Thermal-Rectified Gradient Porous Polymeric Film for Solar-Thermal Regulatory Cooling.

Solar-thermal regulation concerning thermal insulation and solar modulation is pivotal for cooling textiles and smart buildings. Nevertheless, a contradiction arises in balancing the demand to prevent external heat infiltration with the efficient dissipation of excess heat from enclosed spaces. Here, a concentration-gradient polymerization strategy is presented for fabricating a gradient porous polymeric film comprising interconnected polymeric microspheres.

Langmuir-Blodgett Film Formed by Amphiphilic Molecules for Facile and Rapid Construction of Zinc-Iodine Cell.

Zinc-iodine batteries (ZIBs) are promising candidates for ecofriendly, safe, and low-cost energy storage systems, but polyiodide shuttling and the complex cathode fabrication procedures have severely hindered their broader commercial usage. Herein, a protocol is developed using phospholipid-like oleylamine molecules for scalable production of Langmuir-Blodgett films, which allows the facile preparation of ZIB cathodes in less than 1 min. The resulting inhomogeneous cathode allows for the continuous conversion of iodine.

Highly Porous Yet Transparent Mechanically Flexible Aerogels Realizing Solar-Thermal Regulatory Cooling.

The demand for highly porous yet transparent aerogels with mechanical flexibility and solar-thermal dual-regulation for energy-saving windows is significant but challenging. Herein, a delaminated aerogel film (DAF) is fabricated through filtration-induced delaminated gelation and ambient drying. The delaminated gelation process involves the assembly of fluorinated cellulose nanofiber (FCNF) at the solid-liquid interface between the filter and the filtrate during filtration, resulting in the formation of lamellar FCNF hydrogels with strong intra-plane and weak interlayer hydrogen bonding.

Cation Substitution Strategy for Developing Perovskite Oxide with Rich Oxygen Vacancy-Mediated Charge Redistribution Enables Highly Efficient Nitrate Electroreduction to Ammonia.

The electrocatalytic nitrate (NO) reduction reaction (eNITRR) is a promising method for ammonia synthesis. However, its efficacy is currently limited due to poor selectivity, largely caused by the inherent complexity of the multiple-electron processes involved. To address these issues, oxygen-vacancy-rich LaFeMO (M = Co, Ni, and Cu) perovskite submicrofibers have been designed from the starting material LaFeO (LF) by a B-site substitution strategy and used as the eNITRR electrocatalyst.

Bio-Inspired Aerobic-Hydrophobic Janus Interface on Partially Carbonized Iron Heterostructure Promotes Bifunctional Nitrogen Fixation.

Competition from hydrogen/oxygen evolution reactions and low solubility of N in aqueous systems limited the selectivity and activity on nitrogen fixation reaction. Herein, we design an aerobic-hydrophobic Janus structure by introducing fluorinated modification on porous carbon nanofibers embedded with partially carbonized iron heterojunctions (Fe C/Fe@PCNF-F). The simulations prove that the Janus structure can keep the internal Fe C/Fe@PCNF-F away from water infiltration and endow a N molecular-concentrating effect, suppressing the competing reactions and overcoming the mass-transfer limitations to build a robust "quasi-solid-gas" state micro-domain around the catalyst surface.

Visible-Light Transparent, Ultrastretchable, and Self-Healable Semicrystalline Fluorinated Ionogels for Underwater Strain Sensing.

The development of ultrastretchable ionogels with a combination of high transparency and unique waterproofness is central to the development of emerging skin-inspired sensors. In this study, an ultrastretchable semicrystalline fluorinated ionogel (SFIG) with visible-light transparency and underwater stability is prepared through one-pot copolymerization of acrylic acid and fluorinated acrylate monomers in a mixed solution of poly(ethylene oxide) (PEO) and fluorinated ionic liquids. Benefiting from the formation of the PEO-chain semicrystalline microstructures and the abundant noncovalent interactions (reversible hydrogen bonds and ion-dipole interactions) in an ionogel, SFIG is rendered with room-temperature stable cross-linking structures, providing high mechanical elasticity as well as high chain segment dynamics for self-healing and efficient energy absorption during the deformation.

Soluble porous organic cages as homogenizers and electron-acceptors for homogenization of heterogeneous alloy nanoparticle catalysts with enhanced catalytic activity.

