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Rechargeable aqueous zinc‐iodine batteries (ZIBs) are considered a promising newly‐developing energy‐storage system, but the corrosion and dendritic growth occurring on the anode seriously hinder their future application. Here, the corrosion mechanism of polyiodide is revealed in detail, showing that it can spontaneously react with zinc and cause rapid battery failure. To address this issue, a sulfonate‐rich ion‐exchange layer (SC‐PSS) is purposely constructed to modulate the transport and reaction chemistry of polyiodide and Zn2+ at the zinc/electrolyte interface. The resulting ZIBs can work properly over 6000 cycles with high‐capacity retention (90.2%) and reversibility (99.89%). Theoretical calculations and experimental characterization reveal that the SC‐PPS layer blocks polyiodide permeation through electrostatic repulsion, while facilitating desolvation of Zn(H2O)62+ and restricting undesirable 2D diffusion of Zn2+ by chemisorption. [ABSTRACT FROM AUTHOR]

Solar energy-driven interfacial evaporators are promising candidates to produce fresh water from seawater and wastewater. However, the photothermal layer of the evaporators under water and the homogeneous water transport layer cause undesired heat loss and inadequate water pumping, reducing the evaporation efficiency. Herein, we report on an advanced aerogel-based interfacial evaporator with self-floating photothermal layer and gradient structured water transport layer. The photothermal aerogels are prepared by assembling phenolic nanoparticles with increasing sizes from the bottom to the top, followed by surface hydrophobic modification and photothermal layer deposition on the large-pore side of the aerogels. The hydrophilic gradient phenolic matrix provides sustained water supply and facilitates water pumping by gradient capillary effect. Meanwhile, the large-pore and hydrophobic photothermal layer can enhance light absorption by multiple scattering and self-float above water for thermal localization. Thus, the obtained aerogels achieve high light absorption of 96.8 %, excellent evaporation rate of 1.64 kg m−2 h−1 under 1 sun irradiation and good long-term stability for at least 30 cycles without solute accumulation. Moreover, the produced distilled water from seawater and acidic/alkaline wastewater is in high quality and meets the World Health Organization's stipulated safe drinking water standards. [Display omitted] • Gradient phenolic aerogels with self-floating photothermal layer are prepared. • The aerogels possess high photothermal conversion and enhanced water pumping. • Highly efficient and stable water evaporation performances are achieved. • Fresh water can be produced from seawater and acidic/alkaline wastewater. [ABSTRACT FROM AUTHOR]

The development of aqueous rechargeable zinc‐iodine (Zn‐I2) batteries is still plagued by the polyiodide shuttle issue, which frequently causes batteries to have inadequate cycle lifetimes. In this study, quaternization engineering based on the concept of "electric double layer" is developed on a commercial acrylic fiber skeleton ($1.55–1.7 kg−1) to precisely constrain the polyiodide and enhance the cycling durability of Zn‐I2 batteries. Consequently, a high‐rate (1 C–146.1 mAh g−1, 10 C–133.8 mAh g−1) as well as, ultra‐stable (2000 cycles at 20 C with 97.24% capacity retention) polymer‐based Zn‐I2 battery is reported. These traits are derived from the strong electrostatic interaction generated by quaternization engineering, which significantly eliminates the polyiodide shuttle issue and simultaneously realizes peculiar solution‐based iodine chemistry (I−/I3−) in Zn‐I2 batteries. The quaternization strategy also presents high practicability, reliability, and extensibility in various complicated environments. In particular, cutting‐edge Zn‐I2 batteries based on the concept of derivative material (commercially available quaternized resin) demonstrate ≈100% capacity retention over 17 000 cycles at 20 C. This work provides a general and fresh insight into the design and development of large‐scale, low‐cost, and high‐performance zinc‐iodine batteries, as well as, other novel iodine storage systems. [ABSTRACT FROM AUTHOR]

Keywords: anodic protection; ion-exchange layers; polyiodide corrosion mechanism; zinc-iodine batteries EN anodic protection ion-exchange layers polyiodide corrosion mechanism zinc-iodine batteries 1 1 1 04/10/23 20230406 NES 230406 B Zinc-Iodine Batteries b Polyiodide shuttling and dendritic growth are the major constraints for developing zinc-iodine cells. Tuning Ion Transport at the Anode-Electrolyte Interface via a Sulfonate-Rich Ion-Exchange Layer for Durable Zinc-Iodine Batteries (Adv. In article number 2203790, Jiajia Huang, Feili Lai, and co-workers revelation the corrosion mechanism of polyiodide on zinc, and develop a sulfonate-rich ion-exchange fiber layer to prevent polyiodide permeation. [Extracted from the article]

