Terminal Functional Groups Research Articles

Robust Sodium Storage Enabled by Heterogeneous Engineering and Electrolyte Modification

AbstractThe modulation of heterointerfaces in 2D materials is critically important for improving the electrochemical performance of sodium‐ion batteries (SIBs). In this context, the MoS2/Ti3C2Tx MXene heterostructure is taken as a typical example to reveal the fundamental principle of high sodium storage performance by regulating the terminal groups of Ti3C2Tx. It is demonstrated that MoS2/Ti3C2(OH)x (M/‐(OH)x) heterostructure with a high work function difference generates an enhanced built‐in electric field, which facilitates charge transfer. Moreover, ether‐based electrolytes, when compared to ester‐based electrolytes, provide lower solvation‐free energies and exhibit high compatibility with M/‐(OH)x, resulting in superior rate capability. Notably, COMSOL simulations of sodium ion (Na+) concentration and Na+ flux distributions reveal that the M/‐(OH)x electrode has low concentration polarization and rapid diffusion kinetics in ether‐based electrolytes. Consequently, the combination of M/‐(OH)x heterostructure with the ether‐based electrolyte provides 224.06 mAh g−1 after 1000 cycles at 5.0 A g−1. Furthermore, the Na3V2(PO4)3/C//M/‐(OH)x full cell demonstrates robust electrochemical performance, delivering 116.49 mAh g−1 after 140 cycles at 1.0 A g−1. These findings emphasize the impact of modulating terminal functional groups to optimize the electrochemical functionality of heterostructures and highlight the crucial role of electrode/electrolyte synergistic coupling in advancing the practical applications of SIBs.

Natural Chiral Ligand Strategy: Metal-Catalyzed Reactions with Ligands Prepared from Amino Acids and Peptides

Amino acids and peptides are readily available biomolecules and can function as chiral ligands for transition metal catalysis. An example is the copper complex catalyzed 1,4-addition of dialkylzinc to acyclic enones, which employs peptide ligands. This review provides a dataset of amino acids and peptides reported in the literature proving to be effective ligands for metal-centered catalysts. Several parameters were highlighted, including amino acid combination, metal atoms, carboxyl and amino protecting groups, modification of natural amino acids, and the mechanism of catalysis. Along with analyzing physical-chemical properties, the SMILES representation for each amino acid and/or peptide was generated and made available online, providing an easy-to-use means of training machine learning models. This review offers an opportunity for the development of more efficient peptide ligands for enantioselective metal-centered catalysts. The available online dataset is a reliable manually curated table, it enables the benchmark for comparison of new terminal functional groups. Moreover, the review provides insight into the structures of the more successful peptide ligands and can be used as the foundation for the development of the next generation of peptide-based chiral ligands.

Conjugated Group Tuning of Self‐Assembled Monolayer for Efficient Hole‐Transport Layer in Organic Solar Cells

AbstractP‐type carbazole‐derived self‐assembled monolayers (SAMs) have garnered significant attention as promising hole transport layers (HTLs) in the development of highly efficient organic solar cells (OSCs). However, it still lacks the effective navigation to modulate the terminal functional groups of SAMs to achieve a compromise between the highest occupied molecular orbital (HOMO) energy levels and self‐aggregation behavior. Herein, the terminal functional groups are adjusted and three SAMs are synthesized, namely, t‐Bu‐3PACz, Ph‐3PACz, and Bz‐3PACz to comprehensively investigate their intrinsic properties and influence on photovoltaic performance. Among them, Ph‐3PACz featuring an exceptionally suitable conjugated region and steric hindrance exhibits the best compatibility with the active layer, superior electrical conductivity, HOMO energy level aligning with polymer donor, and ordered film packing. As a result, the photovoltaic devices based on Ph‐3PACz exhibit an open‐circuit voltage (VOC) of 0.850 V, a short‐circuit current density (JSC) of 28.7 mA cm−2, and a fill factor (FF) of 78.5%, thus resulting in a remarkable power conversion efficiency (PCE) of 19.2%. This work provides an effective and easily navigable method to modulate the molecular packing and energy levels of SAMs, thereby achieving highly efficient OSCs.

Unprecedented cubic mesomorphic behaviour of crown-ether functionalized amphiphilic cyclodextrins.

