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The low cycling efficiency and uncontrolled dendrite growth resulting from an unstable and heterogeneous lithium-electrolyte interface have largely hindered the practical application of lithium metal batteries. In this study, a robust all-organic interfacial protective layer has been developed to achieve a highly efficient and dendrite-free lithium metal anode by the rational integration of porous polymer-based molecular brushes (poly(oligo(ethylene glycol) methyl ether methacrylate)-grafted, hypercrosslinked poly(4-chloromethylstyrene) nanospheres, denoted as xPCMS-g-PEGMA) with single-ion-conductive lithiated Nafion. The porous xPCMS inner cores with rigid hypercrosslinked skeletons substantially increase mechanical robustness and provide adequate channels for rapid ionic conduction, while the flexible PEGMA and lithiated Nafion polymers enable the formation of a structurally stable artificial protective layer with uniform Li

Lithium metal anode has attracted wide research interests because of its very high theoretical capacity and low potential. However, severe safety issues arising from lithium dendrite growth have gripped the throat of the practical application of lithium metal batteries. Herein, a novel superstructured single-ion conducting polymer brush (CNF-g-PSSLi) is proposed as artificial solid electrolyte interphase (SEI) film to inhibit the lithium dendrite growth. The as-obtained CNF-g-PSSLi integrates merits of robust CNF backbone nanonetwork, brush-improved interfacial compatibility, -SO3− group-guided rapid transportation of lithium ions, and -SO3− group-induced electrostatic repulsion against initially formed lithium dendrites. As a result, CNF-g-PSSLi film exhibits good mechanical properties (elasticity modulus = 5.3 GPa) against dendrite growth upon cell cycling, comfortable interfacial contact, and fast ionic transport. Symmetric Li|Li cells with CNF-g-PSSLi as artificial SEI show outstanding plating/stripping stabilities at ultrahigh current densities (20 mA cm−2). In addition, Li|LiFePO4 full cell with Li@CNF-g-PSSLi anode exhibits a long lifespan (300 cycles) with a tiny capacity decay of 0.08% per cycle at a high current density of 5 C. This work could provide an efficient attempt to develop superior artificial SEI films by well-orchestrated macromolecular engineering.

A generalized and facile strategy toward 2D hybrid porous carbons (2DHPCs) with various highly active functional species (e.g. Co, B, and P) is developed via 2D molecular brushes as biomimetic building blocks. The resulting 2DHPCs present superior electrochemical energy conversion and storage properties.

How to successfully achieve the effective construction and precisely control the pore structure of porous carbon materials based on advanced precursors, is still challenging. Herein, a kind of precise organic-inorganic hybrid nanospheres have been designed to synthesize activation-free and high-surface-area microporous carbon materials (MCMs), in which metastable silica-nanonetwork and confined phenyl are formed by the emulsion polymerization of phenyltriethoxysilane. Within this strategy, it is successful to realize the efficient formation of carbon framework, benefiting from the self-crosslinking of confined phenyl and the dual roles of metastable silica-nanonetwork. It is surprising that the silica-nanonetwork can act as the role of template, as well as cross-linker, making the obtained MCMs with high surface area (up to 2614 m2 g−1). Thus, as-prepared MCMs exhibit excellent performance as the electrode materials of supercapacitors in organic electrolyte, i.e. an energy density of 15.36 W h kg−1 at a power density of 27 kW kg−1.

Two-dimensional (2D) porous carbon materials have attracted great attention for various applications in energy conversion/storage, catalysis, and adsorption because of their unique physicochemical ...

Yolk-shell nanostructures have recently attracted tremendous research interests in various areas because of their unique structural merits. Currently, there is an urgent need for developing porous shells with multifunctional features to enhance their performance in various applications. Herein, advanced yolk-shell nanospheres have been facilely prepared by encapsulating silver nanoparticles with porous Janus polymer shells that consist of a hypercrosslinked polystyrene (xPS) outer layer and a tethered poly(acrylic acid) (PAA) brush lining. The xPS outer layer possesses well-developed porosity as mass diffusion pathways. More importantly, the tethered PAA brushes with customized carboxyl groups exhibit great affinity toward specific species (e.g., cationic dyes), leading to their enrichment from the bulk solution into the interior cavity. The unusual combination of highly porous outer layers with customizable inbuilt polymer linings in the porous Janus shells endows them with great promise for synergistically catalytic degradation of cationic dyes.

