Strong Interchain Interactions Research Articles

Association of Thermoresponsive Diblock Copolymer PDEGMA-b-PDIPAEMA in Aqueous Solutions: The Influence of Terminal Groups

Aqueous solutions of a thermoresponsive diblock copolymer poly(di-[ethylene glycol] methyl ether methacrylate)-b-poly(2-[diisopropylamino] ethyl methacrylate) (PDEGMA-b-PDIPAEMA) were studied by static, dynamic and electrophoretic light scattering, small-angle X-ray scattering and differential scanning calorimetry. Thermoresponsive behavior of PDEGMA-b-PDIPAEMA was investigated at two pH values, pH = 2, at which the terminal carboxylic group of the PDEGMA chain and the PDIPAEMA block are protonated, and pH = 7, where the carboxyl terminal group is ionized while the PDIPAEMA block is partially deprotonated and more hydrophobic. Both at pH = 2 and 7, PDEGMA-b-PDIPAEMA copolymer underwent extensive association (the size of the aggregates was between 100 and 300 nm), indicating strong interchain interactions. While the measurements confirmed thermoresponsive behavior of PDEGMA-b-PDIPAEMA at pH = 7, no changes in the association with temperature were observed at pH 2 as the thermoresponsivity of PDEGMA was suppressed by hydrogen bonding between carboxylic groups and PDEGMA segments, as well as due to the increased hydrophilicity of the PDIPAEMA block. Fluorescence measurements with pyrene as a fluorescent probe showed that both at pH = 2 and pH = 7 the associates were able to solubilize hydrophobic substances.

Electrochemiluminescence enhanced by molecular engineering linear π-conjugated polymer: An ingenious ECL emitter for the construction of exosome sensing platform

Linear π-conjugated polymers (LCPs) with π-electron conjugation system have many remarkable optical characteristics such as fluorescence and electrochemiluminescence (ECL). However, the extremely strong interchain interaction and π-π stacking limit the luminescence efficiency. In this work, 1H-1,2,4-triazole-3,5-diamine was chosen as the polymer monomer and reacted with terephthalaldehyde via simple Schiff base condensation to synthesize LCPs. Subsequently, molecular engineering strategy was adopted to construct zirconium-based LCPs (MLCPs), which not only prevented π-π stacking but also ensured that extended π-coupling was maintained in the LCPs, thus effectively promoting charge transport and achieving strong luminescence. Second, the coreactant polyethyleneimine (PEI) was assembled onto the MLCPs (MLCPs@PEI) to further promote the emission of ECL. To further explore the potential of the obtained MLCPs@PEI as emerging ECL emitter, colorectal cancer exosome was chosen as model biomarker, and an innovative ECL ratiometric system based on MLCPs@PEI and luminol was designed to improve the validity and accuracy of the sensors. This research provides a fresh nanoplatform for exosome detection and broadens the application of LCPs in ECL immunoassay.

Mechanochemical synthesis of a red luminescent coordination polymer from a polydentate quinoline ligand with large conjugation

Abstract A red luminescent coordination polymer has been prepared from a polydentate 8-hydroxyquinoline ligand via mechanochemical synthesis. The obtained coordination polymer is micro/nano spherical and can suspend stably in organic solvents after ultrasonic treatment. Due to the large conjugation of the ligand with a strong polar s-triazine core, the coordination polymer shows a largely red-shifted emission relative to the ligand. The photoluminescence peak of the coordination polymer in organic solvent is at 613 nm, while a largely red-shifted photoluminescence peak at 675 nm and a shoulder peak at 770 nm are found in the photoluminescence spectrum of the coordination polymer in solid due to the strong interchain interaction.

Facile strategy for intrinsic low-κ dielectric polymers: molecular design based on space charge conservation.