Amphiphilic supramolecular materials based on biodegradable cyclodextrins (CDs) have been known to self-assemble into different types of thermotropic liquid crystals, including smectic and hexagonal columnar mesophases. Previous studies on amphiphilic CDs bearing 14 aliphatic chains at the primary face and 7 oligoethylene glycol (OEG) chains at the secondary face showed that the stability of the mesophase can be rationally tuned through implemation of terminal functional groups to the OEG chains. Here, we report the syntheses of first examples of crown ether-functionalized amphiphilic cyclodextrins that unexpectedly form thermotropic bicontinuous cubic phases. This constitutes the first reported examples of cyclodextrins forming such phases, which are potentially capable of 3D ion transport. Lithium composites were made to assess lithium conduction in the material. XRD revealed the added lithium salt destabilizes the cubic phase in favour of the smectic phase. Solid-state NMR studies showed that these materials conduct lithium ions with a very low activation energy.

Highly selective triethylamine gas sensor based on ZnO/Ti3C2Tx MXene self-assembly heterostructure

MXenes, as new two-dimensional transition metal compounds, has become promising sensing materials due to the excellent metal conductivity, abundant adsorption sites and the terminal groups of -O, -OH and -F. In this study, we report the well-etched accordion-like Ti3C2Tx by removing Al layer in Ti3AlC2, where Tx represents a wealth of terminal functional groups (-OH, -F, -O, etc.). In addition, unique hierarchical self-assembly ZnO/Ti3C2Tx nanocomposites are synthesized by hydrothermal method. The Brunauer-Emmett-Teller Method investigation also shows that the ZnO/Ti3C2Tx nanocomposites has a specific surface area of about 22.08 m2/g, and the pore size is mainly located at 11.1 nm. The innovative nanostructure is conducive to the adsorption and response of gas molecules. By investigating the gas sensitive properties of the sensors, it is found that the response of the ZnO/Ti3C2Tx sensor to triethylamine (TEA) is improved by 66 times and 1.58 times over that of pure Ti3C2Tx and ZnO, and the optimal operating temperature is 60℃ lower than that of pure ZnO. In addition, the LOD (Low Of Detection) of about 32.7 ppb indicates that the ZnO/Ti3C2Tx sensor is suitable for the detection of low concentrations TEA. The sensing performances of the ZnO/Ti3C2Tx sensor at a high humidity of 75 % RH verifies the strong sensing performance in high humidity environment. Furthermore, the composite sensor stabilize in 6 repetitive tests and present slight decrease in response value over 30 days. The excellent TEA sensitive properties indicate that the ZnO/Ti3C2Tx nanocomposite sensor may have promising applications in the gas sensitive field.

Double transition metal MXenes for enhanced electrochemical applications: Challenges and opportunities

AbstractDouble transition metal (DTM) MXenes are a recently discovered class of two‐dimensional composite nanomaterials with excellent potential in energy storage applications. Since their emergence in 2015, DTM MXenes have expanded their composition boundary beyond traditional single‐metal carbide and nitride MXenes. DTM MXenes offer tunable structures and properties through variations in the constituent transition metals and positioning within the layered lattice. These MXenes can exist in two primary forms: ordered DTMs and solid solutions. The compositional versatility of DTM MXenes offers opportunities to enhance their performance in electrochemical energy storage applications. However, the quality, stability, and surface chemistry of DTM MXenes are influenced by several factors, including the etching process, etchant type, and synthesis route. Currently, limited literature is available on experimentally synthesized DTM MXenes, with most studies focusing on carbide‐based MXenes. Most of the articles have dedicated their efforts only to generalized synthesis strategies. Although extensive theoretical studies have explored the suitability of etchants, synthesis parameters, and methods for producing high‐quality MXene with selective terminal functional groups, their stability issues have not been thoroughly examined. This review addresses various types of DTM MXenes, their synthesis techniques, and the impact of these methods on their physicochemical properties and electrochemical performance. Additionally, it provides a critical analysis of the causes of instability in MXenes, particularly DTMs, from synthesis to application. The challenges associated with these materials are discussed, along with opportunities and prospects for enhancing synthesis, structural tuning, surface modification, and applications in electrochemical energy storage.image

Ultrastable NAC-Capped CdZnTe Quantum Dots Encapsulated within Dendritic Mesoporous Silica As an Exceptional Tag for Anti-Interference Fluorescence Aptasensor with Signal Amplification.

