hard templating, soft templating, and self‐templating method. [ 17,21,26,30,34,40,42–44 ] Hard and soft templating methods generally use rigid materials and micelles as templates. However, these methods usually suffer from complex template removing procedures, nonuniform coatings of particles, and difficulty in selecting templates that are compatible with the targeted material.…”

“…However, these methods usually suffer from complex template removing procedures, nonuniform coatings of particles, and difficulty in selecting templates that are compatible with the targeted material. [ 32–34,42,45 ] In self‐templating preparation strategies, amorphous coordination polymers can be used as synthetic precursors to produce highly complex metal oxide shells by adjusting the composition, offering a clear advantage compared to other templating methods. [ 18,21,33,46 ] The complex multishell hollow materials with heterogeneous structures are expected to provide unique properties and functions because they retain the advantages of a single component while offering synergetic effects between the different components.…”

When hollow multishelled structures (HoMSs) meet metal–organic frameworks (MOFs)

“…Owing to their hierarchical micro/mesoporous structure, high nitrogen doping, large surface area, graphitic structure, and the unique multi-shell hollow structure, the MOF-derived nitrogen-doped carbon HoMS dodecahedrons exhibited a distinguished capacitance of 346 F g À1 at a current density of 0.5 A g À1 , excellent stability with approximately 93% capacitance retention aer 10 000 cycles, and a high energy density of 11.64 W h kg À1 at a power density of 250 W kg À1 as a supercapacitor. 49 Ion-exchange is also an effective way to prepare HoMSs. 50 For instance, precisely controlling the interfacial reaction between the solid MOF and the solution (especially the reagent) can effectively convert MOFs into HoMS materials.…”

Transformation of Stöber Silica Spheres to Hollow Nanocatalysts

“…Furthermore, an increasing surge of interest is also directed to the emerging field of hollow multi‐shelled structures (HoMSs) . Among various applications of HoMSs, catalysis is in the vanguard to apprehend the enormous advantage of hierarchical HoMSs into fabrication of discrete complex nanocatalysts . HoMSs can be discreetly tailored in terms of shell number, shell thickness, inter‐shell spaces, shell porosity, and the composition of each individual shell .…”