The creation of ultrafine alloy nanoparticles (<5 nm) that can maintain surface activity and avoid aggregation for heterogeneous catalysis has received much attention and is extremely challenging. Here, ultrafine PtRh alloy nanoparticles imprisoned by the cavities of reduced chiral covalent imine cage (PtRh@RCC3) are prepared successfully by an organic molecular cage (OMC) confinement strategy, while the soluble RCC3 can act as a homogenizer to homogenize the heterogeneous PtRh alloy in solution. Moreover, the X-ray absorption near-edge structure (XANES) results show that the RCC3 can act as an electron-acceptor to withdraw electrons from Pt, leading to the formation of higher valence Pt atoms, which is beneficial to improving the catalytic activity for the reduction of 4-nitrophenol.

A Universal Spinning-Coordinating Strategy to Construct Continuous Metal-Nitrogen-Carbon Heterointerface with Boosted Lithium Polysulfides Immobilization for 3D-Printed LiS Batteries.

Constructing intimate coupling between transition metal and carbon nanomaterials is an effective means to achieve strong immobilization of lithium polysulfides (LiPSs) in the applications of lithium-sulfur (LiS) batteries. Herein, a universal spinning-coordinating strategy of constructing continuous metal-nitrogen-carbon (MNC, M = Co, Fe, Ni) heterointerface is reported to covalently bond metal nanoparticles with nitrogen-doped porous carbon fibers (denoted as M/MN@NPCF). Guided by theoretical simulations, the Co/CoN@NPCF hybrid is synthesized as a proof of concept and used as an efficient sulfur host material.

Semicrystalline Conjugated Polymers with Well-Defined Active Sites for Nitrogen Fixation in a Seawater Electrolyte.

Faradaic efficiency for the nitrogen reduction reaction (NRR) is often limited by low N solubility in the electrolyte, while a large number of intimate contacts between the electrolyte and solid catalyst can also inevitably sacrifice many active sites for the NRR. Here, it is reported that a "quasi-gas-solid" interface formed in donor-acceptor-based conjugated polymers (CPs) is beneficial to boosting the NRR process and at the same time suppressing the competing hydrogen evolution reaction. Of particular interest, it is found that a semicrystalline CP catalyst, SC-PBDT-TT, exhibits a high Faradaic efficiency of up to 60.

Homogeneous electric field and Li flux regulation in three-dimensional nanofibrous composite framework for ultra-long-life lithium metal anode.

Lithium (Li) metal is considered as the best anode candidate for next-generation high-energy batteries due to its ultralow electrochemical potential and extremely high theoretical capacity. However, issues arising from the undesired growth of lithium dendrites and infinite volumetric change have seriously hindered the practical application of lithium metal batteries (LMBs). Here, we designed a super-lithiophilic amorphous zinc oxide-doped carbon nanofiber framework with uniformly-distributed and parallel multichannels (MCCNF@ZnO) to achieve the homogeneous distribution of electric field and Li flux.

Recent advances and perspectives of 3D printed micro-supercapacitors: from design to smart integrated devices.

3D-printed micro-supercapacitors (MSCs) have emerged as the ideal candidates for energy storage devices owing to their unique characteristics of miniaturization, structural diversity, and integration. Exploring the 3D printing technology for various materials and architectures of MSCs is key to realizing customization and optimizing the performance of 3D-printed MSCs. In this review, we summarize the latest progress in 3D-printed MSCs with regards to general printing approaches, printable materials, and rational design considerations.

Asymmetric Sodiophilic Host Based on a Ag-Modified Carbon Fiber Framework for Dendrite-Free Sodium Metal Anodes.

Sodium (Na) metal is considered a promising anode material for high-energy Na batteries due to its high theoretical capacity and abundant resources. However, uncontrollable dendrite growth during the repeated Na plating/stripping process leads to the issues of low Coulombic efficiency and short circuits, impeding the practical applications of Na metal anodes. Herein, we propose a silver-modified carbon nanofiber (CNF@Ag) host with asymmetric sodiophilic features to effectively improve the deposition behavior of Na metal.

Gradient phosphorus-doping engineering and superficial amorphous reconstruction in NiFeO nanoarrays to enhance the oxygen evolution electrocatalysis.