The growing need for high-power and compact-size microelectronic integrated circuits (ICs) in modern microelectronic industries and 5G communication systems demands low dielectric constant (κ) polymer dielectrics with excellent temperature capability, mechanical property and processability. However, conventional molecular design strategies often face difficulties of a trade-off between optimizing the dielectric performance of polymers and maintaining the aforementioned properties. Herein, we present an innovative and facile strategy that utilizes the space charge distribution characteristics of the target co-monomer to solve this trade-off. Based on this design strategy, a novel polyaryl ether ketone (PAEK) with two different charge distribution units (BAF and SBI) was designed and synthesized. Both the experimental results and computational simulations confirm that these two components serve to weaken the polarization of molecular chains in the electric field, induce higher molecular chain packing density and fewer weaknesses, and synchronously regulate the κ, dielectric loss (tan δ), thermal and mechanical properties and processability by generating a strong inter-chain electrostatic interaction. The resultant copolymer, PAEK-4F6S, exhibits exceptional low κ and tan δ values of 1.98 and 0.0024 at 1 MHz, respectively, and these values remain stable over a broad frequency (1-106 Hz, 8.2-12.4 GHz) and temperature range (30-150 °C). Furthermore, the resultant copolymer demonstrates excellent thermal stability and mechanical properties, with a glass transition temperature (Tg) of 195 °C, 5 wt% decomposition temperature (Td5%) of 498 °C under N2, tensile strength of 63.5 MPa and tensile modulus of 1011.2 MPa, respectively. The synthesis procedure of these resultant copolymers is facile, and they are found to have favorable solution and melt processing properties, making them suitable for processing and scalable production. More importantly, this design strategy is beneficial for lowering the κ and tan δ values, and simultaneously enhancing the comprehensive performances of the objective polymers, which provides a completely novel and facile approach for the design and fabrication of high performance low-κ polymers suitable for the needs of microelectronics and communication fields.

Highly Conductive Inkjet-Printed PEDOT:PSS Film under Cyclic Stretching.

Inkjet-printed conductive polymer PEDOT:PSS films have provided a new developing direction for realizing the stretchable transparent electrodes in optoelectronic devices. However, their conductivity and stretchability are limited as the presence of insulating PSS chains, rigid PEDOT conjugated backbone, and stronger inter-chain interactions in the pristine polymer, respectively. Here, we report a PEDOT:PSS film with preferable electrical and mechanical performances by inkjet-printing the formulated printable ink containing PEDOT:PSS, formamide (FA), d-sorbitol (SOR), sodium dodecyl benzene sulfonate (DBSS), and ethylene glycol (EG). The inkjet-printed uniform PEDOT:PSS film exhibits a high conductivity of 1050 S/cm and sheet resistance of less than 145 Ω/sq on both rigid and flexible substrates. Moreover, the resistance can remain stable after 200 cycles of stretching at 55% strain. The film also presents good stability during repetitive stretching-releasing cycles. The significantly enhanced conductivity of the film lies on the conformational transition of the backbone by secondary doping and post-treatment with FA as well as removing the excess PSS components after phase separation between PEDOT and PSS. Meanwhile, SOR serves as a plasticizer to break the original hydrogen bonds between PSSH chains and provides larger free volume for polymer chain extension, which gives the PEDOT:PSS film the ability to tolerant cyclic tension. This is one of the optimal performances currently reported for inkjet-printed stretchable PEDOT:PSS films. The inkjet-printed PEDOT:PSS film with high conductivity, stretching properties, as well as good biocompatibility exhibits promising prospects as anodes on optoelectronic devices.

Recyclable Polycarbosilane from a Biomass-Derived Bifuran-Based Monomer.

Two of the most fundamental principles for the development of next-generation polymers are production from renewable biomass and well-designed recyclability. Bifuran derivatives represent promising building blocks for functional polymers on account of their high rigidity, strong interchain interactions, and extended π-conjugation. In this study, a polycarbosilane containing a bifuran-based repeat unit was prepared via the hydrosilylation of dihydrosilylbifuran and 1,5-hexadiene. The crystallinity and thermal properties of the bifuran-containing polycarbosilane were superior to those of a corresponding polycarbosilane containing a single-furan-based repeat unit and comparable to those of the benzene-based analogue due to the rigidity and interchain interactions of the poly(bifurancarbosilane) unit. The bifuran moiety in the repeat unit causes a red-shift and strong UV absorption of the polycarbosilane compared to that containing the single-furan-based and benzene-based repeat units. The bifuran moiety also renders the resulting polycarbosilane strongly fluorescent, while the polycarbosilanes containing the benzene-based and single-furan-ring-based repeat units did not emit fluorescence. These desirable photoproperties result from the extension of the σ-π conjugation in the repeat unit. Furthermore, the chemical recyclability is a unique and attractive property of the bifuran-based polycarbosilane; upon treatment with trifluoroacetic acid, bifuran can be regenerated as the monomer, while trifluoroacetate silane can be up-cycled to the corresponding polysiloxane. Thus, the bifuran motif endows polycarbosilane with improved thermal, optical, and recycling properties.

