A polyimine aerogel separator with electron cloud design to boost Li-ion transport for stable Li metal batteries.

The separator with high Young's modulus can avoid the danger of large-sized dendrites, but regulating the chemical behavior of lithium (Li) at the separator/anode interface can effectively eliminate the dendrite issue. Herein, a polyimine aerogel (PIA) with accurate nitrogen (N) functional design is used as the functional separator in Li metal batteries to promote uniform Li nucleation and suppress the dendrite growth. Specifically, the imine (N1) and protonated tertiary amine (N2) sites in the molecular structure of the PIA are significantly different in electron cloud density (ECD) distribution. The N1 site with higher ECD and the N2 site with lower ECD tend to attract and repulse Li+ through electrostatic interactions, respectively. This synergy effect of the PIA separator accelerates the interfacial Li+ diffusion on the Li anode to sustain a uniform two-dimensional Li nucleation behavior. Meanwhile, the well-defined nanochannels of the PIA separator show high affinity to electrolyte and bring uniform Li+ flux for Li plating/stripping. Consequently, the dendrites are effectively suppressed by the PIA separator in routine carbonate electrolyte, and the Li metal batteries with the PIA separator exhibit high Coulombic efficiency and stable high-rate cycling. These findings demonstrate that the ingenious marriage of special chemical structure designs and hierarchical pores can enable the separator to affect the interfacial Li nucleation behavior.

Biomimetic Design of 3D Fe3O4/V-EVOH Fiber-Based Self-Floating Composite Aerogel to Enhance Solar Steam Generation Performance.

An interfacial solar steam generation evaporator for seawater desalination has attracted extensive interest in recent years. Nevertheless, challenges still remain in relatively low evaporation rate, unsatisfactory energy conversion efficiency, and salt accumulation. Herein, we have demonstrated a biomimetic bilayer composite aerogel consisting of bottom hydrophilic and vertically aligned EVOH channels and an upper hydrophobic conical Fe3O4 array. Thanks to the design merits, the 3D Fe3O4/V-EVOH evaporator exhibits a high evaporation rate of ∼2.446 kg m-2 h-1 and an impressive solar energy conversion efficiency of ∼165.5% under 1 sun illumination, which is superior to those of state-of-the-art evaporators reported so far. Moreover, the asymmetrical wettability not only allows the evaporator to self-float on the water but also facilitates the salt ion diffusion in the channels; thus, the evaporator shows no salt crystals on its surface and only a 6% decrease in evaporation performance even after the salt concentration increases from 0 to 10.0 wt %.

Strong, Lightweight, and Shape-Memory Bamboo-Derived All-Cellulose Aerogels for Versatile Scaffolds of Sustainable Multifunctional Materials.

Strong, lightweight, and shape-memory cellulose aerogels have great potential in multifunctional applications. However, achieving the integration of these features into a cellulose aerogel without harsh chemical modifications and the addition of mechanical enhancers remains challenging. In this study, a strong, lightweight, and water-stimulated shape-memory all-cellulose aerogel (ACA) is created using a combination strategy of partial dissolution and unidirectional freezing from bamboo. Benefiting from the firm architecture of cellulose microfibers bridging cellulose nanofibers /regenerated cellulose aggregated layers and the bonding of different cellulose crystal components (cellulose Iß and cellulose II), the ACA, with low density (60.74 mg cm-3 ), possesses high compressive modulus (radial section: 1.2 MPa, axial section: 0.96 MPa). Additionally, when stimulated with water, the ACA exhibits excellent shape-memory features, including highly reversible compression-resilience and instantaneous fold-expansion behaviors. As a versatile scaffold, ACA can be integrated with hydroxyapatite, carboxyl carbon nanotubes, and LiCl, respectively, via a simple impregnation method to yield functionalized cellulose composites for applications in thermal insulation, electromagnetic interference shielding, and piezoresistive sensors. This study provides inspiration and a reliable strategy for the elaborately structural design of functional cellulose aerogels endows application prospects in various multifunction opportunities.

Hydrosilylation Adducts to Produce Wide-Temperature Flexible Polysiloxane Aerogel under Ambient Temperature and Pressure Drying.

