Coordination Bonds Research Articles

MOF-derived strategy for in-situ assembly of nickel phyllosilicate nanoflowers: Enhancing smoke suppression, flame retardancy and mechanical properties of epoxy resins

Epoxy resin (EP) is a highly versatile polymer extensively used in high-end applications, including aerospace components, electronics encapsulation and adhesives. To custom-design flame retardant materials for high-performance epoxy resins, a MOF-derived zeolitic imidazolate framework-8@nickel phyllosilicate (ZIF@Ni-PS) was synthesized through the in-situ assembly of nickel phyllosilicate nanoflowers. The results showed that the smoke suppression, flame retardancy, and mechanical properties of the EP composites containing 5 wt% ZIF@Ni-PS were significantly enhanced. The peak heat release rate (pHRR) and the peak smoke production rate (pSPR) were reduced by 33.2% and 12.7%, respectively. The presence of ZIF@Ni-PS promoted the formation of a dense, high-quality carbon layer that isolated heat and oxygen transfer, effectively reducing heat release during combustion and suppressing smoke generation. Furthermore, the imidazole ring and Zn ions on the surface of ZIF@Ni-PS facilitated the formation of coordination and hydrogen bonds with the epoxy (EP), thereby enhancing the dispersion, compatibility, and mechanical properties of the epoxy resin matrix. This study presents a straightforward preparation method for high-performance EP composites, providing a novel pathway for EP research.

Gallocyanine-mediated non-covalent functionalization and exfoliation of h-BN for efficient anticorrosion reinforcement of waterborne epoxy coating

Hexagonal boron nitride (h-BN) is commonly used to enhance the anti-corrosion of organic coatings due to its excellent barrier properties, dielectricity and mechanical robustness. However, the bulky h-BN tends to create poor dispersibility and interfacial compatibility problems with the resin matrix, leading to coating cracking and failure. H-BN nanosheets exfoliated by conventional methods only provide passive barrier effect with coatings at the initial stage of corrosion. Herein, we used a mussel-inspired non-covalent functionalization strategy, using the catechol groups and heteroaromatic ring structure of gallocyanine to achieve the functionalization and exfoliation of h-BN through ball milling, and obtained ultra-thin h-BN@G nanosheets. Remarkably, spare gallocyanine can further suppress the erosion, whose inhibition efficiency is 95.48 % at the concentration of 100 mg/L in 1 M HCl within 9 h. Typically, after 105 days of immersion in 3.5 wt% NaCl solution, the low-frequency impedance of h-BN@G/WEP coating is still as high as 1.45 × 109 Ω cm2, which is two orders of magnitude higher than that of the pure coating. The superior long-term anti-corrosion capacity can be ascribed to the triple protection of enhanced shielding property of desirable-exfoliated h-BN, passivation films adsorbed on the metal and coordination bonds formed between gallocyanine and the iron to resist the active corrosion. Our work offers an innovative idea for the functionalization and exfoliation of other lamellar materials, which can be applied to the implementation of long-lasting anti-corrosion coatings.

Band Structure Engineering in 2D Metal-Organic Frameworks.

The design of 2D metal-organic frameworks (2D MOFs) takes advantage of the combination of the diverse electronic properties of simple organic ligands with different transition metal (TM) centers. The strong directional nature of the coordinative bonds is the basis for the structural stability and the periodic arrangement of the TM cores in these architectures. Here, direct and clear evidence that 2D MOFs exhibit intriguing energy-dispersive electronic bands with a hybrid character and distinct magnetic properties in the metal cores, resulting from the interactions between the TM electronic levels and the organic ligand π-molecular orbitals, is reported. Importantly, a method to effectively tune both the electronic structure of 2D MOFs and the magnetic properties of the metal cores by exploiting the electronic structure of distinct TMs is presented. Consequently, the ionization potential characteristic of selected TMs, particularly the relative energy position and symmetry of the 3d states, can be used to strategically engineer bands within specific metal-organic frameworks. These findings not only provide a rationale for band structure engineering in 2D MOFs but also offer promising opportunities for advanced material design.

