Hierarchical porous carbons with layer-by-layer motif architectures from confined soft-template self-assembly in layered materials

Abstract

Although various two-dimensional (2D) nanomaterials have been explored as promising capacitive materials due to their unique layered structure, their natural restacking tendency impedes electrolyte transport and significantly restricts their practical applications. Herein, we synthesize all-carbon layer-by-layer motif architectures by introducing 2D ordered mesoporous carbons (OMC) within the interlayer space of 2D nanomaterials. As a proof of concept, MXenes are selected as 2D hosts to design 2D–2D heterostructures. Further removing the metal elements from MXenes leads to the formation of all-carbon 2D–2D heterostructures consisting of alternating layers of MXene-derived carbon (MDC) and OMC. The OMC layers intercalated with the MDC layers not only prevent restacking but also facilitate ion diffusion and electron transfer. The performance of the obtained hybrid carbons as supercapacitor electrodes demonstrates their potential for upcoming electronic devices. This method allows to overcome the restacking and blocking of 2D nanomaterials by constructing ion-accessible OMC within the 2D host material.

Nitrogen Codoped Unique Carbon with 0.4 nm Ultra‐Micropores for Ultrahigh Areal Capacitance Supercapacitors

“…Moreover, when the ultra‐micropore total volume of the carbon microspheres increased from 0.006 to 0.016 cm 3 g −1 , the gravimetric capacitance increased from 147 to 294 F g −1 . More importantly, due to the narrow size distribution of ultra‐microporous carbon than typical carbon‐based electrodes, the area capacitance of obtained sample reaches the value of 330 µF cm −2 , significantly higher than that of previously reported electrode materials . This work provides a better understanding of the correlation between ultra‐microporous structures and their capacitance.…”

“…For such pore diameter, a slightly increasing coverage of the inner ultra‐micropore is more suitable to the ion coming in and out from the pore channel. And due to the ultra‐microporous carbon possesses a much lower surface area than other typical carbon‐based electrodes (1500–2000 m 2 g −1 ), the area‐normalized capacitance ( C a , µF cm −2 ) of the CM‐D electrode is up to 330 µF cm −2 at 0.1 A g −1 , significantly higher than those from carbon‐based electrodes, such as activated carbons (10–25 µF cm −2 ), carbide‐derived carbons (5–22 µF cm −2 ), MXene‐derived carbons (24 µF cm −2 ), nitrogen‐enriched carbon materials (73.4 µF cm −2 ), and functionalized graphene sheets (54.1 µF cm −2 ) …”

Confined Self‐Assembly in Two‐Dimensional Interlayer Space: Monolayered Mesoporous Carbon Nanosheets with In‐Plane Orderly Arranged Mesopores and a Highly Graphitized Framework

“…[19] After carbonization, however, the (001) peak becomes unclear, suggesting disordering/distortion of the interlayer distance of MONT.As shown in the scanning electron microscopy (SEM) image (Figure 2a), the OMCNS exhibit sheet-like shape with al ateral extent of several micrometers.S uch al ayered structure is important evidence that the carbonization process occurs inside the interlayer space.A ss hown in Figure 2b, these carbon nanosheets possess good electron transparency, indicating that they are very thin. Since the interlayer space is only about 0.87 nm, it is speculated that the F127 micelles@Resol are in ellipsoidal shape.…”

“…[4][5][6] However,t he applications of 2Dstructured carbon materials are mostly hampered by the severe aggregation, especially after processing into ac ompressed electrode,w hich cause limitations,n amely ion accessibility,diffusion, and mass transportation. [19] Thei ntercalated OMC layers not only facilitate ion diffusion but also promote electron transfer,[*] Dr. [9][10][11][12][13][14][15][16][17] Thecommonly used methods include preparing crumpled nanosheets or incorporating small dimensional nanoparticles within the nanosheets, which can generate interlayer space when being packed together; [9][10][11][12][13] however,t he curved interlayer spacer and the randomly distributed interlayer spacers will lead to acomplex and even blocked pathway for ion diffusion, reducing the ionaccessible surface area.…”

Progress of Nanostructured Electrode Materials for Supercapacitors

“…In our group, Wang et al synthesized the all-carbon layer-by-layer motif architectures by introducing 2D ordered mesoporous carbons (OMC) within the interlayer space. [110] In this work, MXenes was selected as 2D host to design the 2D-2D heterostructures. The all-carbon 2D-2D heterostructures consisted of alternating layers of MXenes-derived carbon (MDC) and OMC have achieved by removing the metal elements from MXenes.…”