Hierarchical Porous Structure Research Articles

Synthesis of Granular MCM-22 Zeolite with a Hierarchical Porous Structure

Synthesis of Granular MCM-22 Zeolite with a Hierarchical Porous Structure

Nanoporous Carbon Materials Derived from Zanthoxylum Bungeanum Peel and Seed for Electrochemical Supercapacitors

In order to prepare biomass-derived carbon materials with high specific capacitance at a low activation temperature (≤700 °C), nanoporous carbon materials were prepared from zanthoxylum bungeanum peels and seeds via the pyrolysis and KOH-activation processes. The results show that the optimal activation temperatures are 700 °C and 600 °C for peels and seeds. Benefiting from the hierarchical pore structure (micropores, mesopores, and macropores), the abundant heteroatoms (N, S, and O) containing functional groups, and plentiful electrochemical active sites, the PAC-700 and SAC-600 derive the large capacities of ~211.0 and ~219.7 F g−1 at 1.0 A g−1 in 6 M KOH within the three-electrode configuration. Furthermore, the symmetrical supercapacitors display a high energy density of 22.9 and 22.4 Wh kg−1 at 7500 W kg−1 assembled with PAC-700 and SAC-600, along with exceptional capacitance retention of 99.1% and 93.4% over 10,000 cycles at 1.0 A g−1. More significantly, the contribution here will stimulate the extensive development of low-temperature activation processes and nanoporous carbon materials for electrochemical energy storage and beyond.

Anti-Oxidized Self-Assembly of Multilayered F-Mene/MXene/TPU Composite with Improved Environmental Stability and Pressure Sensing Performances

MXenes, as emerging 2D sensing materials for next-generation electronics, have attracted tremendous attention owing to their extraordinary electrical conductivity, mechanical strength, and flexibility. However, challenges remain due to the weak stability in the oxygen environment and nonnegligible aggregation of layered MXenes, which severely affect the durability and sensing performances of the corresponding MXene-based pressure sensors, respectively. Here, in this work, we propose an easy-to-fabricate self-assembly strategy to prepare multilayered MXene composite films, where the first layer MXene is hydrogen-bond self-assembled on the electrospun thermoplastic urethane (TPU) fibers surface and the anti-oxidized functionalized-MXene (f-MXene) is subsequently adhered on the MXene layer by spontaneous electrostatic attraction. Remarkably, the f-MXene surface is functionalized with silanization reagents to form a hydrophobic protective layer, thus preventing the oxidation of the MXene-based pressure sensor during service. Simultaneously, the electrostatic self-assembled MXene and f-MXene successfully avoid the invalid stacking of MXene, leading to an improved pressure sensitivity. Moreover, the adopted electrospinning method can facilitate cyclic self-assembly and the formation of a hierarchical micro-nano porous structure of the multilayered f-MXene/MXene/TPU (M-fM2T) composite. The gradient pores can generate changes in the conductive pathways within a wide loading range, broadening the pressure detection range of the as-proposed multilayered f-MXene/MXene/TPU piezoresistive sensor (M-fM2TPS). Experimentally, these novel features endow our M-fM2TPS with an outstanding maximum sensitivity of 40.31 kPa−1 and an extensive sensing range of up to 120 kPa. Additionally, our M-fM2TPS exhibits excellent anti-oxidized properties for environmental stability and mechanical reliability for long-term use, which shows only ~0.8% fractional resistance changes after being placed in a natural environment for over 30 days and provides a reproducible loading–unloading pressure measurement for more than 1000 cycles. As a proof of concept, the M-fM2TPS is deployed to monitor human movements and radial artery pulse. Our anti-oxidized self-assembly strategy of multilayered MXene is expected to guide the future investigation of MXene-based advanced sensors with commercial values.

Application of Hierarchically Porous Chitosan Monolith for Enzyme Immobilization.