One-step green synthesis of melamine-modified cellulose nanofiber composite aerogels for efficient removal of Pb(II) and Cu(II): Experiments and DFT calculations

A composite aerogel (CGMA) with high porosity (98.32 %) and multiple active sites was prepared for the adsorption of Pb(II) and Cu(II) by sol-gel combined with freeze-drying process using melamine and (3-Glycidyloxypropyl)trimethoxysilane as cellulose nanofiber modifying materials. Characterized by SEM-EDS, XPS, FTIR, BET, MIP and TG, CGMA has a hierarchical pore structure and abundant adsorption sites. At pH = 6, the adsorption reached equilibrium within 120 min, following the Pseudo second-order kinetic model and the Langmuir model, with maximum capacities of 268.1 mg/g for Pb(II) and 152.6 mg/g for Cu(II). The process was primarily governed by homogeneous chemisorption. The coexisting ion, organic matter, and water quality experiments confirmed the excellent anti-interference properties of CGMA. Competitive adsorption experiments showed that CGMA has excellent selective adsorption performance for Pb(II). After 5 cycles, Pb(II) and Cu(II) adsorption performance decreased to 79.21 % and 83.40 %, respectively. FTIR, XPS, DFT and RDG analysis showed that amino groups and oxygen-containing groups were the main sites of adsorption. CGMA forms coordination bonds and complexes with Pb(II) and Cu(II) via amine and oxygen groups and adsorbs via electron transfer, hydrogen bonding, and van der Waals forces, with Pb(II) being more selective. CGMA has good prospects for application in heavy metal ion treatment.

Multifunctional organohydrogels enabling sensitive strain sensing and self-powered triboelectricity

Hydrogels have broad application prospects in portable strain sensors and triboelectric nanogenerators (TENG), and have attracted great attention in the field of wearable electronic devices and energy transfer devices. However, the development of multifunctional gels that can meet a variety of application scenarios is still a challenging problem. In this study, a multifunctional poly(acrylamide-co-2-acrylamide-2-methylpropanesulfonic acid)/lignosulfonate/Zr4+ organohydrogel noted as “P(AM-co-AMPS)/LS/Zr4+” was fabricated based on dynamic metal coordination bonds and hydrogen bonds, which could be used as flexible strain sensor and TENG electrode material. The organohydrogel based strain sensor could monitor both large and tiny human movements due to the high sensitivity (GF = 4.37, up to 200 %) and circulation stability. The assembled organohydrogel-based triboelectric nanogenerator (O-TENG) could generate an open-circuit voltage of 70.47 V and a short-circuit current of 25.21 μA. It is worth mentioning that the O-TENG could light up 44 LED bulbs by tapping with the palm at −20 °C, and the electronic output performance of the O-TENG after self-healing was unaffected. Additionally, the O-TENG exhibited enormous potentials in the biomechanical energy harvesting and self-powered motion sensors in the areas of human movements detection, human–computer interaction, electronic skin and self-powered devices.

Tough strippable hydrogel films based on acrylic acid/acrylamide/zirconyl chloride for surface radioactive decontamination at low temperatures