Despite incorporation of organic groups into silica-based aerogels to enhance their mechanical flexibility, the wide temperature reliability of the modified silicone aerogel is inevitably degraded. Therefore, facile synthesis of soft silicone aerogels with wide-temperature stability remains challenging. Herein, novel silicone aerogels containing a high content of Si are reported by using polydimethylvinylsiloxane (PDMVS), a hydrosilylation adduct with water-repellent groups, as a "flexible chain segment" embedded within the aerogel network. The poly(2-dimethoxymethylsilyl)ethylmethylvinylsiloxane (PDEMSEMVS) aerogel is fabricated through a cost-effective ambient temperature/pressure drying process. The optimized aerogel exhibits exceptional performance, such as ultra-low density (50 mg cm-3), wide-temperature mechanical flexibility, and super-hydrophobicity, in comparison to the previous polysiloxane aerogels. A significant reduction in the density of these aerogels is achieved while maintaining a high crosslinking density by synthesizing gel networks with well-defined macromolecules through hydrolytic polycondensation crosslinking of PDEMSEMVS. Notably, the pore/nanoparticle size of aerogels can be fine-tuned by optimizing the gel solvent type. The as-prepared silicone aerogels demonstrate selective absorption, efficient oil-water separation, and excellent thermal insulation properties, showing promising applications in oil/water separation and thermal protection.

Biomimetic Transparent Layered Tough Aerogels for Thermal Superinsulation and Triboelectric Nanogenerator.

Transparent aerogels are ideal candidates for thermally insulating windows, solar thermal receivers, electronics, etc. However, they are usually prepared via energy-consuming supercritical drying and show brittleness and low tensile strength, significantly restricting their practical applications. It remains a great challenge to prepare transparent aerogels with high tensile strength and toughness. Herein, biomimetic transparent tough cellulose nanofiber-based nanocomposite aerogels with a layered nanofibrous structure are achieved by vacuum-assisted self-assembly combined with ambient pressure drying. The nacre-like layered homogeneous nanoporous structures can reduce light scattering and effectively transfer stress and prevent stress concentration under external forces. The aerogels exhibit an attractive combination of excellent transparency and hydrophobicity, high compressive and tensile strengths, high toughness, excellent machinability, thermal superinsulation, and wide working temperature range (-196 to 230 °C). It is demonstrated that they can be used for superinsulating windows of buildings and high-efficient thermal management for electronics and human bodies. In addition, a prototype of transparent flexible aerogel-based triboelectric nanogenerator is developed. This work provides a promising pathway toward transparent tough porous materials for energy saving/harvesting, thermal management, electronics, sensors, etc.

Spin Effect to Regulate the Electronic Structure of Ir─Fe Aerogels for Efficient Acidic Water Oxidation.

"Spin" has been recently reported as an important degree of electronic freedom to promote catalysis, yet how it influences electronic structure remains unexplored. This work reports the spin-induced orbital hybridization in Ir─Fe bimetallic aerogels, where the electronic structure of Ir sites is effectively regulated by tuning the spin property of Fe atoms. The spin-optimized electronic structure boosts oxygen evolution reaction (OER) electrocatalysis in acidic media, resulting in a largely improved catalytic performance with an overpotential of as low as 236 mV at 10 mA cm-2. Furthermore, the gelation kinetics for the aerogel synthesis is improved by an order of magnitude based on the introduction of a magnetic field. Density functional theory calculation reveals that the increased magnetic moment of Fe (3d orbital) changes the d-band structure (i.e., the d-band center and bandwidth) of Ir (5d orbital) via orbital hybridization, resulting in optimized binding of reaction intermediates. This strategy builds the bridge between the electron spin theory with the d-band theory and provides a new way for the design of high-performance electrocatalysts by using spin-induced orbital interaction.

Metal Halide Nanocrystals@Silica Aerogel Composite with Enhanced Dispersion Stability and Light Output for Efficient X-Ray Imaging in Harsh Environment.

Metal halide nanocrystals (MHNCs) embedded in a polymer matrix as flexible X-ray detector screens is an effective strategy with the advantages of low cost, facile preparation, and large area flexibility. However, MHNCs easily aggregate during preparation, recombination, under mechanical force, storage, or high operating temperature. Meanwhile, it shows an unmatched refractive index with polymer, resulting in low light yield. The related stability and properties of the device remain a huge unrevealed challenge. Herein, a composite screen (CZBM@AG-PS) by integrating MHNCs (Cs2ZnBr4: Mn2+ as an example) into silica aerogel (AG) and embedded in polystyrene (PS) is successfully developed. Further characterization points to the high porosity AG template that can effectively improve the dispersion of MHNCs in polymer detector screens, essentially decreasing nonradiative transition, Rayleigh scattering, and performance aging induced by aggregation in harsh environments. Furthermore, the higher light output and lower optical crosstalk are also achieved by a novel light propagation path based on the MHNCs/AG and AG/PS interfaces. Finally, the optimized CZBM@AG-PS screen shows much enhanced light yield, spatial resolution, and temperature stability. Significantly, the strategy is proven universal by the performance tests of other MHNCs embedded composite films for ultra-stable and efficient X-ray imaging.