Enzyme immobilization is a crucial technique for improving the stability of enzymes. Compared with free enzymes, immobilized enzymes offer several advantages in industrial applications. Efficient enzyme immobilization requires a technique that integrates the advantages of physical absorption and covalent binding while addressing the limitations of conventional support materials. This study offers a practical approach for immobilizing α-amylase on a hierarchically porous chitosan (CS) monolith. An optimized CS monolith was fabricated using chemically modified chitin by thermally induced phase separation. By combining physical adsorption and covalent bonding, this technique leverages the amino and hydroxy groups present in CS to facilitate effective enzyme binding and stability. α-Amylase immobilized on the CS monolith demonstrated excellent stability, reusability, and increased activity compared to its soluble counterpart across various pH levels and temperatures. In addition, the CS monolith exhibited a significant potential to immobilize other enzymes, namely, lipase and catalase. Immobilized lipase and catalase exhibited higher loading capacities and enhanced activities than their soluble forms. This versatility highlights the broad applicability of CS monoliths as support materials for various enzymatic processes. This study provides guidelines for fabricating hierarchical porous monolith structures that can provide efficient enzyme utilization in flow systems and potentially enhance the cost-effectiveness of enzymes in industrial applications.

3D-interconnected N-doped porous carbon with hierarchical pore structure as a high-efficiency catalyst for H2S oxidation at room temperature

Nitrogen-doped porous carbons (NPCs) have been regarded as an efficient metal-free catalyst for H2S oxidation. However, critical factors affecting their desulfurization ability are still unclear, making it difficult to accurately adjust their desulfurization performance to meet industrial requirements. Herein, a novel 3D-interconnected NPC with hierarchical pore structure was synthesized by one-step “leavening” strategy using rice husk and (NH4)2C2O4 as a carbon source and foaming agent, respectively, for H2S oxidation at room temperature. Pyrolysis temperature is the major factor for physicochemical properties of NPCs, and breakthrough sulfur capacity of the optimal NPC reaches up to 1036.68 mg/g, which can remain stable during three desulfurization-regeneration cycles. Comparative experiment shows that H2S capacity of NPC is 1.8 and 4.0 times those of PC and NC, respectively, revealing the excellent desulfurization performance of NPC. The structure-effect relationships between H2S and NPC reveal that both textural and chemical properties of NPC, especially specific surface area, structural defect, and pyrrolic N, play dominant roles in H2S removal. It is very necessary to balance the relationship between textural performances and pyrrolic N to synthesize optimal NPC catalyst. This work provides a valuable reference for rational design of high-efficiency carbon-based catalysts for persistent desulfurization at room temperature.

Flower-like covalent organic frameworks as host materials for high-performance lithium-sulfur batteries

Lithium-sulfur (Li-S) batteries have emerged as a promising alternative energy storage system due to their high energy density and cost-effectiveness. However, practical applications of Li-S batteries are hindered by challenges such as the shuttle effect and sluggish redox kinetics. In this study, a three-dimensional (3D) flower-like diaminoanthraquinone (DAAQ)-covalent organic framework (COF) was developed, featuring nanorod-like petals and enriched with abundant N and O adsorption sites, serving as a host material for the sulfur cathode of Li-S batteries. Through a process of sulfur melting-diffusion, the resulting DAAQ-COF@S cathode material demonstrated a stable 3D cross-linked morphology with a hierarchical pore structure, maximizing the exposure of N/O adsorptive sites and facilitating rapid ion diffusion. This effectively inhibited the shuttling effect of lithium polysulfides (LiPSs) and enhanced rate performance. Consequently, DAAQ-COF@S cathodes exhibited a high initial discharge capacity of 1182.0 mAh g−1 at 0.1 C, with a capacity retention rate of 79.6% after 500 cycles at 2 C. Even at a high current density of 4 C, they maintained a high capacity of 616.8 mAh g−1, surpassing the majority of previously reported COF-based host materials for Li-S batteries. This work underscores the significance of COF micromorphology and advances the development of high-performance cathodes for Li-S batteries.

