Large-Scale Synthesis of MOF-Derived Superporous Carbon Aerogels with Extraordinary Adsorption Capacity for Organic Solvents

Carbon aerogels (CAs) with 3D interconnected networks hold promise for application in areas such as pollutant treatment, energy storage, and electrocatalysis. In spite of this, it remains challenging to synthesize high-performance CAs on a large scale in a simple and sustainable manner. We report an eco-friendly method for the scalable synthesis of ultralight and superporous CAs by using cheap and widely available agarose (AG) biomass as the carbon precursor. Zeolitic imidazolate framework-8 (ZIF-8) with high porosity is introduced into the AG aerogels to increase the specific surface area and enable heteroatom doping. After pyrolysis under inert atmosphere, the ZIF-8/AG-derived nitrogen-doped CAs show a highly interconnected porous mazelike structure with a low density of 24 mg cm⁻³, a high specific surface area of 516 m² g⁻¹, and a large pore volume of 0.58 cm⁻³ g⁻¹. The resulting CAs exhibit significant potential for application in the adsorption of organic pollutants.     

Hierarchically Ordered Porous Carbon with Atomically Dispersed FeN4 for Ultraefficient Oxygen Reduction Reaction in Proton-Exchange Membrane Fuel Cells

The low catalytic activity and poor mass transport capacity of platinum group metal free (PGM-free) catalysts seriously restrict the application of proton-exchange membrane fuel cells (PEMFCs). Catalysts derived from Fe-doped ZIF-8 could in theory be as active as Pt/C thanks to the high intrinsic activity of FeN₄; however, the micropores fail to meet rapid mass transfer. Herein, an ordered hierarchical porous structure is introduced into Fe-doped ZIF-8 single crystals, which were subsequently carbonized to obtain an FeN₄-doped hierarchical ordered porous carbon (FeN₄/HOPC) skeleton. The optimal catalyst FeN₄/HOPC-c-1000 shows excellent performance with a half-wave potential of 0.80 V in 0.5 m H₂SO₄ solution, only 20 mV lower than that of commercial Pt/C (0.82 V). In a real PEMFC, FeN₄/HOPC-c-1000 exhibits significantly enhanced current density and power density relative to FeN₄/C, which does not have an optimized pore structure, implying an efficient utilization of the active sites and enhanced mass transfer to promote the oxygen reduction reaction (ORR).     

Toughening a Self-Healable Supramolecular Polymer by Ionic Cluster-Enhanced Iron-Carboxylate Complexes

Supramolecular polymers that can heal themselves automatically usually exhibit weakness in mechanical toughness and stretchability. Here we exploit a toughening strategy for a dynamic dry supramolecular network by introducing ionic cluster-enhanced iron-carboxylate complexes. The resulting dry supramolecular network simultaneous exhibits tough mechanical strength, high stretchability, self-healing ability, and processability at room temperature. The excellent performance of these distinct supramolecular polymers is attributed to the hierarchical existence of four types of dynamic combinations in the high-density dry network, including dynamic covalent disulfide bonds, noncovalent H-bonds, iron-carboxylate complexes and ionic clustering interactions. The extremely facile preparation method of this self-healing polymer offers prospects for high-performance low-cost material among others for coatings and wearable devices.     

Facile Synthesis of Hierarchical Nanosized Single-Crystal Aluminophosphate Molecular Sieves from Highly Homogeneous and Concentrated Precursors

The synthesis of hierarchical nanosized zeolite materials without growth modifiers and mesoporogens remains a substantial challenge. Herein, we report a general synthetic approach to produce hierarchical nanosized single-crystal aluminophosphate molecular sieves by preparing highly homogeneous and concentrated precursors and heating at elevated temperatures. Accordingly, aluminophosphate zeotypes of LTA (8-rings), AEL (10-rings), AFI (12-rings), and -CLO (20-rings) topologies, ranging from small to extra-large pores, were synthesized. These materials show exceptional properties, including small crystallites (30–150 nm), good monodispersity, abundant mesopores, and excellent thermal stability. A time-dependent study revealed a non-classical crystallization pathway by particle attachment. This work opens a new avenue for the development of hierarchical nanosized zeolite materials and understanding their crystallization mechanism.     

Stimuli-Responsive Circularly Polarized Organic Ultralong Room Temperature Phosphorescence

Purely organic materials showing room temperature phosphorescence (RTP) and ultralong RTP (OURTP) have recently attracted much attention. However, it is challenging to integrate circularly polarized luminescence (CPL) into RTP/OURTP. Here, we show a strategy to realize CPL-active OURTP (CP-OURTP) by binding an achiral phosphor group directly to the chiral center of an ester chain. Engineering of this flexible chiral chain enables efficient chirality transfer to carbazole aggregates, resulting in strong CP-OURTP with a lifetime of over 0.6 s and dissymmetry factor of 2.3×10⁻³ after the conformation regulation upon photo-activation. The realized CP-OURTP is thus stable at room temperature but can be deactivated quickly at 50 °C to CP-RTP with high CPL stability during the photo-activation/thermal-deactivation cycles. Based on this extraordinary photo/thermal-responsive and highly reversible CP-OURTP/RTP, a CPL-featured lifetime-encrypted combinational logic device has been successfully established.     

Li/Garnet Interface Stabilization by Thermal-Decomposition Vapor Deposition of an Amorphous Carbon Layer

Applying interlayers is the main strategy to address the large area specific resistance (ASR) of Li/garnet interface. However, studies on eliminating the Li₂CO₃ and LiOH interfacial lithiophobic contaminants are still insufficient. Here, thermal-decomposition vapor deposition (TVD) of a carbon modification layer on Li_6.75La₃Zr_1.75Ta_0.25O₁₂ (LLZTO) provides a contaminant-free surface. Owing to the protection of the carbon layer, the air stability of LLZTO is also improved. Moreover, owing to the amorphous structure of the low graphitized carbon (LGC), instant lithiation is achieved, and the ASR of the Li/LLZTO interface is reduced to 9 Ω cm². Lithium volatilization and Zr⁴⁺ reduction are also controllable during TVD. Compared with its high graphitized carbon counterpart (HGC), the LGC-modified Li/LLZTO interface displays a higher critical current density of 1.2 mA cm⁻², as well as moderate Li plating and stripping, which provides enhanced polarization voltage stability.