In this work, we explored the potential of thiol-capped CdZnTe quantum dots (QDs) as an exceptional signal tag for fluorescence aptasensing applications. Employing a one-pot hydrothermal approach, we modulated the terminal functional groups of CdZnTe QDs using l-cysteine (Lcys), 3-mercaptopropionic acid (MPA), and N-acetyl-l-cysteine (NAC) as ligands. Our comparative analysis revealed that NAC-capped CdZnTe QDs (NAC-CdZnTe QDs) exhibited superior anti-interference capabilities and storage stability across various temperatures, pH levels, and storage durations. Encouraged by these promising results, we further optimized the use of ultrastable NAC-CdZnTe QDs encapsulated in dendritic mesoporous silica nanoparticles (DMSN@QDs) as an exceptional tag for the development of an advanced anti-interference fluorescence aptasensor for aflatoxin B1 (AFB1) detection. The developed aptasensor using DMSN@QDs as signal tags achieved a remarkable signal amplification of approximately 10.2 fold compared to the NAC-CdZnTe QDs coated silica (SiO2@QDs) labeled fluorescence aptasensor. This aptasensor was able to detect AFB1 within a wide range of 1 pg mL-1 to 200 ng mL-1, achieving a limit of detection as low as 0.41 pg mL-1 (S/N = 3). Crucially, the specific binding affinity between the aptamer and the target enabled the aptasensor to be easily customized for various targets by simply replacing the aptamer sequence with the desired one. The exceptional potential of NAC-CdZnTe QDs, particularly when encapsulated in DMSNs, leads to the development of highly sensitive and selective anti-interference fluorescence aptasensors for various targets, thereby, paving the way for advancements in a diverse range of applications.

Tailoring surface terminals of Ti3C2Tx MXene microgels via interlayer domain-confined polyphosphate ammonium for flexible supercapacitor applications

The MXene material shows potential for flexible energy storage devices due to its high pseudocapacitance and mechanical flexibility. However, MXene nanosheet self-stacking and –F terminal functional groups can hinder active site and ion dynamics, thus affecting the energy storage performance. Herein, we present an interlayer domain-confined strategy that involves the introduction and crosslinking of ammonium polyphosphate (APP) confined to the interlayer of Ti3C2Tx MXene sheets, which induces gelation of the MXene to form a 3D network structure and enlarge their interlayer spacing. And then the cross-linked APP is converted into nitrogen and phosphorus terminals on Ti3C2Tx MXene via thermal treatment. The nitrogen terminals in the form of the pyrrole nitrogen and pyridine nitrogen, and phosphorus terminals of P–O bonds enhance the activity of the redox reaction and the dynamics of the ions, resulting in the boosted energy storage capacity of MXene. The density functional theory (DFT) calculations reveal that nitrogen-phosphorus co-doping modulates the surface electronic states of MXene and contributes to the increase of the electrical conductivity of Ti3C2Tx MXene. As a supercapacitor electrode, Ti3C2Tx MXene with N/P terminals exhibits a higher specific capacitance of 597.8 F/g (1777F cm−3) than the raw Ti3C2Tx MXene (384 F/g). In addition, the quasi-solid state flexible symmetric supercapacitor assembled by Ti3C2Tx MXene with N/P terminals can achieve an energy density of 12.5 Wh kg−1 at a power density of 250 W kg−1. Therefore, this work provides a new strategy for terminal modification of MXene and high-performance MXene supercapacitors.

Design, synthesis and biological evaluation of glucose metabolism inhibitors as anticancer agents

Compared to normal cells, tumour cells exhibit an upregulation of glucose transporters and an increased rate of glycolytic activity. In previous research, we successfully identified a promising hit compound BH10 through a rigorous screening process, which demonstrates a potent capacity for inhibiting cancer cell proliferation by targeting glucose metabolism. In the current study, we identify Kelch-like ECH-associated protein 1 (Keap1) as a potential protein target of BH10via avidin pull-down assays with biotinylated-BH10. Subsequently, we present a comprehensive analysis of a series of BH10 analogues characterized by the incorporation of a naphthoimidazole scaffold and the introduction of a triazole ring with diverse terminal functional groups. Notably, compound 4d has emerged as the most potent candidate, exhibiting better anti-cancer activities against HEC1A cancer cells with an IC50 of 2.60 μM, an extended biological half-life, and an improved pharmacokinetic profile (compared to BH10) in mice.