Efficient Template-Catalyzed In Situ Polymerization for Carbon Xerogels with Large Specific Surface Area and High Adsorption.

The limited specific surface area (SSA), long preparation period, and high cost are significant challenges for carbon xerogels (CXs). To overcome these limitations, we propose an approach to prepare tannin-resorcinol-formaldehyde-based CXs through template-catalyzed in situ polymerization. ZnCl2 acts as a catalyst and significantly accelerates the polymerization reaction through the coordination of Zn2+ to the carbonyl group in formaldehyde, while atmospheric drying instead of special drying and without solvent exchange reduces the preparation period to 24 h. In addition, ZnCl2 acts as an activator for the formation of many pores. Plant-derived tannins not only reduce the preparation cost but also regulate the pore structure. The resulted CXs with hierarchical porous structures show an optimal SSA of 1308 m2/g, high adsorption capabilities (for cationic, nitrosoaniline dyes, metal, and nonmetallic ions, especially for methylene blue with 454.93 mg/g), low shrinkage down to 10%, and reusability with 92.9% retention after 5 cycles. This work provides a promising and cost-effective method for the large-scale preparation of porous carbon materials with large SSA, offering potential applications in adsorption, energy storage, and catalysis.

Indirect 3D printing CDHA scaffolds with hierarchical porous structure to promote osteoinductivity and bone regeneration

Hierarchical porous structures, which include macropores, minor pores, and micropores in scaffolds, are essential in the multiple biological functions of bone repair and regeneration. In this study, patient-customized calcium-deficient hydroxyapatite (CDHA) scaffolds with the three-level hierarchical porous structure were fabricated by indirect 3D printing technology and particulate leaching method. The sacrificial template scaffolds were fabricated using a photo-curing 3D printer, which provided a prerequisite for the integral structure and interconnected macro pores of CDHA scaffolds. Additionally, the 20 wt% pore former was incorporated into the slurry to enhance the content of smaller pores within the CDHA-2 scaffolds, and then the CDHA-2 scaffolds were sintered to remove the sacrificial template scaffolds and pore former. The obtained CDHA-2 scaffolds exhibited interconnected macropores (300–400 μm), minor pores (∼10–100 μm), and micropores (< 10 μm) distributed throughout the scaffolds, which could promote bone tissue ingrowth, increase surface roughness, and enhance protein adsorption of scaffolds. In vitro studies identified that CDHA-2 scaffolds had nanocrystal grains, high specific surface area, and outstanding protein adsorption capacity, which could provide a microenvironment for cell adhesion, spreading, and proliferation. In addition, the murine intramuscular implantation experiment suggested that CDHA-2 scaffolds exhibited excellent osteoinductivity and were superior to traditional BCP ceramics under conditions without the addition of live cells and exogenous growth factors. The rabbit calvarial defect repair results indicated that CDHA-2 scaffolds could enhance in situ bone regeneration. In conclusion, these findings demonstrated that the hierarchical porous structure of CDHA scaffolds was a pivotal factor in modulating osteoinductivity and bone regeneration, and CDHA-2 scaffolds were a potential candidate for bone regeneration.

A hierarchical porous structure and nitrogen-doping jointly enhance the lithium-ion storage capacity of biomass-derived carbon materials

Biomass-derived carbon materials are considered potential lithium-ion anode materials because they are sustainable, renewable, economical, and environmentally friendly and have tunable microstructures. However, biomass-derived carbon materials have low specific capacity and show capacity degradation during long-term electrochemical cycling, which prevents their application in high-performance lithium-ion batteries. Hence, in this paper, nitrogen-doped hierarchical porous carbon (NHPC) is synthesized from a biomass waste material, corncob, through one-step activation and carbonization procedures. N-doping in the NHPC modifies the electron distribution on the surface of carbon, resulting in the generation of additional lithium-ion storage sites and enhancing electrode wettability to increase the conductivity. Additionally, the doping procedure results in a hierarchical porous structure with an increased specific surface area and pore volume, which facilitates ion transport and provides remarkable cycling stability. The electrochemical performance of NHPC is improved by the jointly beneficial combination of N-doping and the hierarchical porous structure. The optimized NHPC electrode provides a reversible specific capacity of 700 mAh g−1 after 100 cycles at 100 mA g−1. This study provides a simple and efficient method for improving the electrochemical properties of biomass-derived carbon materials through elemental doping and modulation of microscopic morphology and structure.