Nonstoichiometric silica suboxides (SiOx) have been regularly investigated as hopeful anode materials for the substitutions of silicon. However, the inherently poor conductivity of SiOx limits its ...

A novel strategy is developed to produce an FeS-FeNC-decorated hierarchical porous N,S-co-doped carbon (FeS-FeNC@NSC) electrocatalyst via introducing volatile FeCl3 into a porphyrin polymer framework followed by carbonization. The synergistic effect between the FeS nanoparticles and FeNC active sites in FeS-FeNC@NSC is beneficial for enhancing the ORR activity.

Carbon‐based nanomaterials have been regarded as promising non‐noble metal catalysts for renewable energy conversion system (e.g., fuel cells and metal–air batteries). In general, graphitic skeleton and porous structure are both critical for the performances of carbon‐based catalysts. However, the pursuit of high surface area while maintaining high graphitization degree remains an arduous challenge because of the trade‐off relationship between these two key characteristics. Herein, a simple yet efficient approach is demonstrated to fabricate a class of 2D N‐doped graphitized porous carbon nanosheets (GPCNSs) featuring both high crystallinity and high specific surface area by utilizing amine aromatic organoalkoxysilane as an all‐in‐one precursor and FeCl3·6H2O as an active salt template. The highly porous structure of the as‐obtained GPCNSs is mainly attributed to the alkoxysilane‐derived SiO x nanodomains that function as micro/mesopore templates; meanwhile, the highly crystalline graphitic skeleton is synergistically contributed by the aromatic nucleus of the precursor and FeCl3·6H2O. The unusual integration of graphitic skeleton with porous structure endows GPCNSs with superior catalytic activity and long‐term stability when used as electrocatalysts for oxygen reduction reaction and Zn–air batteries. These findings will shed new light on the facile fabrication of highly porous carbon materials with desired graphitic structure for numerous applications., 2D N‐doped graphitized porous carbon nanosheets (GPCNSs) featuring both high crystallinity and high specific surface area are prepared by molecular engineering. The unusual integration of graphitic skeleton with porous structure endows GPCNSs with superior catalytic activity and long‐term stability when used as electrocatalysts for oxygen reduction reaction and Zn–air batteries.

Advanced antimicrobial agents that treat infectious diseases are greatly needed. Various silver-based nanomaterials have been developed and are considered potential candidates for many commercial products, but they lack durability and adequate antibacterial activity. A new class of nanohybrids of silver nanoparticles (AgNPs) grown in-situ on graphene oxide (GO) using a silver ion salt was synthesized by a simple ultrasonic mixing method. The structure and composition of the nanohybrids were investigated by SEM, TEM, FTIR, TGA, XRD and XPS. Results indicated that GO acts not only as a negatively charged macromolecule for capturing Ag+ ions, but also a reducing agent to reduce the Ag+ ions to AgNPs. The heterogeneous structure leads to abundant well-dispersed AgNPs and Ag+ ions on the GO support. The as-prepared nanohybrids make full use of the advantages of both AgNPs and GO-Ag+ salts, leading to improved and long-term antibacterial activity against both S.aureus and E. coli.

