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Abstract The sophisticated hierarchical structure that precisely combines contradictory mechanical and biological characteristics is ideal for biomaterials, but it is challenging to achieve. Herein, we engineer a spatiotemporally hierarchical guided bone regeneration (GBR) membrane by rational bilayer integration of densely porous N-halamine functionalized bacterial cellulose nanonetwork facing the gingiva and loosely porous chitosan-hydroxyapatite composite micronetwork facing the alveolar bone. Our GBR membrane asymmetrically combine stiffness and flexibility, ingrowth barrier and ingrowth guiding, as well as anti-bacteria and cell-activation. The dense layer has a mechanically matched space maintenance capacity toward gingiva, continuously blocks fibroblasts, and prevents bacterial invasion with multiple mechanisms including release-killing, contact-killing, anti-adhesion, and nanopore-blocking; the loose layer is ultra-soft to conformally cover bone surfaces and defect cavity edges, enables ingrowth of osteogenesis-associated cells, and creates a favorable osteogenic microenvironment. As a result, our all-in-one porous membrane possesses full protective abilities in GBR.

Abstract Lithium–sulfur (Li–S) batteries have been regarded as promising next‐generation energy‐storage devices owing to their inherently high theoretical energy density. Unfortunately, the poor capacity and cycling life caused by severe polysulfide shuttle effect and sluggish redox kinetics in sulfur cathodes greatly impede the practical application of Li–S batteries. Herein, a new class of nanonetwork‐structured carbon decorated with oxygen‐vacancy‐containing cerium oxide nanoparticles (NSC–CeO2−x), in which carbon skeleton is composed of highly conductive carbon nanotube core welded by hybrid carbon shell, has been developed via one‐step heating treatment of hybrid molecular brush and further employed as functional interlayer to modify separator of Li–S battery. Owing to the synergistic effect of the highly active CeO2−x nanoparticles and the three‐dimensional carbon nanonetwork in enhancing the preservation of the soluble polysulfides and boosting the redox kinetics of sulfur species, the NSC–CeO2−x significantly promotes the electrochemical performance of sulfur cathode. As a result, the as‐constructed Li–S batteries exhibit an ultrahigh initial sulfur utilization of 92.9% and an extremely large capacity of 751 mA h g−1 at a high rate of 5 C. Remarkably, a stable capacity of 728 mA h g−1 over 300 cycles at 1 C is also achieved.

Abstract With the overconsumption of disposable plastics, there is a considerable emphasis on the recycling of waste plastics to relieve the environmental, economic, and health‐related consequences. Here, a sulfur‐assisted pyrolysis strategy is demonstrated for versatile upcycling of plastics into high‐value carbons with an ultrahigh carbon‐atom recovery (up to 85%). During the pyrolysis process, the inexpensive elemental sulfur molecules are covalently bonded with polymer chains, and then thermally stable intermediates are produced via dehydrogenation and crosslinking, thereby inhibiting the decomposition of plastics into volatile small hydrocarbons. In this manner, the carbon products obtained from real‐world waste plastics exhibit sulfur‐rich skeletons with an enlarged interlayer distance, and demonstrate superior sodium storage performance. It is believed that the present results offer a new solution to alleviate plastic pollution and reduce the carbon footprint of plastic industry.

Heteroatom doping, especially nitrogen doping, has been regarded as an efficient strategy to break through the capacity limitation of carbonaceous anode materials in potassium-ion batteries (PIBs). Constructing edge-nitrogen-rich carbon skeleton with highly exposed active sites and efficient charge transfer is critical for the high performance of nitrogen-doped carbonaceous anode materials. Herein, a kind of ultrahigh edge-nitrogen (up to 16.2 at%) doped carbon nanosheets (ENCNS) has been developed by an efficient assembly of high-nitrogen-ratio melamine (MA) with polyacrylic acid grafted graphene oxide (GO-g-PAA) molecular brushes. The assembled PAA/MA structure facilitates the formation of an edge-nitrogen-rich carbon skeleton during heat treatment, while the highly conductive graphene backbone with a 2D nanomorphology enables shortened ion diffusion pathways and numerous exposed active surfaces. As a result, the ENCNS demonstrate excellent rate performance (up to 144 mAh g−1 at 10 A g−1) and good cycle stability (136 and 100 mAh g−1 after 400 cycles at 5 and 10 A g−1, respectively).

Abstract 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 SiOx 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.