Porous coordination polymer synthesized from a polydentate 8-hydroxyquinoline ligand via interface reaction

A polydentate 8-hydroxyquinoline ligand with a triazine core has been synthesized via aryl nitrile trimerization, which chelates Zn2+ ions at ice surface to form porous coordination polymer via interface reaction. The porous coordination polymer in organic solvent shows a photoluminescence (PL) spectrum with a peak at 610 nm, while a red-shifted PL peak at 675 nm and a new PL shoulder peak at 770 nm appear in the PL spectrum of the porous coordination polymer film. The 770 nm emssion is inferred from the interchain excited state due to the strong interchain interaction caused by the polar triazine core.

Halogen-Free Donor Polymers Based on Dicyanobenzotriazole with Low Energy Loss and High Efficiency in Organic Solar Cells.

Halogenation of organic semiconductors is an efficient strategy for improving the performance of organic solar cells (OSCs), while the introduction of halogens usually involves complex synthetic process and serious environment pollution problems. Herein, three halogen-free ternary copolymer donors (PCNx, x= 3, 4, 5) based on electron-withdrawing dicyanobenzotriazole are reported. When blended with the Y6, PCN3 with strong interchain interactions results in appropriate crystallinity and thermodynamic miscibility of the blend film. Grazing-incidence wide-angle X-ray scattering measurements indicate that PCN3 has more ordered arrangement and stronger π-π stacking than previous PCN2. Fourier-transform photocurrent spectroscopy and external quantum efficiency of electroluminescence measurements show that PCN3-based OSCs have lower energy loss than PCN2, which leads to their higher open-circuit voltage (0.873V). The device based on PCN3 reaches power conversion efficiency (PCE) of 15.33% in binary OSCs, one of the highest values for OSCs with halogen-free donor polymers. The PCE of 17.80% and 18.10% are obtained in PM6:PCN3:Y6 and PM6:PCN3:BTP-eC9 ternary devices, much higher than those of PM6:Y6 (16.31%) and PM6:BTP-eC9 (17.33%) devices. Additionally, this ternary OSCs exhibit superior stability compared to binary host system. This work gives a promising path for halogen-free donor polymers to achieve low energy loss and high PCE.

Raspberry-like Aggregate Formation of π-Stacked Block Copolymer of Dibenzofulvene and Methyl Methacrylate Synthesized by Atom-transfer Radical Polymerization

Block copolymerization of dibenzofulvene (DBF) forming a sequence having π-stacked conformation and methyl methacrylate (MMA) forming a flexible sequence was conducted by atom-transfer radical polymerization (ATRP) where MMA was polymerized first and DBF was then blocked. The block copolymer contained a fraction with number-averaged molar mass of 873400 (vs. polystyrene) which was found to be raspberry-like aggregates with sizes of hundreds of nanometers composed of smaller spherical particles with sizes of a few to low tens of nanometers. The aggregates are considered to have a core-shell structure where strong inter-chain interaction between poly(DBF) segments form the core and flexible poly(MMA) segments are the shell, and the formation appeared to be thermally driven. The aggregates having a rigid structure stabilized the π-stacked conformation of poly(DBF) segments both in the ground state and in excited states as found by NMR and fluorescence spectra, respectively, and restricted molecular motion of both the poly(DBF) segments and poly(MMA) segments.

Intrachain and Interchain Excited-State Dynamics of Temperature-Dependent Aggregation Copolymer in Solution.

Poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene)-co-(1,3-di(5-thiophene-2-yl)-5,7-bis (2-ethylhexyl)benzo[1,2-c:4,5-c']dithiophene-4,8-dione)] (PBDB-T) is a donor-acceptor copolymer widely used as a donor material in high-efficiency organic solar cells. In this work, we studied the temperature-dependent aggregation properties of PBDB-T in solution. Through the characterization of UV-vis absorption and the photoluminescence spectrum, we found that PBDB-T formed strong interchain interactions that facilitate aggregation at room temperature. In contrast, warmer temperatures cause PBDB-T to coil and increase intrachain interactions, thus reducing aggregation. We further use transient absorption spectroscopy to explore the effect of temperature-dependent aggregation behavior on excited-state dynamics. The results show that the intrachain interaction is beneficial to increase the production of polaron pairs, and the interchain interaction is beneficial to accelerate the production of free polarons. Finally, we investigated the corresponding films and demonstrated that regulating the solution aggregation is an effective way to control the crystallinity, and morphology of the corresponding films.

Achieving 16% Efficiency for Polythiophene Organic Solar Cells with a Cyano‐Substituted Polythiophene

AbstractPolythiophenes (PTs) are promising electron donors in organic solar cells (OSCs) due to their simple structures and excellent synthetic scalability. However, the device performance of PT‐based OSCs is rather poor due mainly to large photon energy losses and an unfavorable active layer morphology. Herein, the authors report a new PT, which is abbreviated as P5TCN‐2F and features cyano‐group substituents for high‐efficiency OSCs. The cyano‐group endows P5TCN‐2F with a deep‐lying highest occupied molecular orbital energy level, which thereby contributed to high open‐circuit voltage in OSCs as a result of reduced non‐radiative recombination energy loss. Moreover, the cyano‐group leads to strong interchain interaction, improved polymer crystallinity, and appropriate miscibility with the prevailing non‐fullerene acceptors. Consequently, P5TCN‐2F offers over 15% power conversion efficiency when blended with various Y‐series non‐fullerene acceptors (Y6, Y6‐BO, eC9, and L8‐BO). Particularly, a champion efficiency of 16.1% is obtained by the P5TCN‐2F:Y6 blend, which is largely higher than that of any previous PT‐based OSCs. Moreover, the average figure of merit of the active layer based on P5TCN‐2F is much superior to that of benzodithiophene‐based polymers. These results suggest the renaissance of PT‐based OSCs and have opened an avenue to access high‐performance materials for the large‐scale production of OSC modules.

Polythiophenes for organic solar cells with efficiency surpassing 17%

<h2>Summary</h2> Polythiophenes (PTs) are promising electron donors for organic solar cells (OSCs) due to their low production cost. However, the device performance of PTs in OSCs is rather poor due to unmatched energy levels and unfavorable active layer morphology. Herein, we report a set of new PTs (P5TCN-Fx) with cyano-group substitutions and varied fluorination degrees to achieve high-efficiency OSCs. The incorporation of the cyano-group endows the new PTs with deep-lying energy levels, and backbone fluorination leads to strong interchain interaction, improved polymer crystallinity, and appropriate thermodynamic miscibility with the prevailing acceptor Y6 for the new PTs. As a result, multiple PTs have offered over 16% efficiency in binary OSCs. Moreover, a prominent PCE of 17.2% has been obtained by P5TCN-F25 via ternary blend design, which is the new efficiency record and represents a big breakthrough for PT-based OSCs. This work opens a promising avenue to achieve high-performance OSCs from low-cost materials.

Regulation of High Miscibility for Efficient Charge-Transport in n-Doped Conjugated Polymers.

Strong interchain interactions of conjugated polymers usually result in poor miscibility with molecular dopants, limiting the doping efficiency because of uncontrolled phase separation. We have developed a strategy to achieve efficient charge-transport and high doping miscibility in n-doped conjugated polymers. We solve the miscibility issue through disorder side-chains containing dopants better. Systemic structural characterization reveals a farther side-chain branching point will lead to higher disorders, which provides appropriate sites to accommodate extrinsic molecular dopants without harming original chain packings and charge-transport channels. Therefore, better sustainability of solid-state microstructure is obtained, yielding a stable conductivity even when overloading massive dopants. This work highlights the importance of realizing high host-dopant miscibility in molecular doping of conjugated polymers.