A kind of three-dimensionally nanostructured carbon materials (3DNCMs) with tube-in-tube structure was fabricated based on a novel structural design and precise control of ternary bottlebrushes by surface-initiated atom transfer radical polymerization (SI-ATRP). The 3D interconnected network of 3DNCMs consists of the hybrid carbon framework with unique tube-in-tube structure rooting from the ternary bottlebrushes and the microporous carbon shell generated from the carbonization of hypercrosslinked polystyrene (PS). The nanostructure of 3DNCMs can be changed precisely by controlling the ternary bottlebrush structures. The tube-in-tube structure provides 3DNCMs an abundant of microspores within outer amorphous carbon tube and a lot of mesopores from the removal of coated silica, which favor for the hosting of sulfur element. Moreover, carbon nanotubes, the core of the tube-in-tube structure, afford the 3DCNMs with excellent electrical conductivity. In view of the prominent advantages of the tube-in-tube structure, the sulfur cathode based on 3DNCMs hosts shows a remarkable rate capability and reversible discharge capacity of 691 mAh g−1 after 200 cycles at a 2 C current density. We hope this concept of novel design and construction of well-defined nanostructure will pave the way toward high-performance nanoporous carbon materials for energy storage and other practical applications.

Nowadays, it has been more and more important to ingeniously design sheet-like structures since the performance of many modern materials fundamentally depends upon the exploitation of these structures. In this work, we have successfully developed a facile and effective strategy for fabricating a class of 2D porous carbon nanosheets that simultaneously exhibit high surface areas and uniform distribution of metal chalcogenides for superior oxygen evolution reaction. The synthesis of these 2D carbon nanosheets involves the in-situ metal ion adsorption and exchange by the sulfonate radicals of polymer sheets followed by carbonization to form a series of metal chalcogenides loaded porous carbon nanosheets (PCNs/MxSy). The abundant mesopores (e.g., 3–7 nm, 524 m2 g−1) that derived from the spontaneous stacking of flexible GO precursor are advantageous to the exposure of heteroatom sites. The uniform catalytic sites (33.8 nm) formed in-situ effectively avoid the agglomeration of functional components, which are conducive to make full use of catalytic sites and consequently shows excellent OER performance. We hope that our novel strategy can open a new door for the application and innovation of fabricating 2D porous carbon nanosheets in a wide range of areas including energy storage, adsorption, catalysis, separation and so on.

Atom transfer radical polymerization was utilized to prepare well-defined cylindrical molecular bottlebrushes which were employed as building blocks and transformed into porous nanonetwork-structured carbons (PNSCs) via hypercross-linking chemistry and shape-regulated carbonization. The as-prepared PNSCs exhibited a unique nanomorphology-tunable characteristic by simply varying carbonization conditions. Because of their three-dimensional network nanomorphologies with well-developed hierarchical porous structures and conductive carbon framework, the PNSCs demonstrated excellent electrochemical performance in lithium-sulfur batteries.

3D porous carbon networks with highly dispersed SiOx have been successfully prepared by molecular-scale engineering with 1D molecular-brush precursors. Benefiting from the high-porosity interconnected structure and the lithiophilic SiOx nanodomains, the as-obtained composites show great advantages as 3D hosts to achieve stable Li plating/stripping.

Development of efficient, low-cost, and durable electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is scientifically and technologically important for the conversion and storage of renewable energy. Herein, cobalt and nitrogen codoped ultrathin porous carbon nanosheet (Co-N-PCN) is developed by directly carbonizing the graphene oxide sandwiched cobalt ion adsorbed polyaniline-co-polypyrrole (PACP) precursors. The nitrogen-rich PACP favors the formation of abundant Co-Nx-C active species, while the 2D ultrathin nanosheet structure ensures the high exposure of the generated Co-Nx-C active sites to the electrolyte. In addition, the sandwiched graphene acts as the conductive backbone to facilitate fast charge transfer and enhance the electrode conductivity. Benefiting from the synergistic effect, the Co-N-PCN presents superior electrocatalytic properties with low overpotentials and favorable kinetics to Pt and RuO2 as a bifunctional electrocatalyst for ORR and OER. Remarkably, the potential difference of OER and ORR (ΔE = Ej=10 - E1/2) is as low as 0.81 V in 0.1 M KOH, indicating the Co-N-PCN outperforms most of the previously reported bifunctional electrocatalysts.