MD simulations of diffusion of cyanobiphenyl molecules adsorbed on the graphene surface coated with alkane and alcohol molecules

AbstractMolecular dynamics simulations were carried out to study the structural and diffusion properties of a cyanobiphenyl monolayer composed of pentyl cyano biphenyl (5CB) and pentyloxy cyano biphenyl (5OCB) molecules on a graphene surface coated with alkane and alcohol molecules. To investigate the diffusion properties of 5CB and 5OCB molecules on the graphene surface, the molecules of pentane ( ) and dodecane ( ) from alkanes and dodecanol ( ) from alcohols with a polar hydroxyl ( ) terminal functional group were chosen as orienting surfactant molecules. It was found that the diffusion ability of cyanobiphenyl molecules in a graphene substrate coated with alkane and alcohol molecules depends on the chain length of these molecules and on the presence of polar hydroxyl –OH terminal groups. With an increase in the length of alkane molecules from to , the value of the diffusion coefficient (or ), it decreases slightly, while the presence of the polar hydroxyl terminal group leads to a significant decrease in this diffusion coefficient of cyanobiphenyl molecules.

Rational Design and Engineering of Terminal Functional Groups in Dibenzothiophene‐Diphenylamine Small Molecular Electron Donors for Enhanced Photovoltaic Efficiency in All‐Small‐Molecule Organic Solar Cells

AbstractAll‐small‐molecule organic solar cells (ASM‐OSCs) offer advantages like well‐defined molecular structures and excellent reproducibility. However, lower photovoltaic efficiencies hinder their adoption due to limitations in designing small molecular electron donors (SMEDs) with optimal energy levels, light absorption, and optoelectronic properties. The present study addresses this gap by rationally designing a series of SMEDs (DBT‐2FA1 to DBT‐2FA6) through terminal acceptors engineering into dibenzothiophene core with diphenylamine side donors for potential applications in ASM‐OSCs. Density functional theory simulations are carried‐out to establish structure‐property relationships based on structural, electrochemical, photophysical, and charge transfer (CT) properties. Results show that the SMEDs exhibit low‐lying HOMOs for suitable energy level alignment with benchmark Y6 acceptor, promoting open‐circuit voltage and charge separation. The panchromatic absorption spectra covering Vis‐NIR region and maximum light harvesting efficiency are beneficial for high current‐density in ASM‐OSCs. Notably, the push‐pull mechanism within SMEDs results in dominant intramolecular CT with above 70% CT excitations. Whereas, a moderate variation in dipole moments and electrostatic potential differences with acceptor material led to 99.9% intermolecular CT, thus ensuring robust exciton dissociation and efficient photocurrent generation. Overall, this work provides a molecular‐level understanding of designing novel SMEDs and their compatibility with acceptor materials for developing future high‐performance ASM‐OSCs.

Recognition site modifiable tetrapodal receptor and the effect of alkane chains on monosaccharide recognition

Traditional molecular recognition studies usually focus on obtaining strong host–guest interactions, which may lead to the neglect of important tendencies caused by other factors. Moreover, most receptors typically fix their recognition sites in the backbone of the receptor, resulting in great synthetic challenges for varying recognition functional groups. In this contribution, we developed a new class of tetrapodal receptors. The terminal functional groups of the receptor can be varied by simple chemistry. Through 1H NMR titration experiments and binding constant analysis, the influence of the size and shape of alkane chains on monosaccharide recognition was investigated. The introduction of ester functional groups allows the access of moderate binding affinity to unveil otherwise masked contribution of dispersion force in saccharide recognition. These results also imply that stronger forces may not always be beneficial for host–guest binding while functional groups with a particular shape may favor the discrimination of isomers through steric hindrance effect. Thereby, these tetrapodal receptors and their analogues provide an ideal platform for comparing the effects of various functional groups on molecular recognition.

Assembling carbon nitride quantum dots into hollow fusiformis and loading CoP for photocatalytic hydrogen evolution

The self-assembled carbon nitride quantum dots (CNQDs) has been largely advanced owing to the structure-relative photocatalytic activities, especially its electronic structure, which can be regulated by defects, functional groups, and doping. However, there are still issues such as wide band gaps for the assembles and severe recombination of photoinduced charges. Herein, we demonstrate the self-assembly of CNQDs into fusiform hollow superstructures (CNFHs), induced by hydrogen bonding between the terminal functional groups (–OH, –COOH, and –NH2). During the top-down assembly process, the hydrogen bonding dominates and initiates lateral cross-linking between adjacent CNQDs, which further twist into fusiform hollow structures. Benefitted greatly from the ultrathin and hollow nature of the superstructure that provides more exposed active sites, coupled with the introduction of phosphorus doping atoms into the framework induced narrowed band gap, CNFHs exhibits an 18-fold higher activity than the bulk counterpart toward photocatalytic hydrogen evolution after loading the CoP co-catalyst. This work presents a new platform to design and manipulate carbon nitride superstructures.