Boosting Photocatalytic CO2 Methanation through Interface Fusion over CdS Quantum Dot Aerogels.

In the field of photocatalytic CO2 reduction, quantum dot (QD) assemblies have emerged as promising candidate photocatalysts due to their superior light absorption and better substrate adsorption. However, the poor contacts within QD assemblies lead to low interfacial charge transfer efficiency, making QD assemblies suffer from unsatisfactory photocatalytic performance. Herein, a novel approach is presented involving the construction of strongly interfacial fused CdS QD assemblies (CdS QD gel) for CO2 reduction. The novel CdS QD gel demonstrates outstanding photocatalytic performance for CO2 methanation, achieving a CH4 generation rate of ≈296 µmol g-1 h-1, with a selectivity surpassing 76% and an apparent quantum yield (AQY) of 1.4%. Further investigations reveal that the robust interfacial fusion in these CdS QDs not only boosts their ability to absorb visible light but also significantly promotes charge separation. The present work paves the way for utilizing QD gel photocatalysts in realizing efficient CO2 reduction and highlights the critical role of interfacial engineering in photocatalysts.

Superelastic Cellulose Sub-Micron Fibers/Carbon Black Aerogel for Highly Sensitive Pressure Sensing.

Superelastic aerogels with rapid response and recovery times, as well as exceptional shape recovery performance even from large deformation, are in high demand for wearable sensor applications. In this study, a novel conductive and superelastic cellulose-based aerogel is successfully developed. The aerogel incorporates networks of cellulose sub-micron fibers and carbon black (SMF/CB) nanoparticles, achieved through a combination of dual ice templating assembly and electrostatic assembly methods. The incorporation of assembled cellulose sub-micron fibers imparts remarkable superelasticity to the aerogel, enabling it to retain 94.6% of its original height even after undergoing 10 000 compression/recovery cycles. Furthermore, the electrostatically assembled CB nanoparticles contribute to exceptional electrical conductivity in the cellulose-based aerogel. This combination of electrical conductivity and superelasticity results in an impressive response time of 7.7 ms and a recovery time of 12.8 ms for the SMF/CB aerogel, surpassing many of the aerogel sensors reported in previous studies. As a proof of concept, the SMF/CB aerogel is utilized to construct a pressure sensor and a sensing array, which exhibit exceptional responsiveness to both minor and substantial human motions, indicating its significant potential for applications in human health monitoring and human-machine interaction.

Title High Solar-Thermal Conversion Aerogel for Efficient Atmospheric Water Harvesting.

The shortage of freshwater is a global problem, however, the gel that can be used for atmospheric water harvesting (AWH) in recent years studying, suffer from salt leakage, agglomeration, and slow water evaporation efficiency. Herein, a solar-driven atmospheric water harvesting (SAWH) aerogel is prepared by UV polymerization and freeze-drying technique, using poly(N-isopropylacrylamide) (PNIPAm), hydroxypropyl cellulose (HPC), ethanolamine-decorate LiCl (E-LiCl) and polyaniline (PANI) as raw materials. The PNIPAm and HPC formed aerogel networks makes the E-LiCl stably and efficiently loaded, improving the water adsorption-desorption kinetics, and PANI achieves rapid water vapor evaporation. The aerogel has low density ≈0.12-0.15 g cm-3, but can sustain a weight of 1000 times of its own weight. The synergist of elements and structure gives the aerogel has 0.46-2.95 g g-1 water uptake capability at 30-90% relative humidity, and evaporation rate reaches 1.98 kg m-2 h-1 under 1 sun illumination. In outdoor experiments, 88% of the water is harvesting under natural light irradiation, and an average water harvesting rate of 0.80 gwater gsorbent -1 day-1. Therefore, the aerogel can be used in arid and semi-arid areas to collect water for plants and animals.

Promoting Electromagnetic Wave Absorption Performance by Integrating MoS2@Gd2O3/MXene Multiple Hetero-Interfaces in Wood-Derived Carbon Aerogels.