Nonstoichiometric silicon oxide (SiOx) with high theoretical capacity is a promising anode material for lithium-ion batteries (LIBs). However, volume changes and poor electronic conductivity of SiOx are major impediments to its practical application. The modification of SiOx with carbonaceous materials to accommodate volume variations and improve conductivity is a valuable strategy. Nanonetwork-structured (NNS) carbons have been paid great attention because of their unique three-dimensional structure, and high electronic and ionic conductivity. Incorporating SiOx with well-designed NNS carbons is a promising method to prepare high quality electrode materials for lithium-ion batteries. In this work, a fabrication approach is developed to synthesize a 3D carbon network composed of carbonaceous hybrid nanotubes with well-dispersed SiOx nanodomains (CNT@SiOx–C) from 1D gelable bottlebrushes as network building blocks based on molecular-scale interface engineering technology. Herein, nano-sized SiOx particles are embedded into the carbonaceous matrix to prevent their volume change during cycling. The experimental results indicated that the CNT@SiOx–C presents high reversible capacity, remarkable cycle life and high rate capability due to the high dispersion of nano-sized SiOx and conductive 3D carbon nanonetwork.

A simple yet efficient interfacial crosslinking strategy was developed to fabricate an ultrathin two-dimensional composite in which silicon nanoparticles are uniformly enwrapped in silicon oxycarbide nanosheets (Si/SiOC-NS). The conceptual interfacial crosslinking strategy includes polymeric precipitation at the oil/water interface and simultaneous in situ crosslinking of organosilicon polymers, which overcomes the bottleneck of the conventional sol–gel method to synthesize 2D precursors for SiOC. Moreover, the nanostructures of precursors are well-controlled because of the facile precipitation process. The high aspect ratio of the as-obtained Si/SiOC-NSs exposes a large surface to the electrolyte and facilitates the penetration and diffusion of Li ions around Si nanoparticles. The stable SiOC matrix not only buffers the volume changes of active materials during the charge–discharge process but also contributes to lithium storage. As a result, the anodes of LIBs based on Si/SiOC-NS deliver excellent rate capability (a high capacity retention rate of 65% at 1 A g−1 in comparison with that 0.1 A g−1) and a long lifetime of 500 stable cycles with high capacities at a large current density of 5 A g−1.

Nitrogen-doped porous carbon spheres have attracted great interest in diversified fields owing to their unique physical and chemical properties. However, the synthesis of nitrogen-doped porous carbon spheres with hierarchical superstructures and refined micropore structures is still a challenge. Herein, we develop a molecular-scale silica templating strategy to prepare nitrogen-doped microporous carbon spheres (MCSSs) with high porosity and a well-defined micropore structure. Octa(aminophenyl) polyhedral oligomeric silsesquioxane is used as a building block in MCSS precursors to provide precise molecular-scale templating and nitrogen doping. The morphology of MCSSs can be easily tuned by choosing the proper solvent. The as-synthesized MCSS with a large surface area (2036 m

Porous carbon nanosheets have the advantages of longitudinal continuity, transverse ultrathin, high specific surface area, and surface atomic activity, as well as the synergistic effect of micro and nanoproperties, so the research on their preparation, structure, and properties has attracted wide attention. A series of ultrathin hierarchical porous carbon nanosheets (HPCNs) is fabricated through carbonization of precursors obtained through the Friedel-Crafts reaction-assisted loading of polystyrene on graphene oxide. Hierarchical pore structures consist of three parts: (1) the micropores (1.3 nm), which were provided by porous polystyrene through the Friedel-Crafts reaction; (2) the mesopores (3.8 nm), which were provided by slab pores from the stack of carbon nanosheets; and (3) the pores (5 nm) formed from the random stack of carbon nanosheets. Controlling the carbonization time and temperature adds to a prominent increase in specific surface area from 405.8 to 1420 m