The practical application of Zn metal anodes is currently hindered by uncontrolled dendritic growth and water‐induced parasitic reactions that are closely related to the solvation structure and interfacial transport kinetics of Zn2+. Herein, a facile interface self‐gelation strategy is proposed to stabilize Zn anode by introducing ‐OH‐rich silica aerogel (HSA) on Zn anode surface. The unique interconnected network structure and strong hydrophilia of HSA made the aqueous electrolyte near Zn anode gel rapidly and spontaneously, resulting in the formation of a water‐poor gel interface layer. The interface layer can effectively accelerate the desolvation process and reduce water molecule activity near anode surface through hydrogen bonding interaction, thus achieving rapid Zn migration kinetics and alleviating side reactions. In addition, the well‐defined aerogel nanochannels can provide a fast Zn2+ migration path and homogenize Zn2+ flux, enabling rapid and uniform Zn deposition. As a result, the HSA‐modified Zn (HSA@Zn) anode exhibits excellent long‐term cycling stability (over 6000 h at 4 mA cm−2), and the feasibility for practical application of this HSA@Zn anode is further demonstrate in full cells. The aerogel‐driven interface self‐gelation strategy propose in this work provides new insights into the design of advanced Zn anode for aqueous zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

Creating bionic intelligent robotic systems that emulate human‐like skin perception presents a considerable scientific challenge. This study introduces a multifunctional bionic electronic skin (e‐skin) made from polyacrylic acid ionogel (PAIG), designed to detect human motion signals and transmit them to robotic systems for recognition and classification. The PAIG is synthesized using a suspension of liquid metal and graphene oxide nanosheets as initiators and cross‐linkers. The resulting PAIGs demonstrate excellent mechanical properties, resistance to freezing and drying, and self‐healing capabilities. Functionally, the PAIG effectively captures human motion signals through electromechanical sensing. Furthermore, a bionic intelligent sorting robot system is developed by integrating the PAIG‐based e‐skin with a robotic manipulator. This system leverages its ability to detect frictional electrical signals, enabling precise identification and sorting of materials. The innovations presented in this study hold significant potential for applications in artificial intelligence, rehabilitation training, and intelligent classification systems. [ABSTRACT FROM AUTHOR]

Low utilization of solar energy remains a challenge that limits photocatalytic efficiency. To address this issue, this work proposes a bionic solar photocatalytic reactor (BSPR) for efficient selective oxidation of aromatic alcohols. A biomimetic phototropic hydrogel is prepared by coupling chlorine‐doped polypyrrole (Cl‐PPy) and poly(N‐isopropyl acrylamide) (PNIPAm) to maximize light‐harvesting efficiency automatically, allowing the BSPR to maintain high catalytic levels throughout the day. Molecular dynamics simulations are used to unveil the understanding of the fast photoresponsive behavior of Cl‐PPy/PNIPAm from a molecular level, while COMSOL simulations are conducted to follow the macroscopically phototropic mechanism of BSPR. Attributing to the existence of PdS/S vacancies riched ZnIn2S4 nanocomposite in the top flower‐shaped hydrogel, the BSPR displays a special function for efficiently photocatalytic oxidation of aromatic alcohols under solar illumination (yield of 4‐methoxybenzaldehyde: 479.5 µmol g−1 h−1; selectivity: 68.8%). Two possible reaction pathways are identified as follows: photogenerated holes can attract aromatic alcohols directly and generate aromatic aldehydes; photoexcited electrons oxidize O2 to ·O2− can also react with the adsorbed aromatic alcohol. This study presents a promising paradigm that explores opportunities for enhanced utilization of light energy, offering a novel approach to maximize its efficiency in practical applications. [ABSTRACT FROM AUTHOR]

High‐entropy alloys (HEAs) made up of multiple metallic elements have gained attention for their excellent electrocatalytic performance. However, their application in the field of nitrogen (N2) oxidation reaction (NOR) remains underexplored. In this study, a "pomegranate‐like" carbon embedded with ultrafine AuPdPtRhIr HEA (HEA@C) is synthesized using a polymer‐confined pyrolysis strategy. Molecular dynamics (MD) simulations show that small‐sized metal nanoparticles formed by the confinement of polyvinyl alcohol (PVA) during the hydrothermal process can easily form a single‐phase HEA through a thermodynamically‐driven solid‐phase diffusion process during subsequent pyrolysis. Additionally, a porous carbon layer which in situ converted from the PVA shell can effectively inhibit the agglomeration of HEA nanoparticles and confine the surrounding N2. Experimentally, the HEA@C nanohybrid demonstrates a satisfactory NO3− yield rate of 23.8 µg h−1 mgcat.−1 and a high Faraday efficiency of 13.8% for the NOR process. By using operando Fourier Transform Infrared spectroscopy, online differential electrochemical mass spectrometry (DEMS), and density functional theory calculations, potential efficient active sites (Rh–Ir–o) and pathways for the electrochemical conversion of inert N2 to NO3− are revealed. This research provides an effective strategy for producing highly dispersed ultrafine HEA nanoparticles, showing a wide range of applications in advanced electrocatalysis. [ABSTRACT FROM AUTHOR]