Strippable films are extensively utilised for the decontamination of radioactive surfaces because of their cost-effectiveness, ease of operation, and minimal liquid waste. However, traditional strippable detergents are formulated for use at normal ambient temperatures and typically lose their efficacy at low temperatures because of poor performance or excessively long film-forming time. In this study, we have developed an anti-freezing and sprayable AMZW detergent based on acrylic acid (AA), acrylamide (AM), zirconyl chloride octahydrate (ZrOCl2·8H2O), and water (H2O), which possesses a freezing point of approximately −34 ℃ due to the solvation interaction between Zr4+ and H2O. Even at temperatures as low as −25 ℃, the AMZW detergent can be easily sprayed using a conventional apparatus and rapidly cured into a strippable hydrogel film under irradiation by 365 nm UV LED light (LED@365 nm), household LED panel light, or sunlight. The coordination bond formed between Zr4+ and the carboxyl group of the polymer chain imparts excellent mechanical properties to the hydrogel while the carboxyl group can complex with uranyl nitrate hexahydrate (UO2(NO3)2·6H2O)—a radioactive simulant. As a result, the strippable hydrogel film demonstrates high tensile strength (6.1 ∼ 19.3 MPa), excellent flexibility (elongation of 90 ∼ 855 %), moderate peel strength (0.05 ∼ 3 N/cm, room temperature (RT)), and high decontamination efficiency (>91.6 % on stainless steel and glass; >81.3 % on concrete) over a wide range of temperatures (−25 ∼ 25 ℃). This work presents a novel approach for producing anti-freezing, fast-forming, flexible, and high-strength strippable hydrogel films for surface radioactive decontamination at low temperatures.

‘Rigid–flexible’ strategy for high-strength, near-room-temperature self-healing, photo-thermally functionalised lignin-reinforced polyurethane elastomers

Lignin is the most abundant and only renewable aromatic polymer in nature. Herein, a flexible matrix and the rigid lignin were rationally integrated to prepare high-strength, near-room-temperature self-healing, processable lignin-reinforced polyurethane elastomers (LZPUs). Reversible hydrogen and oxime–amino ester bonds were introduced into the matrix to provide excellent dynamic properties and abundant ligands for lignin–matrix coordination bonds. Abundant metal coordination bonds were constructed between the matrix and lignin via the introduction of Zn2+, which not only effectively enhances the dispersibility and compatibility, but also provides an excellent energy dissipation mechanism for the LZPUs. One of the prepared elastomers, LZPUs, exhibited a high strength of 40.5 MPa, which is twice that of the blank sample and 1.6 times that of the sample without Zn2+. It maintained kinetic stability at mild temperature, but it exhibited a self-healing efficiency of 91.3 % in strength and 99.8 % in elongation at break after decoupling with trace ethanol (≈ 50 μL) at 35 °C. It exhibited a self-healing efficiency of 93.6 % in strength under 1 sun irradiation (0.1 W cm−2) for 4 h. We believe this elastomer offering high mechanical properties with multi-functionality can be applied in flexible drives and photo-thermal power generation.

Tumor Microenvironment Activated Cu Crosslinked Near-Infrared Sonosensitizers for Visualized Cuproptosis-Enhanced Sonodynamic Cancer Immunotherapy.

Reactive oxygen species (ROS)-mediated sonodynamic therapy (SDT) holds increasing potential in treating deep-seated tumor owing to the high tissue-penetration depth. However, the inevitable accumulation of sonosensitizers in normal tissues not only make it difficult to realize the in situ SDT, but also induces sonodynamic effects in normal tissues. Herein, this work reports the passivation and selective activation strategies for the sonodynamic and near-infrared (NIR) imaging performances of an intelligent antitumor theranostic platform termed Cu-IR783 nanoparticles (NPs). Owing to the ruptured coordination bond between IR783 with Cu ions by responding to tumor microenvironment (TME), the selective activation of IR783 only occurred in tumor tissues to achieve the visualized in-situ SDT. The tumor-specific released Cu ions not only realized the cascade amplification of ROS generation through Cu+-mediated Fenton-like reaction, but also triggered cuproptosis through Cu+-induced DLAT oligomerization and mitochondrial dysfunction. More importantly, the immunosuppressive TME can be reversed by the greatly enhanced ROS levels and high-efficiency cuproptosis, ultimately inducing immunogenic cell death that promotes robust systemic immune responses for the eradication of primary tumors and suppression of distant tumors. This work provides a distinct paradigm of the integration of SDT, CDT, and cuproptosis in a controlled manner to achieve visualized in-situ antitumor therapy.