Pyrite FeS2 is a promising alternative to typical intercalation cathodes for rechargeable lithium-ion batteries (LIBs) by virtue of its extremely high theoretical capacity. However, the inferior rate capability and fast capacity degradation caused by the sluggish reaction kinetics and large volume expansion upon lithiation greatly hinder its practical application. Herein, a chemical crosslinking strategy is developed for the synthesis of the yolk-shell pyrite FeS2@porosity-rich sulfur-doped carbon nanonetworks (FeS2@C NNs) as cathode materials for high-performance LIBs. The 3D nanonetwork structure constructed by tight covalent connection of carbon shells can act as highways to facilitate the electron transport kinetics, while the well-orchestrated internal cavities of the yolk-shell nanostructure provide large void space to accommodate the volume expansion of pyrite FeS2. In addition, the porosity-rich characteristic of carbon shells ensures fast pathways for the Li+ diffusion across the shells. As a result, the yolk-shell FeS2@C nanonetworks exhibit excellent high-rate capability (353 mAh g−1 at 10 C) and exceptionally long lifespan of 1000 cycles with a high capacity of 435 mAh g−1 at a large current density of 5 C, which is by far the best of pyrite FeS2-based cathodes for LIBs.

We report the fabrication of porous functional nanonetwork-structured polymers (FNSPs) consisting of poly(acrylic acid) functional cores surrounded by a microporous shell network, via a combination of atom transfer radical polymerization (ATRP) and Friedel–Crafts hyper-cross-linking chemistry. Well-defined molecular brushes with diblock poly(tert-butyl acrylate)-block-polystyrene (PtBA-b-PS) side chains serve as tunable building blocks to synthesize porous networks. The prepared FNSPs demonstrated significantly enhanced adsorption toward basic dyes, up to 767 mg g–1.

A novel class of powdery carbon aerogels (PCAs) has been developed by the union of microemulsion polymerization and hypercrosslinking, followed by carbonization. The resulting aerogels are in a microscale powdery form, demonstrate a well-defined 3D interconnected nanonetwork with hierarchical pores derived from numerous interstitial nanopores and intraparticle micropores, and exhibit high surface area (up to 1969 m2/g). Benefiting from these structural features, PCAs show impressive capacitive performances when utilized as electrodes for organic electrolyte supercapacitors, including large capacitances of up to 152 F/g, high energy densities of 37-15 Wh/kg at power densities of 34–6750 W/kg, and robust cycling stability.

A new class of yolk-shell structured precious metal@microporous polymer nanoparticles has been successfully developed. The polymer shells obtained by hypercrosslinking present well-developed permanent microporosity, controllable thickness, and good mechanical properties, and thus can be utilized to protect the precious metal yolks including Au and Ag nanoparticles from aggregation and inactivation. As a result, compared with unprotected Au nanoparticles, Au@microporous polymer nanoparticles not only present a higher utilization efficiency for the catalytic reduction of nitrobenzene and 4-nitrophenol, but also have a much longer cycling life. Ag@microporous polymer nanoparticles demonstrate highly efficient and long-lasting antibacterial properties, since the microporous shells enable the nanoparticles to release Ag+ from the Ag yolk to the solution in a long-term manner. We hope that our versatile yolk-shell nanoparticles will offer a new thought to solve the structural problems of yolk-shell materials, and thus provide a great opportunity for a spectrum of applications including medicine, catalysis, energy, adsorption and environment.

Carbon aerogels have attracted increasing research interest in a wide range of potential applications owing to their unique structural features, yet the scalable preparation of carbon aerogels configured by nanoporous carbon skeletons with high surface area and precise pore structure is a great challenge. Herein, we report a molecular-scale interface engineering concept for high-throughput and scalable production of well-defined microporous carbon aerogels (MPCAs) based on simple and fast polycondensation (