Reinforcing the poly(silylene arylacetylene)s via strong π-π stacking interactions

Silicon-containing arylacetylene resins show a trade-off between mechanical property and heat resistance as usual. A strategy is proposed by utilizing the interchain π-π stacking interactions to obtain a resin with both high mechanical property and heat resistance. In this work, silicon-containing arylacetylene resins separately with 2,5-diphenyl- [1,3,4]-oxadiazole unit as π-π stacking precursors (PODSA-MM, PODSA-MP) and the phenylene unit (PESA-MM, PESA-MP) in the main chains were synthesized by Grignard reactions. The stronger interchain π-π stacking interactions in the PODSA resins compared with PESA resins were confirmed by UV–Vis, XRD, SAXS analyses, regardless of whether or not the resins are cured. The PODSA resins with more regular structures show higher melting temperature and melt viscosity. The stable physical and chemical crosslinking dual-networks caused by both strong interchain interactions and thermal crosslinking reactions are formed in cured PODSA resins. The cured PODSA resins exhibit higher secondary relaxation temperature (Tβ), mechanical properties and thermal conductivity than cured PESA resins. The enhancement of properties of the cured PODSA resins are mainly attributed to stronger intermolecular π-π stacking interactions derived from 2,5-diphenyl- [1,3,4]-oxadiazole unit.

Structural Analysis of Melt-Spun Polymer-Optical Poly(Methyl Methacrylate) Fibres by Small-Angle X-ray Scattering and Monte-Carlo Simulation.

The structural properties, mainly the spatial variation of density and chain interaction, of melt-spun polymer optical fibres (POFs) are investigated by small-angle X-ray scattering (SAXS) and compared to Monte-Carlo polymer simulations. The amorphous PMMA POFs had been subjected to a rapid cooling in a water quench right after extrusion in order to obtain a radial refractive-index profile. Four fibre samples with different processing parameters are investigated and the SAXS data analysed via Guinier approach. Distance-distribution functions from the respective equatorial and meridional SAXS data are computed to extract the fibres’ nanostructures in the equatorial plane and along the fibre axis, respectively. Temperature profiles of the cooling process are simulated for different locations within the fibre and taken as input for Monte-Carlo simulations of the polymer structure. The simulation results agree with the SAXS measurements in terms of the cooling profile’s strong influence on the structural properties of the fibre: slower cooling in the centre of the fibre leads to stronger interchain interaction, but also results in a higher density and more homogenous materials with less optical scattering.

Electric-field-induced modulation of thermal conductivity in poly(vinylidene fluoride)

Phonon engineering focuses on heat transport modulation in atomic-scale. Different from reported methods, it is shown that electric field can also modulate heat transport in ferroelectric polymers, poly(vinylidene fluoride), by both simulation and measurement. Interestingly, the thermal conductivities of poly(vinylidene fluoride) array can be enhanced by a factor of 3.25 along the polarization direction by simulation. The thermal conductivities of semi-crystalline poly(vinylidene fluoride) film can be also enhanced by a factor of 1.5 which is shown by both simulation and measurement. The mechanism is analyzed by morphology and phonon properties. It is found that the enhancement arises from the higher inter-chain lattice order, stronger inter-chain interaction, higher phonon group velocity and suppressed phonon scattering. This study offers a new modulation strategy with quick response and without fillers. Poled by electric field, thermal conductivity of poly(vinylidene fluoride) (PVDF) can be increased, which is proved by both simulations and experiments. The study offers a brand new strategy to modulate thermal conductivity. • A new strategy to modulate thermal conductivity of polymer with electric field is proposed and proved. • Thermal conductivities in poly(vinylidene fluoride) can be modulated without sacrificing other mechanical properties. • Modulation with electric field is in situ, flexible control, quick response and low energy consumption. • A detailed analysis on the mechanism of thermal conductivity enhancement is presented.