Competition from hydrogen/oxygen evolution reactions and low solubility of N2 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 (Fe3C/Fe@PCNF‐F). The simulations prove that the Janus structure can keep the internal Fe3C/Fe@PCNF‐F away from water infiltration and endow a N2 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. In this proof‐of‐concept system, the Fe3C/Fe@PCNF‐F exhibits excellent electrocatalytic performance for nitrogen fixation (NH3 yield rate up to 29.2 μg h−1 mg−1cat. and Faraday efficiency (FE) up to 27.8 % in nitrogen reduction reaction; NO3− yield rate up to 15.7 μg h−1 mg−1cat. and FE up to 3.4 % in nitrogen oxidation reaction). [ABSTRACT FROM AUTHOR]

Die überwältigende Konkurrenz durch Wasserstoff/Sauerstoff‐Entwicklungsreaktionen und die geringe Löslichkeit von N2 in wässrigen Systemen beeinträchtigen die Selektivität und Aktivität bei der Stickstofffixierungsreaktion. Hier entwerfen wir eine aerob‐hydrophobe Janus‐Struktur, indem wir eine fluorierte Modifikation auf porösen Kohlenstoff‐Nanofasern einführen, die in teilweise karbonisierte Eisen‐Heterokontakte (Fe3C/Fe@PCNF‐F) eingebettet sind. Die Simulationen zeigen, dass die Janus‐Struktur die interne Fe3C/Fe@PCNF‐F vor Wassereindringung schützen und einen N2‐Molekül‐konzentrierenden Effekt verleihen kann. Dadurch werden konkurrierende Reaktionen unterdrückt und die Massentransferbeschränkungen überwunden, um einen robusten "quasi‐fest‐gasförmigen" Mikrobereich um die Katalysatoroberfläche herum zu bilden. In diesem Proof‐of‐Concept‐System zeigt Fe3C/Fe@PCNF‐F eine hervorragende elektrokatalytische Leistung für die Stickstofffixierung (NH3‐Ausbeute von bis zu 29.2 μg h−1 mg−1Kat. und faradayscher Wirkungsgrad (FE) von bis zu 27.8 % im NRR; NO3− Ausbeute bis zu 15.7 μg h−1 mg−1Kat. und FE bis zu 3.4 % in NOR). [ABSTRACT FROM AUTHOR]

Hierarchical porous channels and a well-modulated interface are two main parameters for electrode materials that can promote their energy storage performance by accelerating the electrolyte diffusion and realizing their strong coupling with electrolyte ions. Inspired by the COMSOL Multiphysics simulations and density functional theory calculations, we design B, N dual-doped, hierarchical porous carbon (BN-HPC) by pyrolyzing hierarchical porous zeolitic imidazolate framework-8 with boric acid. The resulted BN-HPC electrode achieves a high specific capacitance of 236.9 F g−1 at a current density of 1 A g−1 in 1 M H 2 SO 4 electrolyte, which is further assembled into the BN-HPC//BN-HPC symmetric supercapacitor with a high energy density of 33.3 Wh kg−1 at a power density of 212.5 W kg−1. The excellent energy storage performance of the BN-HPC electrode is attributed to its hierarchical porous structure and bi-heteroatom (N and B) doped carbon surface with a low binding energy value of −2.77 eV. This work provides a general and fresh insight into the design of dodecahedral carbon by combining hierarchical porous structure and bi-heteroatom doping strategy that can be used for not only aqueous supercapacitors but also other energy storage devices. [Display omitted] • B, N co-doped, hierarchical porous carbon is obtained by pyrolyzing ZIF-8 with H 3 BO 3. • COMSOL Multiphysics and DFT jointly illustrate the improved storage performance. • B, N co-doped strategy shows a synergistic effect on improving the adsorption of H+. • A hierarchical porous structure facilitates the penetration of electrolytes. [ABSTRACT FROM AUTHOR]