Chemical etching optimization of 3D printed α-Al2O3 monoliths to enhance the catalytic applications

Direct Ink Writing has been demonstrated to be a promising route to produce ceramic catalysts with complex geometries and enhanced catalytic performances. To increase the catalytic performances, chemical etching can be conducted to get an interconnected and hierarchical porous structure, to increase the surface area and the contact time of the reactants. In this work, DIW alpha (α)-Al2O3 catalysts were chemically etched with hydrofluoric acid (HF). Several combinations of acid concentrations and etching times were studied to find the optimal etching condition. For HF concentration of 5, 20 and 40wt. %, the optimal etching time was 48, 24 and 5h, respectively, being 40wt. % the concentration that shows the greatest increase of surface porosity (of around 5%). HF etching can produce an interconnected porosity on 3DP α-Al2O3, but it does not yield improvement in catalytic performances when the content of fluor (F) is higher than 10 at. % since it produces parasite reactions.

Ultrafast High-capacitance Supercapacitors Employing Carbons Derived from Al-based Metal-organic Frameworks

Compact supercapacitors (SCs) have garnered significant attention due to their potential to replace bulky aluminum electrolytic capacitors (AECs) in alternating current (AC) line filtering applications. However, the slow response speeds of conventional SCs based on activated carbons are inadequate for such high-frequency applications. Therefore, this paper presents a study on high-frequency SCs using metal-organic framework (MOF)-derived carbon (MDC) electrode materials. Here, the carbonization of the selected MOF results in highly conductive carbons with hierarchical pore structures that offer substantial advantages for use as electrode materials in ultrafast SC applications. Consequently, the as-fabricated MDC SCs exhibit significant areal and volumetric capacitances of 2.41 mF cm–2 and 5.74 F cm–3, respectively, at 120 Hz, coupled with a rapid response speed indicated by a phase angle of –80.1°. Notably, this performance is superior to that of the state-of-the-art high-frequency SCs based on carbon materials. The results underscore the potential of MDCs as electrode materials for use in ultrafast SCs, with eventual implications for the miniaturization of electronic devices.

Utilizing in situ construction of N-doped hierarchical porous carbon to achieve electronic control of highly dispersed Pd nanoparticles for efficient catalytic hydrogenation of CO2 to formic acid

Hydrogenation of CO2 to produce formic acid/formate is a significant pathway for future energy storage and utilization. The development of heterogeneous catalysts with high activity and stability for this process is still a challenge. In this work, the in-situ N-doped hierarchical porous carbon derived from distiller's grains was used as a support for Pd-based catalysts (Pd/NC) to convert CO2 into valuable chemicals while making high-value use of waste biomass. The optimum catalyst, Pd/NC-800, shown exceptional catalytic performance, achieving a turnover frequency (TOF) of 2060h-1 at 100℃, 4MPa in the catalytic CO2 hydrogenation to formate reaction. Comprehensive experimental results and density functional theory calculations indicate that the electronic effect between the pyridine N in the support and the Pd nanoparticles (NPs) can make the Pd surface reach the state of electron enrichment and enhance the metal-support interaction. Moreover, the synthesized material has hierarchical pore structure, which provides abundant Pd anchor location sites and improves mass transfer efficiency. The results not only provide a feasible strategy for the preparation of efficient CO2 hydrogenation catalysts, but also break a new and effective avenue for the resource utilization of distiller's grains.

