Among the rising 2D soft materials, conjugated polymer nanosheets are one of the most promising and new classes of polymeric materials, which are rarely developed because of the challenge in controlling the dimensionality and lack of synthetic strategies. In this study, one kind of sulfur-enriched conjugated polymer nanosheet (2DP-S) with a high aspect ratio of up to ≈400 is successfully synthesized. On the basis of structural characterization, as-prepared 2DP-S possesses the chemical identity of cruciform-fused polymeric backbone consisting of quinoidal polythiophene and poly(p-phenylenevinylene) along horizontal and vertical directions, respectively, by sharing two alternating single–double carbon–carbon bonds in each repeat unit. The unique structural conformation of 2DP-S renders carrier mobilities of up to 0.1 ± 0.05 cm² V⁻¹ s⁻¹, a figure inferred from Terahertz time domain spectroscopy. Moreover, upon thermal treatment, 2DP-S is readily converted into N/S dual-doped porous carbon nanosheets (2DPCs) under ammonia atmosphere, whose N/S ratio can be rationally controlled by adjusting the activation time. The catalytic performance of the oxygen reduction reaction of as-prepared 2DPCs is well tunable by the rationally controlled N/S contents. These results offer a new pathway for exploring heteroatom-doped porous carbons applicable for energy conversion and storage.

The discovery of graphene has triggered great interest in two-dimensional (2D) nanomaterials for scientists in chemistry, physics, materials science, and related areas. In the family of newly developed 2D nanostructured materials, 2D soft nanomaterials, including graphene, B_xC_yN_z nanosheets, 2D polymers, covalent organic frameworks (COFs), and 2D supramolecular organic nanostructures, possess great advantages in light-weight, structural control and flexibility, diversity of fabrication approaches, and so on. These merits offer 2D soft nanomaterials a wide range of potential applications, such as in optoelectronics, membranes, energy storage and conversion, catalysis, sensing, biotechnology, etc. This review article provides an overview of the development of 2D soft nanomaterials, with special highlights on the basic concepts, molecular design principles, and primary synthesis approaches in the context.

A novel phosphorus-containing porous polymer is efficiently prepared from tris(4-vinylphenyl)phosphane by radical polymerization, and it can be easily ionized to form an ionic porous polymer after treatment with hydrogen iodide. Upon ionic exchange, transition-metal-containing anions, such as tetrathiomolybdate (MoS₄ ²⁻) and hexacyanoferrate (Fe(CN)₆ ³⁻), are successfully loaded into the framework of the porous polymer to replace the original iodide anions, resulting in a polymer framework containing complex anions (termed HT-Met, where Met = Mo or Fe). After pyrolysis under a hydrogen atmosphere, the HT-Met materials are efficiently converted at a large scale to metal-phosphide-containing porous carbons (denoted as MetP@PC, where again Met = Mo or Fe). This approach provides a convenient pathway to the controlled preparation of metal-phosphide-loaded porous carbon composites. The MetP@PC composites exhibit superior electrocatalytic activity for the hydrogen evolution reaction (HER) under acidic conditions. In particular, MoP@PC with a low loading of 0.24 mg cm⁻² (on a glass carbon electrode) affords an iR-corrected (where i is current and R is resistance) current density of up to 10 mA cm⁻² at 51 mV versus the reversible hydrogen electrode and a very low Tafel slope of 45 mV dec⁻¹, in rotating disk measurements under saturated N₂ conditions.

Complexation of a boron atom with a series of bidentate heterocyclic ligands successfully gives rise to corresponding BF₂-chelated heteroarenes, which could be considered as novel boron(III)-cored dyes. These dye molecules exhibit planar structures and expanded π-conjugated backbones due to the locked conformation with a boron center. The geometric and electronic structures of these BF₂ complexes can be tailored by embedding heteroatoms in the unique modes to form positional isomer and isoelectronic structures. The structure–property relationship is further elucidated by studying the photophysical properties, electrochemical behavior and quantum-chemical calculations.

Combining the advantages from both porous materials and graphene, porous graphene materials have attracted vast interests due to their large surface areas, unique porous structures, diversified compositions and excellent electronic conductivity. These unordinary features enable porous graphene materials to serve as key components in high-performance electrochemical energy storage and conversion devices such as lithium ion batteries, supercapacitors, and fuel cells. This progress report summarizes the typical fabrication methods for porous graphene materials with micro-, meso-, and macro-porous structures. The structure–property relationships of these materials and their application in advanced electrochemical devices are also discussed.

A series of novel organic conjugated molecules (5a–5d) comprising 2,3-benzopyridiazine as electron-withdrawing core and thiophene derivatives as electron-donating arms have been synthesized successfully in good yields. The ultraviolet-visible (UV-Vis) absorption spectra and fluorescence spectra of 5a–5d revealed that the optical properties are strongly influenced by the interactions between nitrogen and sulfur atoms in the conjugated backbone, as well as the position of the alkyl chains in the thiophene rings. The experimental results and theoretical calculation data clearly indicated that the band gap and the energy levels of LUMO and HOMO could be fine-tuned by the position of alkyl chains in the thiophene rings. Thus, the structure-property correlation of this class of conjugated molecules can be well established.

3D hierarchical tin oxide/graphene frameworks (SnO₂/GFs) were built up by the in situ synthesis of 2D SnO₂/graphene nanosheets followed by hydrothermal assembly. These SnO₂/GFs exhibited a 3D hierarchical porous architecture with mesopores (≈3 nm), macropores (3–6 μm), and a large surface area (244 m² g⁻¹), which not only effectively prevented the agglomeration of SnO₂ nanoparticles, but also facilitated fast ion and electron transport in 3D pathways. As a consequence, the SnO₂/GFs exhibited a high capacity of 830 mAh g⁻¹ for up to 70 charge–discharge cycles at 100 mA g⁻¹. Even at a high current density of 500 mA g⁻¹, a reversible capacity of 621 mAh g⁻¹ could be maintained for SnO₂/GFs with excellent cycling stability. Such performance is superior to that of previously reported SnO₂/graphene and other SnO₂/carbon composites with similar weight contents of SnO₂.

On the basis of our previous communication concerning a new family of thiophene-armed tetraazaanthracene molecules, we present a further intensive investigation on this class of compounds substituted with different alkyl chains and their self-assembled two-dimensional (2D) nanostructures. These tetraazaanthracene molecules with different alkyl chains were prepared in good yields using the synthetic strategy we developed. In addition to the expected typical n-type character, one compound exhibited aggregation behavior upon electrochemical reduction. Moreover, all molecules in the neutral state showed a strong tendency to aggregate in a binary solvent, as confirmed by optical spectral measurements. To investigate such self-assembly behavior, a phase-transfer method with a dichloromethane/methanol (2:3) binary solvent system was used to prepare the nanostructures. By means of atomic force microscopy, transmission electron microscopy, and X-ray diffraction, we found that the morphology of assembled 2D sheet-like structures could be adjusted by varying the alkyl chain. The weak interactions arising from the heteroatoms (N and S) in the conjugated backbones play a key role in the formation and stabilization of layered structures.