Per- and polyfluoroalkyls used as cosmetic ingredients - Qualitative study of 765 cosmetic products

Per- and polyfluoroalkyl substances (PFAS) form a vast family comprising more than 4700 synthetic compounds. Their molecules contain a terminal functional group and a hydrophobic carbon tail (alkyl group) at which the hydrogen atoms are totally (in the case of perfluorinated compounds) or partially (in the case of polyfluorinated compounds) replaced by fluorine atoms. Due to the very specific properties of their structure, they have been used in a vast range of applications over the last 70 years. These substances are considered to be of concern for the environment. Their effects on human health are still poorly understood because studies are still too rare, but the cutaneous route could be a significant pathway of penetration.In this context, we made a qualitative study to assess the presence of PFAS in various cosmetics such as hygiene products, skin care products, make-up and perfumes.Among the 765 products studied, we found 11 different PFAS. Polytetrafluoroethylene (PTFE) and perfluorodecalin, present in 25.9% and 22.2% of products containing it, respectively, were the most frequent.Although the presence of this type of ingredient seems to be limited in Europe, make-up appears to be the type of product most likely to contain PFAS.

Reaction mechanisms of α,ω-bifunctional molecules toward atomic layer deposition versus molecular layer deposition

Atomic layer deposition (ALD) and molecular layer deposition (MLD) are key techniques used to fabricate high-quality thin films. Organic α,ω-bifunctional precursors often exhibit different growth behaviors depending on the functional groups as well as the chain length of the molecular backbone, so that some organic precursors produce thin films of organic-inorganic hybrid materials, while others may deposit purely inorganic thin films without incorporation of the hydrocarbon moiety. In this study, we investigated the surface reaction mechanisms of α,ω-bifunctional molecules (X(CH2)nX, n = 2, 3, 4, 5, 6, and X = OH, SH, NH2) with diethylzinc toward MLD and ALD using density functional theory (DFT) calculations. It was found that the length of the aliphatic alkyl chain and the terminal functional groups of bifunctional organic precursors significantly influences their reactivity, resulting in the possibility toward removal or incorporation of the organic moiety in the product. Bifunctional reactants with longer alkyl backbones (n > 4) showed higher reactivity for removal of the hydrocarbon chain, facilitated by a ω-2 hydrogen transfer reaction. Furthermore, a reactivity trend of SH > OH > NH2 for removal of the hydrocarbon chains was observed. Our study provides in-depth theoretical insights into the adsorption reaction mechanisms occurring when bifunctional molecules are employed as organic reactants in ALD and MLD processes.

Unravelling competitive adsorption phenomena in the aqueous phase reforming of carboxylic acids on Pt catalysts: An experimental and theoretical study

Biorefinery-derived wastewater is considered a valuable source of energy and chemicals thanks to its organic loading. However, it is constituted by different compounds which influence the performance of a catalytic valorization process. In this work, we investigated the treatment of a synthetic hydrothermal liquefaction-derived wastewater (HTL-WW) via aqueous phase reforming (APR) to obtain hydrogen. As a case study, we examined the underlying driving forces for performance differences in the APR of mono- and bi-component solutions of carboxylic acids as a model corn stover HTL-WW over Pt catalysts via a combined experimental and theoretical approach. In mono-component solutions, the conversion ranked as glycolic acid > propionic acid ≈ acetic acid, and the same was found for the hydrogen production tendency. Binary solutions of glycolic and acetic acid, with different concentration among the constituents, showed a strong inhibition of the acetic acid reactivity due to the prevalent adsorption of glycolic acid on Pt surface. The results from the APR of acetic and propionic acid solutions were less affected by such phenomena. DFT results showed that there are strong, attractive lateral interactions between carboxylic acids due to intermolecular hydrogen bonding that cause all carboxylic acids to preferentially adsorb in dimer structures. The lateral interaction strength was determined for both pure and binary mixtures of carboxylic acid dimers, with results showing that pure mixtures of carboxylic acids have stronger attractions and that glycolic acid dimers see the strongest attractions due to the added terminal hydroxyl functional group. The findings presented herein offer significant insights into the utilization of APR for industrial-like multi-component solutions, as well as for any catalytic process involving small organic compounds in an aqueous phase.