One-step synthesis of self-supporting porous Cu81(Ni,Co)19 intermetallic catalysts for hydrogen evolution reaction

The development of hydrogen evolution reaction (HER) catalysts with excellent performance is the key to the wide-scale application of hydrogen energy. Herein, this work facilely synthesizes the self-supporting porous Cu81(Ni,Co)19 electrocatalysts by dealloying ZrNiCoCuAl amorphous alloy in HF solution. By regulating the composition of ZrNiCoCuAl amorphous alloy dealloying precursor, the porous Cu81(Ni,Co)19 composite synthesized by dealloying Zr60Ni8Co8Cu16Al8 amorphous alloy demonstrates the great HER performance with an overpotential of 35mV at 10mAcm-2 and a Tafel slope of 73.3mV dec-1. The outstanding catalytic performance of porous Cu81(Ni,Co)19 is attributed to the hierarchical porous structure, low charge transfer resistance as well as the synergistic interactions among the Cu, Ni and Co elements. Moreover, the theoretical calculations indicate that the constituent Cu, Co and Ni elements in the Cu81(Ni,Co)19 intermetallic alloy can act synergistically to optimize the free energy of hydrogen adsorption, therefore improve HER activity.

Convert bamboo into high-performance, long-time durability, and fire-retardant with hyperbranched polyethylene glycol and boron

Despite renewable bamboo globally available and has been applied in industry, the bamboo modification still absents for achieving long-term anti-mildew, stability and desirable toughness, owing to its inherent hierarchical porous structures, that cannot fully insert and retain ideal drugs/polymers. Hence, a hyperbranched polymer (HPB) with polyether as backbone and phenylboronic acid as binding groups via epoxy ring-opening reactions with amino was designed, and subsequently in situ synthesized in the multi-scaled cellular structures in bamboo. It was demonstrated that the hyperbranched polyether chains filled and swollen the hierarchical bamboo cell walls, which could efficiently replace the inner hydroscopic water in bamboo and greatly improved the bamboo stability, resulted in the wet swelling and dry shrinkage rates reduced by 20.3 % and 14.8 %, respectively. Both the side groups of phenylboronic acid and epoxy on HPB outer layers could generate covalent bonding with bamboo cell walls, which twisted the easy-losing facts of boron and gained a 60.6 % retention rate, surpassed most reported modified bamboo literatures and conferred bamboo with good fire resistance and long-time anti-mildew performance. Importantly, with the cavitation effect of HPB to help stress transmission, the modified bamboo had not expensed bamboo strength, instead of reaching satisfied bending strength and toughness at 154.1 MPa of flexure strength and 10.8 % of bending strain, respectively. That expand the industrial application of bamboo.

Imidazole-based organic polymer frameworks as metal- and halogen-free heterogeneous platforms for efficient CO2 cycloaddition

Developing effective metal- and halogen-free heterogeneous catalysts for the CO2 cycloaddition remains a challenge. In this study, novel imidazole-based hyper-crosslinked polymers (HCP-BZ, HCP-BP and HCP-TBZ) with abundant N sites were constructed via a one-pot polymerization, and employed as heterogeneous catalysts for the CO2 cycloaddition reaction. The special skeletal pore structure with abundant hierarchical pore structures and uniformly distributed active sites were demonstrated by various characterization technologies. The optimal HCP-TBZ(16:1) exhibits a good CO2 selective adsorption performance with a CO2 adsorption capacity of 2.23 mmol/g and CO2/N2 adsorption selectivity of 41 at 273 K and 0.1 MPa. Additionally, the resulting catalyst HCP-TBZ(16:1) achieves an excellent catalytic performance with 96 % yield and 99 % selectivity without metal, halogen, cocatalyst and solvent additions (120 °C, 1.0MPa CO2, 5 h). Moreover, the HCP-TBZ(16:1) also exhibits a satisfactory catalytic activity under the mild conditions (70 °C, 1.0 MPa CO2), and can effectively catalyze the cyclic carbonate preparation from the dilute CO2 (15 %CO2/85 %N2). The comparable catalytic activity and the determined structural stability, reusability and universality make the prepared imidazole-based HCPs a potential heterogeneous catalyst candidate for the CO2 cycloaddition. This study will provide some guidance for developing metal-free and halogen-free CO2 adsorption and conversion platforms.