Porous nanostructured carbon materials exhibit unique structural features such as high surface area and excellent physicochemical stability and have been of significantly scientific and technological interest because of their vital importance in many energy related applications. Synthetic polymers represent a major class of precursors for developing cutting-edge porous carbons, among which conjugated polymers have emerged as an attractive family of carbon precursors. Distinct from those typical polymer precursors, the robust conjugated structure ensures sufficient framework carbonizability and nanoarchitecture-conserving stability during carbonization process, which is crucial to the successful transformation of designed polymer architectures to finally desired carbon nanostructures. Moreover, heteroatom doping (e.g., N, S, B, and metals) or codoping can be naturally integrated into carbon framework directly by using the heteroatom-containing monomers. Especially, using the newly emerged structurally defined carbon-rich conjugated porous networks as precursors, precise control of compositions and structures of carbon materials becomes possible even at the molecular level. In this review, we will highlight recent strategies to the preparation of porous carbon materials with well-defined porous nanostructures using conjugated polymers as versatile precursors. Beginning with a brief introduction to these precursors, including linear-type conjugated polymers and conjugated porous networks, the synthetic techniques for the fabrication of porous nanostructured carbons by direct templating, self-assembly, template-free, chemical activation, and microwave irritation approaches, will be reviewed. Meanwhile, the sophisticated nanomorphologies, precisely controlled porous structures, and custom-designed functionalities of these conjugated-structure-derived carbons, together made them amenable to diverse task-specific applications, such as electrocatalysis, Li-ion batteries, supercapacitors, and adsorption. Finally, a perspective of the research directions in this field will be presented.

Renewable resources (e.g., agricultural byproducts) are widely used in the production of commercial activated carbon, but the activation procedures still have serious drawbacks. Here we develop a green, activation-free, top-down method to prepare high-surface-area carbon materials from agricultural wastes through mechanochemistry. The facile mechanochemical process can smash the monolithic agricultural wastes into tiny microparticles with abundant surfaces and bulk defects, which leads to the generation of well-developed hierarchical porous structures after direct carbonization. The as-obtained carbon materials simultaneously present high surface areas (1771 m2 g–1) and large pore volumes (1.88 cm3 g–1), and thus demonstrate excellent electrochemical performances as the interlayer for lithium–sulfur batteries and much superior creatinine adsorption capabilities to the medicinal charcoal tablets. These results provide a new direction for fabricating high-surface-area porous materials without any toxic reag...

Design and fabrication of the micro/nanostructures of the network units is a critical issue for porous nanonetwork structured materials. Significant progress has been attained in construction of the network units with zero-dimensional spherical shapes. However, owing to the limitations of synthetic methods, construction of porous building blocks in one dimension featuring high aspect ratios for porous nanonetwork structured polymer (PNSP) remains largely unexplored. Here we present the successful design and preparation of PNSP with a novel type of one-dimensional network unit, i.e., microporous heterogeneous nanowire. Well-defined core-shell polymer nanoobjects prepared from a gelable block copolymer, poly(3-(triethoxysilyl)propyl methacrylate)-block-polystyrene are employed as building blocks, and facilely transformed into PNSP via hypercrosslinking of polystyrene shell. The as-prepared PNSP exhibits unique three-dimensional hierarchical nanonetwork morphologies with large surface area. These findings could provide a new avenue for fabrication of unique well-defined PNSP, and thus generate valuable breakthroughs in many applications.

Considering the wide application of nanoporous carbon material in electrochemical double-layer capacitors (EDLCs), the investigation of the structure-performance relationship is critical to constructing suitable nanostructure for high performance EDLCs. Herein, we focus on an important but neglected issue of different applicable pore sizes for electrochemical double-layer (EDL) formation at different current loadings. Small-sized pores with different sizes/distributions are introduced for energy storage while a developed 3D large meso/macroporous structure is constructed for guaranteeing rapid mass transfer. An interesting result is obtained that the applicable pore size greatly depends on the current loadings. For instance, pores larger than 0.59 nm are responsible for EDL formation at a low current density of 0.1 A g −1 in aqueous electrolyte. As increasing the current density to 1 and 10 A g −1 , the most effective pore size increases to larger than 0.73 and 0.93 nm, respectively, which is attributed to the insufficient time of solvent shell removing, squeezing behavior of solvated ions and charge arrangement at higher current densities. These encouraging results may raise concerns about constructing suitable pore size more precisely to realize a target oriented use, particularly those targeting higher power EDLCs applications.