Probing fragment ion reactivity towards functional groups on coordination polymer surfaces.

Functionalization of surface-grown coordination polymer layers by ion soft-landing of highly reactive molecular fragment ions is demonstrated. The ions form covalent bonds to terminal functional groups of the polymer at the vacuum interface, opening new perspectives for controlled bond formation using reactive ions.

Altering the Interfacial Microenvironment of the Photocatalytic System for Boosted H2O2 Generation from Biomass Waste

The catalytic and environmentally friendly synthesis of H2O2 is crucial in green chemistry. Many researchers are dedicated to its study, and various methods have been proposed, but these methods usually require organic solvents or dissipative reagents. It has been reported recently that different biomass could be converted to hydrothermal carbonaceous carbon (HTCC) photocatalysts capable of producing H2O2 with high efficiency. Herein, we report a method to further increase the catalytic efficiency of HTCC, from 0.53 mmol gcat -1 h-1 to 1.35 mmol gcat -1 h-1 under air, by simply changing the neutral solution to basic (pH = 11) where the contact environment between HTCC and the solvent is changed. The radical trap experiment and electron paramagnetic resonance (EPR) spectroscopy confirmed a two-step oxygen reduction reaction as the primary catalytic pathway. The mechanism study indicates that OH- in the solution could react with the acidic terminal functional groups of HTCC originating from the synthesis and hole-induced oxidation within HTCC during photocatalysis, thus enhancing the generation of active species and electron transfer. This study paves a new way to improve the photocatalytic efficiency of HTCC by altering the microenvironment of solvent and photocatalysts.

Tuning graphitic carbon nitride (g-C3N4) electrocatalysts for efficient oxygen evolution reaction (OER)

Nowadays, energy conversion and storage technologies are essential research topics due to the necessity of more sustainable processes. Specifically, water splitting is highly affected by slow kinetics and limited knowledge of the oxygen evolution reaction (OER). This work envisages the preparation of graphitic carbon nitride (g-C3N4) electrocatalysts for efficient OER by a facile one-pot method. The impact of the preparation temperature (450–650 °C) of g-C3N4 was assessed for the first time on water splitting processes and explained by different characterisation techniques. The unique crystal structure, surface chemistry, and electronic properties of the material prepared at 550 °C lead to a remarkable OER efficiency, with an overpotential of 355 mV at 10 mA cm−2 and a Tafel slope of 46.8 mVdec−1. Interestingly, three major differences were observed when comparing the material prepared at 550 °C with those obtained at other temperatures: the reduced structural distortion, the superior composition in oxygen and the presence of terminal functional groups. Also, compared to other metal-free g-C3N4 electrocatalysts reported in the literature, we achieved lower Tafel slope values without additional post-treatments or co-catalysts. Hence, for the first time a metal-free catalyst defeats benchmark IrO2. The prepared electrodes were stable for up to 45 h, even when increasing the applied current density to 100 mA cm−2 for 15 h. Thus, this work provides a simple route for the fabrication of highly-efficient and long-lasting electrocatalysts for a remarkable OER performance.

Enhancing the cycling stability of Li-S batteries with flexible freestanding sulfur cathodes through a spider-hunting strategy

Flexible, high-capacity, and long-lasting freestanding sulfur cathodes are essential for developing advanced lithium-sulfur (Li-S) batteries in next-generation flexible electronic devices. However, the severe shuttle effect of lithium polysulfides (LiPSs) hinders their potential applications. This work introduces a flexible freestanding MX-CPNTs-CNTs@NS cathode for Li-S batteries by utilizing a spider-hunting strategy. In this strategy, carbonized polypyrrole nanotubes (CPNTs) and carbon nanotubes (CNTs) intertwine to form a 3D flexible and conductive spiderweb-like skeleton. The incorporation of MXene nanosheets as a function of spiders enables the regulation of a rich hierarchical porous structure. Additionally, the polar terminal functional groups of MXene nanosheets and the pyridinic N of CPNTs contribute to the chemical adsorption and electrocatalysis of LiPSs. The synergistic effect of physical and chemical inhibition strategies results in stable electrochemical performance, including a high specific capacity of 1203.2 mAh/g at 0.1C, and extended cycling stability of 739.6 mAh/g at 1C after 500 cycles (low decay rate of 0.036%). The excellent flexibility, specific capacity, and cycling stability make the freestanding MX-CPNTs-CNTs@NS cathode promising for high-performance flexible electronic devices.