A better solid-liquid-gas three-phase boundary is vital for low energy cost oxygen evolution reaction (OER), making the designed regulation of interfacial atmosphere necessary. Herein, we find that the OER electrocatalysis can be dramatically improved by synergistically forming disordered electronic structures and superficial amorphous layers, as superficial oxyhydroxide, phosphorus-doped NiFe2O4 nanoarrays on nitrogen-doped carbon nanofibers (OP-NiFe2O4/NCNFs). Unveiled by the depth-profiling analysis from the X-ray photoelectron spectroscopy, the contents of phosphorous doping in the OP-NiFe2O4 nanoarrays change dynamically from outside to inside due to its in situ superficial reconstruction into the oxyhydroxide layer, thereby accelerating electron transfer between heterogeneous phases.

Tracking Airborne Molecules from Afar: Three-Dimensional Metal-Organic Framework-Surface-Enhanced Raman Scattering Platform for Stand-Off and Real-Time Atmospheric Monitoring.

Stand-off Raman spectroscopy combines the advantages of both Raman spectroscopy and remote detection to retrieve molecular vibrational fingerprints of chemicals at inaccessible sites. However, it is currently restricted to the detection of pure solids and liquids and not widely applicable for dispersed molecules in air. Herein, we realize real-time stand-off SERS spectroscopy for remote and multiplex detection of atmospheric airborne species by integrating a long-range optic system with a 3D analyte-sorbing metal-organic framework (MOF)-integrated SERS platform.

Ion-Selective Polyamide Acid Nanofiber Separators for High-Rate and Stable Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have attracted great attention because of their high energy density and high theoretical capacity. However, the "shuttle effect" caused by the dissolution of polysulfides in liquid electrolytes severely hinders their practical applications. Herein, we originally propose a carboxyl functional polyamide acid (PAA) nanofiber separator with dual functions for inhibiting polysulfide transfer and promoting Li migration via a one-step electrospinning synthesis method.

Shape-dependent thermo-plasmonic effect of nanoporous gold at the nanoscale for ultrasensitive heat-mediated remote actuation.

Nanoporous gold (NPG) promises efficient light-to-heat transformation, yet suffers limited photothermal conversion efficiency owing to the difficulty in controlling its morphology for the direct modulation of thermo-plasmonic properties. Herein, we showcase a series of shape-controlled NPG nanoparticles with distinct bowl- (NPG-B), tube- (NPG-T) and plate-like (NPG-P) structures for quantitative temperature regulation up to 140 °C in <1 s using laser irradiation. Notably, NPG-B exhibits the highest photothermal efficiency of 68%, which is >12 and 39 percentage points better than those of other NPG shapes (NPG-T, 56%; NPG-P, 49%) and Au nanoparticles (29%), respectively.

Sulfur-Deficient Bismuth Sulfide/Nitrogen-Doped Carbon Nanofibers as Advanced Free-Standing Electrode for Asymmetric Supercapacitors.

The use of free-standing carbon-based hybrids plays a crucial role to help fulfil ever-increasing energy storage demands, but is greatly hindered by the limited number of active sites for fast charge adsorption/desorption processes. Herein, an efficient strategy is demonstrated for making defect-rich bismuth sulfides in combination with surface nitrogen-doped carbon nanofibers (dr-Bi S /S-NCNF) as flexible free-standing electrodes for asymmetric supercapacitors. The dr-Bi S /S-NCNF composite exhibits superior electrochemical performances with an enhanced specific capacitance of 466 F g at a discharge current density of 1 A g .

Engineering a nanotubular mesoporous cobalt phosphide electrocatalyst by the Kirkendall effect towards highly efficient hydrogen evolution reactions.

Tailoring the size and controlling the morphology of particular nano-architectures are considered as two promising strategies to improve the catalytic performance of metal nanocrystals towards hydrogen evolution reactions (HERs). Herein, mesoporous cobalt phosphide nanotubes (CoP-NTs) with a three-dimensional network structure have been obtained through a facile and efficient electrospinning technique combined with thermal stabilization and phosphorization treatments. The thermal stabilization process has been demonstrated to play a key role in the morphological tailoring of CoO nanotubes (CoO-NTs).