Multi-component composite materials with a magnetic-dielectric synergistic effect exhibit satisfactory electromagnetic wave absorption performance. However, the effective construction of the structure for these multi-component materials to fully exploit the advantages of each component remains a challenge. Inspired by natural biomass, this study utilizes wood as the raw material and successfully prepares high-performance MoS2@Gd2O3/Mxene loaded porous carbon aerogel (MGMCA) composite material through a one-pot hydrothermal method and carbonization treatment process. With a delicate structural design, the MGMCA is endowed with abundant heterogeneous interface structures, favorable impedance matching characteristics, and a magnetic-dielectric synergistic system, thus demonstrating multiple electromagnetic wave loss mechanisms. Benefiting from these advantages, the obtained MGMCA exhibits outstanding electromagnetic wave absorption performance, with a minimum reflection loss of -57.5 dB at an ultra-thin thickness of only 1.9 mm. This research proposes a reliable strategy for the design of multi-component composite materials, providing valuable insight for the design of biomass-based materials as electromagnetic wave absorbers.

A Tent-Inspired Portable Solar-Driven Water Purification Device for Wilderness Explorers.

Wilderness adventure favored by many enthusiasts often endanger lives due to lacking freshwater or drinking contaminated water. Therefore, compared to the inefficient methods of filtration, steaming, and direct solar heating, it is of great meaningfulness to develop a solar-driven water purification device with efficiency, lightweight, portability, and multi-water-quality purification by taking full advantage of solar-driven interfacial evaporation. Here, a tent-inspired portable solar-driven water purification device consisting of Janus-structured bacterial cellulose aerogel (JBCA) solar evaporator and tent-type condensation recovery device is reported. For the JBCA solar evaporator, it is prepared from biomass bacterial cellulose (BC) as raw material and hydroxylated carbon nanotubes (HCNT) as photothermal material, and the Janus property is achieved by the assistance of hydrophobic and hydrophilic chemical cross-linking. It exhibits lightweight, unibody, high photothermal conversion, efficient evaporation, and multi-water-quality purification capability for representative seawater, urine, and bacterial river water. For the tent-type condensation recovery device, it is based on the prototype of tent and uses flexible ultra-transparent polyvinyl chloride (PVC) film as raw material. Thanks to the rational prototype and material selection, it displays outstanding portability and lightweight through the folding/unfolding method. Therefore, the designed tent-inspired portable solar-driven water purification device demonstrates great potential application in wilderness exploration.

Double-Phase-Networking Polyimide Hybrid Aerogel with Exceptional Dimensional Stability for Superior Thermal Protection System.

Polyimide aerogels have been extensively used in thermal protection domain because they possess a combination of intrinsic characteristics of aerogels and unique features of polyimide. However, polyimide aerogels still suffer significant thermally induced shrinkage at temperatures above 200 °C, restricting their application at high temperature. Here, a novel "double-phase-networking" strategy is proposed for fabricating a lightweight and mechanically robust polyimide hybrid aerogel by forming silica-zirconia-phase networking skeletons, which possess exceptional dimensional stability in high-temperature environments and superior thermal insulation. The rational mechanism responsible for the formation of double-phase-networking aerogel is further explained, generally attributing to chemical crosslinking reactions and supramolecular hydrogen bond interactions derived from the main chains of polyimide and silane/zirconia precursor/sol. The as-prepared aerogels exhibit excellent high-temperature (270 °C) dimensional stability (5.09% ± 0.16%), anti-thermal-shock properties, and low thermal conductivity. Moreover, the hydrophobic treatment provides aerogels high water resistance with water contact angle of 136.9°, further suggestive of low moisture content of 3.6% after exposure to 70 °C and 85% relative humidity for 64 h. The proposed solution for significantly enhancing high-temperature dimensional stability and thermal insulation provides a great supporting foundation for fabricating high-performance organic aerogels as thermal protection materials in aerospace.

2D Tantalum Disulfide Reduction Strategy Customized Ta2O5/rGO Heterointerface Aerogel Toward Boosting Electromagnetic Wave Absorption and Flame Retardancy.