Mechanically robust and highly conductive bacterial cellulose hydrogels through synergy of directional freeze–thawing and salting-out for wearable sensors

It is urgent to develop high-performance conductive hydrogels that simultaneously exhibit high biocompatibility, mechanical robustness, exceptional conductivity and frost resistance to fulfil the requirements of wearable flexible sensors. Herein, we present a simple and integrated approach for designing iso/anisotropic bacterial cellulose (BC) hydrogels by immersing the as-prepared polyvinyl alcohol (PVA)–BC–Borax hydrogels in saturated NaCl solutions using a salting-out effect to assist the non–/directional freeze–thawing strategy. Benefitting from the synergistic strengthening of molecular interactions, including hydrogen, coordination, and boron ester bonds, as well as the enhanced PVA and BC crystallinity resulting from the salting-out effect, the tensile strength (0.8–3.2 MPa) and high ionic conductivity (61.5–136.2 mS/cm) of isotropic hydrogels (PVA–BC–Borax/NaCl) can be well tuned by adjusting the feeding mass fractions of PVA, borax and BC. The optimised hydrogel, PVA7.5%–BC0.45%–Borax0.375%/NaCl, demonstrated remarkable mechanical properties (3.2 MPa, 295.1 %), ionic conductivity (72.6 mS/cm) and good anti-freezing properties (–40.8 °C), maintaining excellent conductivity (61.8 mS/cm) even at –20 °C due to the introduction of NaCl. When subjected to directional freeze–thawing cycles, the D(Directional)-PVA7.5%–BC0.45%–Borax0.375%/NaCl hydrogel, with its organised layers and larger pore–sized structures, exhibited higher breaking elongation (609.2 %) and ionic conductivity (81.6 mS/cm) than its isotropic counterpart (295.1 %, 72.6 mS/cm). The D-PVA7.5%–BC0.45%–Borax0.375%/NaCl hydrogel was successfully used as a strain sensor for detecting a variety of human movements, showing excellent responsiveness to external stimuli, thereby demonstrating its potential applications in human–machine interaction, flexible sensing and bioelectronics.

Synthesis and BSA binding study of the Cu(II) complex and applications of it to enhance catalytic activity for C(Sp2)-H bond functionalization and for the synthesis of polyhydroquinolines

Among the various copper-catalyzed coupling reactions, C–S and C–N bond-forming reactions have carried off plentiful recognition due to their demand in the synthesis of molecules having biological and pharmaceutical impact. Organo-copper complex has an incontestable supremacy over the other catalytic complex due to its low cost and the use of readily accessible and stable ligands. As a consequence and in continuation of our explorative studies in this direction, an efficient and novel organo-copper complex has been synthesized and characterized by spectroscopic (NMR, FT-IR) and single crystal X-ray diffraction (XRD) methods. The synthesized stable metal complex has fascinating physical, chemical, biological and catalytic properties. In the chemical exploration refer to protein-metal interactions; we have often used Bovine Serum Albumin (BSA) protein. The synthesized copper complex has the potential to form coordinate bonds with functional groups present in BSA, together with amino acid residues and the protein backbone. The binding of metal complexes to BSA has outstanding imputation in medicinal chemistry. For enhancement of the catalytic activity of the organo-copper complex, we have evaluated it in carbon-hetero bond formation reactions where it proffered an influential tool for the establishment of C–S and C–N bonds.

Aminated lignin and phytic acid-assisted polyacrylic acid hydrogel sensors with enhanced mechanical properties and strong adhesion

Excellent comprehensive performance of hydrogels can be achieved by synergistically combining multiple interaction mechanisms. In this study, a series of hydrogels with rapid gelation and excellent adhesive, mechanical, self-healing, and conductive properties, driven by covalent bonds and multiple reversible interactions, were constructed by mixing acrylic acid (AA), aminated alkaline lignin (AAL), phytic acid (PA), and Fe3+. The rigid skeletons of polyacrylic acid (PAA) and AAL, as well as the metal coordination bonds formed between them and Fe3+, enhance the mechanical properties of the samples. The samples exhibit excellent tensile strength and compressive strength, reaching 73.7 kPa and 4.6 MPa (under a compressive strain of 80 %), respectively, with a tensile strain of 1142 % under the same condition. Adding PA enhances the compliance and adhesion (148.2 kPa for porcine skin) of the gel and endowed it with good flame retardancy. Additionally, the sample maintained its good mechanical properties and conductivity even after five cutting-healing cycles. Good durability, robust adhesion, and high electrical conductivity of the sample render it a promising strain sensor for electronic devices. This work provides a design strategy for preparing hydrogels with superior adhesion and good comprehensive performance.