Hierarchical Porous N-Doped Carbon Particles Derived from ZIF-8 as Highly Efficient H2S Selective Oxidation Catalysts.

In the selective oxidation of H2S, the catalytic activity over N-doped carbon-based catalysts is significantly influenced by the accessibility of active sites and the mass transfer rates of reactant molecules (e.g., H2S and O2) as well as generated sulfur monomers. Therefore, it is crucial for enhancing the initial performance via the controlled synthesis of carbon-based catalysts with highly exposed active sites and unique porous structures. Herein, we reported on an efficient strategy to synthesize nanosized N-doped carbon particles with hierarchical porous structures by directly pyrolyzing an oversaturated NaCl-encapsulated ZIF-8 precursor mixture. The introduction of NaCl not only serves as a pollution-free template to promote the formation of graphitic carbon layers but also acts as an intercalating agent to guide the derivation of hierarchical porous structures, as well as enhances the amount of active nitrogen species in the catalysts. As a result, the as-prepared H-NC800 catalyst shows excellent H2S selective oxidation performance (sulfur formation rate is 794 gsulfur·kgcat-1·h-1), good stability (>80 h), and antiwater vapor properties. The characterization results and DFT calculations indicate the crucial role of pyridinic N in the adsorbing and activating reactant molecules (H2S, O2). Furthermore, nanoscale N-doped carbon particles accelerated the rapid transport of generated sulfur monomers under a hierarchical porous structure. This investigation introduces a distinctive strategy for synthesizing ZIF-8-derived N-doped carbon nanosized with a hierarchical porous structure, while its efficient and stable H2S selective oxidation performance highlights significant potential for practical implementation in the industrial desulfurization process.

Fabrication of Laser-Induced Graphene on Carbon Electrodes for Efficient Hydrogen Evolution Reaction

Hierarchical porous carbon materials have received significant attention for application in catalytic water splitting because of their high efficiency, cost-effectiveness, and biocompatibility. In this study, laser-induced graphene (LIG) was fabricated on a carbon film- (CF-) type substrate for an efficient hydrogen evolution reaction (HER). The LIG-CF electrode was fabricated via laser-induced graphitization on a commercial polyimide (PI) film, followed by the pyrolysis of the LIG on the PI film (LIG-PI). During pyrolysis, the microscopic and material properties of the LIG remained intact, as verified through various characterizations. The as-prepared all-carbon electrode was then utilized as an electrode for the HER study in a 1.0 M KOH electrolyte and compared with LIG-PI and Pt electrodes. In the HER experiments, the optimized LIG-CF electrode exhibited excellent catalytic performance with zero-onset potential, and the potentials required to achieve high current densities of 10 and 20 mA/cm2 were 134 and 139 mV (vs. reversible hydrogen electrode (RHE)), respectively. The excellent performance of the LIG-CF electrode originates from the hierarchical porous structure of the LIG material, which serves as an electrochemically active site, and carbon substrate that facilitates the fast transport of ions at the electrode/electrolyte interface. Additionally, the carbon substrate shortens the transportation length of electrons which played a significant role for the enhanced performance of the LIG-CF electrode.

Precise Construction of Nitrogen-Enriched Porous Ionic Polymers as Highly Efficient Sulfur Dioxide Adsorbent.