The exceptional and substantial electron affinity, as well as the excellent chemical and thermal stability of transition metal oxides (TMOs), infuse infinite vitality into multifunctional applications, especially in the field of electromagnetic wave (EMW) absorption. Nonetheless, the suboptimal structural mechanical properties and absence of structural regulation continue to hinder the advancement of TMOs-based aerogels. Herein, a novel 2D tantalum disulfide (2H-TaS2) reduction strategy is demonstrated to synthesize Ta2O5/reduced graphene oxide (rGO) heterointerface aerogels with unique characters. As the prerequisite, the defects, interfaces, and configurations of aerogels are regulated by varying the concentration of 2H-TaS2 to ensure the Ta2O5/rGO heterointerface aerogels with appealing EMW absorption properties such as a minimum reflection loss (RLmin) of -61.93 dB and an effective absorption bandwidth (EAB) of 8.54 GHz (7.80-16.34 GHz). This strategy provides valuable insights for designing advanced EMW absorbers. Meanwhile, the aerogel exhibits favorable thermal insulation performance with a value of 36 mW m-1 K-1, outstanding fire resistance capability, and exceptional mechanical energy dissipation performance, making it promising for applications in the aerospace industry and consumer electronics devices.

Multifunctional Carbon Fiber Reinforced C/SiOC Aerogel Composites for Efficient Electromagnetic Wave Absorption, Thermal Insulation, and Flame Retardancy.

Carbon fiber composites have great application prospects as a potential electromagnetic (EM) wave-absorbing material, yet it remains extremely challenging to integrate multiple functions of EM wave absorption, mechanical strength, thermal insulation, and flame retardancy. Herein, a novel carbon fiber reinforced C/SiOC aerogel (CF/CS) composite is successfully prepared by sol-gel impregnation combined with an ambient drying process for the first time. The density of the obtained CF/CS composites can be controlled just by changing sol-gel impregnation cycles (original carbon fiber felt (S0), and samples with one (S1) and two (S2) impregnation cycles are 0.249, 0.324, and 0.402 g cm-3, respectively), allowing for efficient tuning of their properties. Remarkably, S2 displays excellent microwave absorption properties, with an optimal reflection loss of -65.45 dB, which is significantly improved than S0 (-10.90 dB). Simultaneously, compared with S0 (0.75 and 0.30 MPa in the x/y and z directions), the mechanical performance of S2 is dramatically improved with a maximum compressive strength of 10.37 and 4.93 MPa in the x/y and z directions, respectively. Moreover, CF/CS composites show superior thermal insulation capability than S0 and obtain good flame-retardant properties. This work provides valuable guidance and inspiration for the development of multifunctional EM wave absorbers.

Hetero-Interface Engineering on 9.0 wt% CoOx -Doped CeO2 Nanorods as Electromagnetic Wave Absorber and Integrated into Multifunctional Aerogel.

Ceria (CeO2 ) becomes a promising candidate as electromagnetic wave absorbing materials (EWAMs) for their abundant natural source, rich oxygen vacancy, charge conversion, and electron transfer abilities. However, it remains challenging to regulate its nanoscale and atom-scale composition to optimize the absorbing performance and develop high-performance commercial devices. Herein, a facile method to large-scale synthesis CeO2 @Co-x% (x = 5, 7, 9, 11, 13) series EWAMs with diverse amounts of decorated CoOx is presented. By modulating the ratio of doped CoOx , a rational hetero-interface is created in CeO2 @Co-9% to enhance natural and exchange resonances, improving magnetic loss capability and optimizing impedance matching. Doped CoOx promotes the charge accumulation, interfacial polarization, and multiple scattering of the CeO2 for strengthening the EW absorption and attenuation, which display superb minimum reflective loss (RLmin ) of -74.4 dB with a wide effective absorbing bandwidth (EAB) of 5.26 GHz. Furthermore, a dual crosslinking strategy is employed to fabricate CeO2 @Co-9% into an aerogel device with integrated lightweight, heat insulation, compression resistance, and fame-retardant functions. This work presents an excellent example of large-scale fast synthesis of high-performance CeO2 -based EWAMs and multiplication 3D devices.

3D-Printed Mullite-Reinforced SiC-Based Aerogel Composites.

There is a growing demand for thermal management materials in electronic fields. Aerogels have attracted interest due to their extremely low density and extraordinary thermal insulation properties. However, the application of aerogels is limited by high production costs and the requirement that aerogel structures not be load-bearing. In this study, mullite-reinforced SiC-based aerogel composite (MR-SiC AC) is prepared through 3D printing combined with in situ growth of SiC nanowires in post processing. The fabricated MR-SiC AC not only has ultra-low thermal conductivity (0.021 W K m-1) and high porosity (90.0%), but also a high Young's modulus (24.4 MPa) and high compressive strength (1.65 MPa), both exceeding the measurements of existing resilient aerogels by an order of magnitude. These properties make MR-SiC AC an ideal solution for the precision thermal management of lightweight structures having complex geometry for functional devices.