Clusters of solvated ferrous ion in water–ammonia mixture: Structures and noncovalent interactions

The behavior of metal ions is commonly studied in pure solvent although, in our daily life, these metals are involved in mixtures of solvents. In the present study, we investigated structures, relative stabilities and temperature dependance of solvated ferrous ion in water–ammonia mixture solvent at 0K and at various temperatures ranging from 25K to 400K. All the calculations are performed at the MN15 level of theory associated with the aug-cc-pVDZ basis set. For deep understanding of binding patterns in solvated ferrous ion in water–ammonia mixture solvent, noncovalent interactions are presented based on the QTAIM analysis using AIMAll. Our results prove that the ferrous ion is more stable when it is solvated by ammonia instead of water. In addition, hydrogen bonds are weakened by the presence of ammonia molecules. The temperature dependence of the different obtained geometries indicates that from s=6 (s is the sum of water and ammonia molecules around the ferrous ion), when the number of water molecules is almost equal to that of ammonia, the structures with coordination number 5 are dominant. However, the coordination number is six when there are a maximum water molecules (rich water solution) or maximum ammonia molecules (rich ammonia solution) around the ferrous ion (for s≥6). The QTAIM analysis shows that there are two coordination bondings and four hydrogen bondings. Furthermore, it is found that the Fe2+⋯N coordination bondings are stronger than the Fe2+⋯O confirming that the ferrous ion prefers to be solvated by ammonia instead of water.

Anchoring Catalytic Metal Nodes within a Single‐Crystalline Pyrazolate Metal‐Organic Framework for Efficient Heterogeneous Catalysis

The synthesis of single‐crystalline and robust pyrazolate metal‐organic frameworks (Pz‐MOFs) capable of facilitating challenging organic transformations is fundamentally significant in catalysis. Here we demonstrate a metal‐node‐based catalytic site anchoring strategy by synthesizing a single‐crystalline and robust Pz‐MOF (PCN‐1004). PCN‐1004 features one‐dimensional (1D) copper‐Pz chains interconnected by well‐organized ligands, forming a porous three‐dimensional (3D) network with two types of 1D open channels. Notably, PCN‐1004 displays exceptional stability in aqueous solutions across a broad pH range (1 to 14), attributed to the robust copper‐Pz coordination bonds. Significantly, PCN‐1004 functions as an outstanding catalyst in cross dehydrogenative coupling reactions for constructing C‐O/C‐S bonds, even in the absence of directing groups, achieving yields of up to ~99%, with long cycle lives and high substrate compatibility. PCN‐1004 outperforms all previously reported porphyrin‐based homogeneous and heterogeneous catalysts. Control experiments and computations elucidate the pivotal catalytic role of the copper‐Pz chains and reveal a free radical pathway for the reaction. This work not only demonstrates the successful implementation of a metal‐node‐based catalytic site anchoring strategy for the efficient catalysis of challenging organic transformations but also highlights the synergistic effect of a robust framework, 1D open channels, and active sites in enhancing catalytic efficiency within MOFs.

Anchoring Catalytic Metal Nodes within a Single-Crystalline Pyrazolate Metal-Organic Framework for Efficient Heterogeneous Catalysis.