Porous ionic polymers with unique features have exhibited high performance in various applications. However, the fabrication of functional porous ionic polymers with custom functionality and porosity for efficient removal of low-concentration SO2 remains challenging. Herein, a novel nitrogen-enriched porous ionic polymer NH2Py-PIP is prepared featuring high-content nitrogen sites (15.9wt.%), adequate ionic sites (1.22mmolg-1), and a hierarchical porous structure. The proposed construction pathway relies on a tailored nitrogen-functionalized cross-linker NH2Py, which effectively introduces abundant functional sites and improves the porosity of porous ionic polymers. NH2Py-PIP with a well-engineered SO2-affinity environment achieves excellent SO2/CO2 selectivity (1165) and high SO2 adsorption capacity (1.13mmolg-1 at 0.002bar), as well as enables highly efficient and reversible dynamic separation performance. Modeling studies further elucidate that the nitrogen sites and bromide anions collaboratively promote preferential adsorption of SO2. The unique design in this work provides new insights into constructing functional porous ionic polymers for high-efficiency separations.

Simple synthesis of acyl coupling conjugated microporous polymers monolithic material for synergistic capture of PM and CO2 in flue gas and process simulation

Adsorption and separation technologies based on physical adsorbents have the advantages of simple operation, low heat of adsorption and easy regeneration. They have received much attention for the capture of CO2 and PM from flue gases. However, the inherent “trade-off” between adsorption capacity and adsorption selectivity, as well as the high gas permeation resistance after powder processing and shaping, severely limit the prospects for industrial applications. Here, acyl functional groups were strategically introduced into polymer frameworks to successfully synthesize monolithic adsorbents (AC-CMPs) with a hierarchical pore structure for PM capture and CO2/N2 selective adsorption. The three-dimensional network structure composed of aligned hollow nanotubes effectively enhances the dispersion and mass transfer of gas flow per unit volume. Based on the porous media, multiphase flow model and discrete phase model, the gas flow process of PM trapped by AC-CMPs was simulated using Fluent. The simulation dynamically revealed the relationship between permeability resistance and filtration efficiency. The highly delocalized π-π conjugated porous skeleton linked by continuous covalent bonds endowed AC-CMPs with good stability, which prevented them from degrading in humid and high-temperature environments, thus keeping the adsorption capacity unchanged. The high polarity environment generated by the open oxygen atoms within the AC-CMPs framework, along with a high micro/mesopore ratio, enable it to achieve a CO2 adsorption capacity of 2.07 mmol/g at 273 K and 1 bar. Ideal adsorption solution theory calculations (IAST) and CO2/N2 column breakthrough experiments confirmed the excellent CO2 selectivity of AC-CMPs under realistic carbon capture conditions.

One-pot synthesis of interconnected carbon-coated silicon nanosheets from clay minerals for high-performance lithium-ion battery anodes

The silicon nanosheet/carbon composite emerges as a promising anode material for the next-generation commercial lithium-ion batteries. However, complex, costly, and energy-intensive synthesis procedures impede its practical application. Herein, the carbon-coated silicon nanosheets (Si/C) have been successfully synthesized via a one-pot strategy, involving a modified magnesiothermic reduction of talc followed by a reaction with CO2. The distinct chemical composition and layered nanostructure of talc enable the retention of Si nanosheets during exothermic reactions without additional templates or heat absorbents. The method shows significant potential for the scalable production of Si/C owing to the abundant silicon source, sustainable carbon source, and straightforward protocol. The resulting Si/C displays a hierarchical porous structure, with both macropores and mesopores, and an interconnected network of carbon-coated Si nanosheets. These structural characteristics facilitate rapid Li+ diffusion and enable the material to accommodate the lithiation-induced mechanical strains. As a result, the Si/C electrode exhibits outstanding electrochemical performance, including a remarkable rate capability (with a specific capacity of 1220 mAh g−1 at 10.0 A g−1) and a high initial Coulombic efficiency of 88%. The work opens a new avenue for the development of Si/C composites from natural clay minerals through an economical and scalable strategy, which would contribute to the practical application of advanced Si-based anodes in lithium-ion batteries.