Carbon aerogels and their precursory polymer aerogels are an important class of porous materials, because they have a unique three-dimensional interconnected nanonetwork structure that can minimize diffusive resistance to mass transport. However, production of conventional aerogels in a monolithic form remains problematic, because of risk of explosive polymerization, tedious supercritical/freeze drying steps, extra ball milling, and difficulty in controlling micro/nanostructures. Here we show that novel powdery carbon aerogels and their polymer aerogel precursors have been developed by utilizing shape-persistent nanoparticles as building blocks, followed by hypercrosslinking for forming a well-defined 3D interconnected nanonetwork with numerous interstitial nanopores and intraparticle micropores. The resulting aerogels are in a microscale powdery form. The preparation route is much more feasible for scaling up, due to avoidance of explosive polymerization and facile drying at ambient pressure. By simple carbonization, powdery carbon aerogels can be obtained with a high surface area of 2052 m 2 g −1 . Benefiting from structural advantages, the aerogels demonstrate excellent electrochemical performances in supercapacitors and lithium-sulfur batteries.

The fabrication of advanced hierarchical porous polymers with a unique 3D nanonetwork structure composed of functional core-microporous shell nanoparticles was reported based on the development of a simple and efficient hypercrosslinking-induced self-assembly strategy.

Advances in the performances of many modern materials fundamentally depend upon the exploitation of new micro/nanostructures. Therefore, ingenious design of hierarchical structures through the mimicking of natural systems is of increasing importance. Currently, there is an urgent need for creation of multidimensional carbonaceous structures by integrating a customized hierarchical pore architecture and hybrid carbon framework. Here we report the pioneering fabrication of novel super-hierarchical carbons with a unique carbonaceous hybrid nanotube-interconnected porous network structure by utilizing well-defined carbon nanotube@polystyrene bottlebrushes as building blocks. Hypercrosslinking of such heterogeneous core-shell structured building blocks not only allows for constructing amorphous microporous carbon shells on the surface of graphitic carbon nanotube cores, but also leads to formation of covalently interconnected nanoscale networks. Benefiting from such a well-orchestrated structure, these super-hierarchical carbons exhibit good electrochemical performances. Our findings may open up a new avenue for fabrication of unique and unusual functional carbon materials which possess well-orchestrated structural hierarchy and thus generate valuable breakthroughs in many applications including energy, adsorption, separation, catalysis and medicine.

Functional nanonetwork-structured polymers with inbuilt poly(acrylic acid) linings were successfully synthesized by combining surface-initiated atom transfer radical polymerization (SI-ATRP) and hypercrosslinking chemistry, and demonstrated superior adsorption performances toward basic dyes and heavy metal ions.

As one of the indispensable components in lithium–sulfur batteries, the binders greatly impact battery performance. Herein, we report a new multifunctional supramolecular eutectic liquid (SEL) binder, consisting of diphenylamine (DP) and benzophenone (BP), which enables a strongly improved conductive network and anchored polysulfides for high-performance lithium–sulfur batteries. Compared with the traditional polyvinylidene fluoride (PVDF) binder, the SEL binder demonstrates remarkable improvement in both the mechanical performance and the capacity retention (83% over 200 cycles at 1C).

Herein, we present a universal bottom-up interface self-assembly of hairy nanoparticle strategy for 2D monolayered composite and functional nanosheets, including polymeric composite nanosheets and functional porous polymer and carbon nanosheets. By using diverse hairy nanoparticles as building blocks, a series of 2D monolayered polymeric composite nanosheets was prepared, demonstrating the universality of our strategy. Furthermore, the 2D polymeric composites could be easily transformed into 2D monolayered functional porous polymer and carbon nanosheets. We hope that this strategy will open a new door for the design and fabrication of advanced 2D composite and functional nanosheets and thus provide new opportunities for different fields including the environment, energy, catalysis and medicine.