The synthesis of single-crystalline and robust pyrazolate metal-organic frameworks (Pz-MOFs) capable of facilitating challenging organic transformations is fundamentally significant in catalysis. Here we demonstrate a metal-node-based catalytic site anchoring strategy by synthesizing a single-crystalline and robust Pz-MOF (PCN-1004). PCN-1004 features one-dimensional (1D) copper-Pz chains interconnected by well-organized ligands, forming a porous three-dimensional (3D) network with two types of 1D open channels. Notably, PCN-1004 displays exceptional stability in aqueous solutions across a broad pH range (1 to 14), attributed to the robust copper-Pz coordination bonds. Significantly, PCN-1004 functions as an outstanding catalyst in cross dehydrogenative coupling reactions for constructing C-O/C-S bonds, even in the absence of directing groups, achieving yields of up to ~99%, with long cycle lives and high substrate compatibility. PCN-1004 outperforms all previously reported porphyrin-based homogeneous and heterogeneous catalysts. Control experiments and computations elucidate the pivotal catalytic role of the copper-Pz chains and reveal a free radical pathway for the reaction. This work not only demonstrates the successful implementation of a metal-node-based catalytic site anchoring strategy for the efficient catalysis of challenging organic transformations but also highlights the synergistic effect of a robust framework, 1D open channels, and active sites in enhancing catalytic efficiency within MOFs.

General Trends in the Compression of Glasses and Liquids

The present work relates the isothermal volumes of silicate glasses and melts to the combined ionic volumes of their chemical constituents. The relation is an extension of a relation that has already been established for crystalline oxides, silicates, alumosilicates, and other materials that have O2− as a constituent anion. The relation provides constraints on bond coordination, indicates pressure-induced changes in coordination in melts and glasses and interatomic distances, and quantifies the extent of transitory regions in pressure-induced coordination changes.

Terpyridine-Based Metal-Organic Cage with Enhanced Emission via Coordination-Induced Rigidity.

Realizing the regulation of photophysical properties by precisely controlling the molecular composition and configuration, thereby obtaining high-performance optical materials, remains of great significance. Due to the directionality and reversibility of the coordination bond, coordination-driven self-assembly endows the molecule with customized thermodynamically stable structures and desired properties. In this paper, a luminous metal-organic cage [Zn12L6] (S) was elaborately designed and quantitatively synthesized by self-assembly of tetrapodal TQPP chromophore-containing terpyridine ligand L with Zn2+. Complex S possessed a rigid cage-like structure, which endows a higher fluorescence quantum efficiency both in solution (∼88%) and neat solid (16%) than the corresponding ligand L. Further, using complex S as the photoactive component, two light-emitting diodes (LEDs) were successfully fabricated and the emission of pure white light (CIE coordinates: 0.3341, 0.3300) was achieved. These results afford a method to obtain enhanced luminescence performance via the formation of rigid coordination-driven supramolecular architectures.

Mechanical Properties of Epoxy Networks with Metal Coordination Bonds: Insights from Temperature and Molar Mass Variation.

We investigate the thermal and mechanical properties of poly(ethylene glycol), PEG, networks with either solely covalent epoxy bonds (single networks, SNs) or coexisting epoxy and iron-catecholate bonds (dual networks, DNs). The latter has recently been shown to be a promising material that combines mechanical strength with significant deformability. Here, we address the previously unexplored effects of the temperature and PEG precursor molar mass on the mechanical properties of the networks. We focus on PEG molar masses of 500 g/mol, where crystallization is suppressed, and 1000 g/mol, where some weak crystals are formed. SNs soften with an increasing PEG molar mass. Heating reversibly softens the DN, but it has a minimal effect on SNs. Nonlinear shear deformation of the DN breaks iron-catecholate bonds, and subsequent recovery upon shear cessation occurs to a long-time steady-state modulus whose value is almost triple the original one, likely due to the formation of tris-complexes versus initial sterically or kinetically trapped bis-complexation. The response under elongation indicates that the DN with sacrificial bonds is stiffer and more extensible than the other networks. These results may provide guidelines for designing dual networks with tunable mechanics at the molecular level.