Multifunctional Super-Hydrophilic MXene/Biomass Composite Aerogel Evaporator for Efficient Solar-Driven Desalination and Wastewater Treatment.

Solar-driven interfacial evaporation is recognized as a sustainable and effective strategy for desalination to mitigate the freshwater scarcity issue. Nevertheless, the challenges of oil contamination, salt accumulation, and poor long-term stability of the solar desalination process limit its applications. Herein, a 3D biomass-based multifunctional solar aerogel evaporator is developed for water production with fabricated chitosan/lignin (CSL) aerogel as the skeleton, encapsulated with carbonized lignin (CL) particles and Ti3C2TiX (MXene) nanosheets as light-absorbing materials. Benefitting from its super-hydrophilic wettability, interconnected macropore structure, and high broadband light absorption (ca. 95.50%), the prepared CSL-C@MXene-20 mg evaporator exhibited a high and stable water evaporation flux of 2.351 kg m-2 h-1 with an energy conversion efficiency of 88.22% under 1 Sun (1 kW m-2) illumination. The CSL-C@MXene-20 mg evaporator performed excellent salt tolerance and long-term solar vapor generation in a 3.5 wt.% NaCl solution. Also, its super-hydrophilicity and oleophobicity resulted in superior salt resistance and anti-fouling performance in high salinity brine (20 wt.% NaCl) and oily wastewater. This work offers new insight into the manufacture of porous and eco-friendly biomass-based photothermal aerogels for advanced solar-powered seawater desalination and wastewater purification.

Multifunctional MoCx Hybrid Polyimide Aerogel with Modified Porous Defect Engineering for Highly Efficient Electromagnetic Wave Absorption.

Traditional electromagnetic absorbing materials (EWAMs) are usually single functions and can easily affect their performance in diverse application scenarios. Effective integration of EWAMs into multiple function components is a valuable strategy to achieve maximum absorption and multifunction performance while maintaining their indispensable physical and chemical properties. In this work, the polyoxometalates (POMs) serving as "guests" are embedded within the Co-MOFs to construct 3d/4d-bimetallic based crystalline precursors of dielectric/magnetic synergistic system. The proper pyrolysis temperature induced the homogeneously distributed metallic Co and MoCx hetero-units into carbon matrix with modified porous defect engineering to enhance electromagnetic wave (EW). Owing to the brilliant synergistic effect of polarization, magnetic loss, and impedance matching, the superior RLmin of -47.72 dB at 11.76 GHz at the thickness of 2.0 mm and a wide adequate absorption bandwidth (EAB) of 4.58 GHz (7.44-12.02 GHz) covered the whole X-band at the thickness of 2.5 mm for η-MoC/Co@NC-800 are observed. More importantly, the resulting MoCx hybrid polyimide (MCP) aerogel exhibits desirable properties such as structural robustness, nonflammability, excellent thermal insulation, and self-cleaning capabilities that are comparable to those of commercially available products. This work offers inspiration and strategy for creating multipurpose microwave absorbers with intricate structural designs.

Amorphous K-Co-Mo-Sx Chalcogel: A Synergy of Surface Sorption and Ion-Exchange.

Chalcogel represents a unique class of meso- to macroporous nanomaterials that offer applications in energy and environmental pursuits. Here, the synthesis of an ion-exchangeable amorphous chalcogel using a nominal composition of K2 CoMo2 S10 (KCMS) at room temperature is reported. Synchrotron X-ray pair distribution function (PDF), X-ray absorption near-edge structure (XANES), and extended X-ray absorption fine structure (EXAFS) reveal a plausible local structure of KCMS gel consisting of Mo5+ 2 and Mo4+ 3 clusters in the vicinity of di/polysulfides which are covalently linked by Co2+ ions. The ionically bound K+ ions remain in the percolating pores of the Co-Mo-S covalent network. XANES of Co K-edge shows multiple electronic transitions, including quadrupole (1s→3d), shakedown (1s→4p + MLCT), and dipole allowed 1s→4p transitions. Remarkably, despite a lack of regular channels as in some crystalline solids, the amorphous KCMS gel shows ion-exchange properties with UO2 2+ ions. Additionally, it also presents surface sorption via [S∙∙∙∙UO2 2+ ] covalent interactions. Overall, this study underscores the synthesis of quaternary chalcogels incorporating alkali metals and their potential to advance separation science for cations and oxo-cationic species by integrating a synergy of surface sorption and ion-exchange.