3D porous carbon networks with highly dispersed SiOx have been successfully prepared by molecular-scale engineering with 1D molecular-brush precursors. Benefiting from the high-porosity interconnected structure and the lithiophilic SiOx nanodomains, the as-obtained composites show great advantages as 3D hosts to achieve stable Li plating/stripping.

Lithium metal batteries have been considerably limited by the problems of uncontrolled dendritic lithium formation and the highly reactive nature of lithium with electrolytes. Herein, we have developed functional porous bilayer composite separators by simply blade-coating polyacrylamide-grafted graphene oxide molecular brushes onto commercial polypropylene separators. Our functional porous bilayer composite separators integrate the lithiophilic feature of hairy polyacrylamide chains and fast electrolyte diffusion pathways with the excellent mechanical strength of graphene oxide nanosheets and thus enable molecular-level homogeneous and fast lithium ionic flux on the surfaces of electrodes. As a result, dendrite-free uniform lithium deposition with a high Coulombic efficiency (98%) and ultralong-term reversible lithium plating/stripping (over 2600 h) at a high current density (2 mA cm−2) are achieved for lithium metal anodes. Remarkably, lithium metal anodes with an unprecedented stability of more than 1900 h cycling at an ultrahigh current density of 20 mA cm−2 are demonstrated., The authors use polyacrylamide grafted graphene oxide as a molecular brush to coat the commercial polypropylene separator. The bilayer design combines lithiophilicity chemistry and high mechanical strength, rendering high performance Li metal anodes and offering a strategy for the design of separators.

Nonstoichiometric silicon oxide (SiO

It remains a formidable challenge to construct advanced adsorbents with superb adsorption, environmental stimuli response, and real-time detection capability for efficiently treating contaminants from complex environmental systems. A novel class of an all-in-one microporous adsorbent that simultaneously has excellent environmental chemosensory responsivity, visual detectivity, superfast micropollutant adsorption, as well as easy regeneration is reported herein. The advanced microporous adsorbent discussed in this study presents a hairy nanospherical morphology composed of a hairy stimuli-responsive polymeric shell and a shell-assisted superadsorptive microporous core. The adsorbent not only exhibits a valuable capability of pollutant detection by visible fluorescence quenching, but can also remove organic micropollutants from polluted water with super-rapid speed (79%, 98%, and 100% of its equilibrium uptake in 7 s, 10 s, and 2 min, respectively) and excellent recyclability (>96%). More importantly, the adsorbent still shows unimpeded adsorption performance in the flow-through adsorption tests (15 mL min-1 ), indicating a very appealing application prospect.

Development of facile synthetic procedures for the fabrication of well-defined hollow carbon nanospheres with a highly porous shell structure is still a very important but really challenging issue. Herein, we report a facile hypercrosslinking strategy to prepare hollow microporous carbon nanospheres with a BET surface area as high as 1166 m2 g−1. SiO2@polystyrene core–shell nanospheres were first prepared, and then were treated through a hypercrosslinking reaction to provide the polystyrene shell with well-developed microporosity. Moreover, the as-constructed hypercrosslinked shell structure ensures a good framework carbonizability and nanostructure inheritability during the high-temperature carbonization process. The porous structure and morphology of the resulting hollow microporous carbon nanospheres can be easily tailored by varying the hypercrosslinking and carbonization conditions. Due to the rational integration of a highly microporous shell structure and a well-defined hollow spherical morphology in the nanometer range, the hollow microporous carbon nanospheres prepared here show good electrochemical performances as active electrodes of lithium ion batteries and supercapacitors.

The interconnected ordered pore channels facilitate faster permeation of Li(+) ions during the charge-discharge process than the isolated ordered pore channels, resulting in significantly enhanced capacities, better rate capabilities and more remarkable cycling stability.

The pioneered construction of novel monodisperse hollow and yolk-shell structured periodic mesoporous polymer nanoparticles was reported by the development of an efficient reactive interface-guided co-assembly approach.