2D mesh-knots metal organic frameworks functionalized with phytic acid for improving flame retardancy

Metal ions and organic compounds were adopted to form a two-dimensional mesh-knots metal organic frameworks (TMMOFs), which could functionalize with Phytic Acid (PA) for fireproof. The results of the functional group test show that two-dimensional mesh-knots metal organic frameworks (TM), TM with -NH2 (TMN) and TMN with PA (TMNP) have been successfully prepared by coordination bond. The samples appeared irregular ellipsoid with size of particles below 100 nm. The values of limiting oxygen index (LOI) test depicted the flame resistance have been enhanced from 22.7 % to 30 % due to the addition of -NH2 and PA. The peak heat release rate (pHRR) and total heat release (THR) value of TM-PA@wood declined noticeably by 55.9 % and 68.6 % compared to pure wood. CO2 emissions intensity of TMNP@wood declined from about 0.40 to 0.12 compared with samples without PA. The CO2 and CO maximum production of TMNP@wood were significantly lower 246% and 64% than TMN@wood, respectively. PA and ZrO2 after combustion could catalyze wood to form carbon residue as condense phase, delay and minimize the peak of CO2 and CO to reduce toxicity. This work provides an effective strategy for synthesis and application of two-dimensional materials in flame retardant field.

Stretchable supramolecular hydrogel with instantaneous self-healing for electromagnetic interference shielding control and sensing

Conductive hydrogels possess instantaneous self-healing and adhesive properties have generated great excitement in the fields of sensing and electromagnetic interference (EMI) shielding. In this study, we ingeniously designed hydrogel-based soft materials with high conductivity by using poly(vinyl alcohol) (PVA), positively charged Ti3C2Tx MXene and thioctic acid (TA) as source materials. Through concentration-induced ring-opening polymerization of TA monomers in an aqueous solution of potassium hydroxide (KOH), supramolecular poly(potassium thioctate) (poly(PT)) was obtained. Then, the multifunctional poly(PT)/PVA/p-MXene hydrogel with exceptional stretchability, substrate-adhesion and self-healing capability was achieved through abundant dynamic bonds, including disulfide bonds, hydrogen bonds, coordination bonds and electrostatic interactions. The hydrophobic main chains within poly(PT) provide robust protection against the oxidative degradation of MXene. This hydrogel shows outstanding strain sensing and extraordinary EMI shielding effectiveness (SE) of 48.56 dB caused by the inner structure, conductivity, and water content. Interestingly, the EMI SE can be regulated by reabsorbing moisture from the air, thereby enabling the reuse of dried hydrogel. Furthermore, the EMI SE can be dynamically modulated through controlled deformations, confirming the potential application for electromagnetic waves (EMWs) sensing. This innovative approach not only simplifies the fabrication of multifunctional materials but also expands the applications of adhesive hydrogels with conductivity.

Controllable Iodoplumbate-Coordination of Hybrid Lead Iodide Perovskites via Additive Engineering for High-Performance Solar Cells.

The crystallization and growth of perovskite crystals are two crucial factors influencing the performance of perovskite solar cells (PSCs). Moreover, iodoplumbate complexes such as PbI2, PbI3-, and PbI42- in perovskite precursor solution dictate both the quality of perovskite crystals and the optoelectrical performance of PSCs. Here, we propose an iodoplumbate-coordination strategy that employs pentafluorophenylsulfonyl chloride (PTFC) as an additive to tailor the crystal quality. This strategy directly affects the thermodynamics and kinetics of perovskite crystal formation by regulating hydrogen bonds or coordination bonds with Pb2+ or I- ions. Subsequently, the synergistic effect of the PTFC and FA+ complex was beneficial for intermediate-to-perovskite phase transition, improving the crystalline quality and reducing the defect density in the perovskite film to suppress nonradiative recombination loss. Consequently, the treated PSCs achieved a power conversion efficiency (PCE) of 24.61%, demonstrating enhanced long-term stability under both light and thermal stress. The developed device retained 92.53% of its initial PCE after 1200 h of continuous illumination and 88.6% of its initial PCE after 600 h of 85 °C thermal stability tests, respectively, both conducted in N2 atmospheres.