Bionanofiber Assisted Decoration of Few-Layered MoSe Nanosheets on 3D Conductive Networks for Efficient Hydrogen Evolution.

Molybdenum diselenide (MoSe ) has emerged as a promising electrocatalyst for hydrogen evolution reaction (HER). However, its properties are still confined due to the limited active sites and poor conductivity. Thus, it remains a great challenge to synergistically achieve structural and electronic modulations for MoSe -based HER catalysts because of the contradictory relationship between these two characteristics.

Elastic Carbon Aerogels Reconstructed from Electrospun Nanofibers and Graphene as Three-Dimensional Networked Matrix for Efficient Energy Storage/Conversion.

Three-dimensional (3D) all-carbon nanofibrous aerogels with good structural stability and elasticity are highly desirable in flexible energy storage/conversion devices. Hence, an efficient surface-induced co-assembly strategy is reported for the novel design and reconstruction of electrospun nanofibers into graphene/carbon nanofiber (CNF) composite aerogels (GCA) with hierarchical structures utilizing graphene flakes as cross-linkers. The as-obtained GCA monoliths possess interconnected macropores and integrated conductive networks, which exhibit high elasticity and great structural robustness.

Biomass-Derived Nitrogen-Doped Carbon Nanofiber Network: A Facile Template for Decoration of Ultrathin Nickel-Cobalt Layered Double Hydroxide Nanosheets as High-Performance Asymmetric Supercapacitor Electrode.

The development of biomass-based energy storage devices is an emerging trend to reduce the ever-increasing consumption of non-renewable resources. Here, nitrogen-doped carbonized bacterial cellulose (CBC-N) nanofibers are obtained by one-step carbonization of polyaniline coated bacterial cellulose (BC) nanofibers, which not only display excellent capacitive performance as the supercapacitor electrode, but also act as 3D bio-template for further deposition of ultrathin nickel-cobalt layered double hydroxide (Ni-Co LDH) nanosheets. The as-obtained CBC-N@LDH composite electrodes exhibit significantly enhanced specific capacitance (1949.

A CNT@MoSe2 hybrid catalyst for efficient and stable hydrogen evolution.

Exploration of high-efficiency Pt-free electrochemical catalysts for hydrogen evolution reaction (HER) is considered as a great challenge for the development of sustainable and carbon dioxide free energy conversion systems. In this work, a unique hierarchical nanostructure of few-layered MoSe2 nanosheets perpendicularly grown on carbon nanotubes (CNTs) is synthesized through a one-step solvothermal reaction. This rationally designed architecture based on a highly conductive CNT substrate possesses fully exposed active edges and open structures for fast ion/electron transfer, thus leading to remarkable HER activity with a low onset potential of -0.

Polymer/Carbon-Based Hybrid Aerogels: Preparation, Properties and Applications.

Aerogels are synthetic porous materials derived from sol-gel materials in which the liquid component has been replaced with gas to leave intact solid nanostructures without pore collapse. Recently, aerogels based on natural or synthetic polymers, called polymer or organic aerogels, have been widely explored due to their porous structures and unique properties, such as high specific surface area, low density, low thermal conductivity and dielectric constant. This paper gives a comprehensive review about the most recent progresses in preparation, structures and properties of polymer and their derived carbon-based aerogels, as well as their potential applications in various fields including energy storage, adsorption, thermal insulation and flame retardancy.

Flexible Hybrid Membranes with Ni(OH)2 Nanoplatelets Vertically Grown on Electrospun Carbon Nanofibers for High-Performance Supercapacitors.

The practical applications of transition metal oxides and hydroxides for supercapacitors are restricted by their intrinsic poor conductivity, large volumetric expansion, and rapid capacitance fading upon cycling, which can be solved by optimizing these materials to nanostructures and confining them within conductive carbonaceous frameworks. In this work, flexible hybrid membranes with ultrathin Ni(OH)2 nanoplatelets vertically and uniformly anchored on the electrospun carbon nanofibers (CNF) have been facilely prepared as electrode materials for supercapacitors. The Ni(OH)2/CNF hybrid membranes with three-dimensional macroporous architectures as well as hierarchical nanostructures can provide open and continuous channels for rapid diffusion of electrolyte to access the electrochemically active Ni(OH)2 nanoplatelets.