Diketopyrrolopyrrole–thiophene–methoxythiophene based random copolymers for organic field effect transistor applications

Abstract Methoxy-substituted thiophene units were incorporated into a diketopyrrolopyrrole and quaterthiophene based copolymer to produce random copolymers. Inclusion of the methoxy group narrowed the optical energy gap of the resulting copolymers owing to the enhanced planar backbone that results in more effective conjugation. At a low loading ratio of 25mol% random copolymer exhibited a hole mobility of ~0.3 cm2 V−1 s−1 comparable to that of the diketopyrrolopyrrole and quaterthiophene based original polymer. Although increasing the methoxy-substituted thiophene ratio in the polymers resulted in decreased molecular weights, it was concluded that incorporation of the methoxy-substituted thiophenes enhanced the hole mobility from 0.02 cm2 V−1 s−1 for 50mol% loading to 0.07 cm2 V−1 s−1 for 100mol% loading. The enhancement was attributed to the formation of pre-aggregates with stronger interchain interactions with increasing backbone coplanarity, resulting in edge-on dominant and bimodal edge-on/face-on molecular packing orientations. The addition of tetramethylammonium iodide as an ionic additive proved not to be an effective method for improving the performance of polymers containing the methoxy-substituted thiophenes, whereas the original polymer displayed a noticeable improvement of the charge transport properties.

Boosting up printability of biomacromolecule based bio-ink by modulation of hydrogen bonding pairs

This study describes low dose UV curable and bioprintable new bioink made of hydrogen bond donor-acceptor adaptor molecule 2-isocyanatoethyl methacrylate (NCO)modified gelatin (NCO-Gel). Our theoretical calculations demonstrate that insertion of 2-isocyanatoethyl methacrylate doubles the interaction energy (500 meV) between gelatin chains providing significant contribution in interchain condensation and self-organization as compared to methacrylic anhydride modified gelatin (GelMA). The NCO-Gel exhibits peak around 1720 cm−1 referring to bidentate hydrogen bonding between H-NCO and its counterpart OCNH. These strong interchain interactions drive chains to be packed and thereby facilitating UV crosslinking. The NCO-Gel is exhibiting a rapid, 10 s gelation process by the exposure of laser (3 W, 365 nm). The dynamic light scattering characterization also reveals that NCO-Gel has faster sol to gel transition as compared to GelMA depending on the UV curing time. The NCO-Gel was found to be more firm and mechanically strong that provides advantages in molding as well as bioprinting processes. Bioprinted NCO-Gel has shown sharp borders and stable 3D geometry as compared to GelMA ink under 10 s UV curing time. The cell viability tests confirm that NCO-Gel facilitates cell proliferation and supports cell viability. We foresee that NCO-Gel bioink formulation provides a promising opportunity when low dose UV curing and rapid printing are required.

Impact of amine additives on the mechanical properties of hydrogen bonding π-conjugated polymers

Reversibly interacting π-conjugated polymers of lower modulus are needed to generate intrinsically healable materials for bioelectronics applications. However, strong interchain interactions between π-conjugated polymers increases modulus and reduces flexibility of networks as well as self-healing capability. Herein, to understand the impact of amine additives on the thin film moduli of hydrogen bonding π-conjugated polymer, poly[3-(6-carboxyhexyl)thiophene-2,5-diyl] (PTCOOH) was complexed with a lean (Di-2oMe) and bulky (Di-2onBu) 1,6-difunctional secondary amines. The amines interact with the PTCOOH via weak ionic interactions and/or hydrogen bonding interactions. Amine complexed PTCOOH polymer samples and PTCOOH are characterized using DSC and PXRD to correlate the assembly structure with the observed modulus. The amines acted as plasticizers and reduced the modulus of PTCOOH. Moreover, the polymer modulus decreased with increasing amine group size, indicating the importance of the amine group size. Also, the difunctional amines acted as a better plasticizer than the monofunctional amines. PXRD analysis indicates that the interchain hydrogen bonding interactions between the polymer chains play a key role in determining the moduli of thin films.

Full Poly(ethylene glycol) Hydrogels with High Ductility and Self-Recoverability.

Energy dissipation is a common mechanism to improve the ductility of polymeric hydrogels. However, for poly(ethylene glycol) (PEG) hydrogels, it is not easy to dissipate energy, as polymer chains are dispersed in water without strong interchain interactions or decent entanglement. The brittleness limits the real applications of PEG hydrogels, although they are promising candidates in biomedical fields, as PEG has been approved by the U.S. Food and Drug Administration. Herein, we chemically introduced a center for energy dissipation in the PEG hydrogel system. Amphiphilic segmented PEG derivatives were designed through the melt polycondensation of triethylene glycol (PEG150) and high molecular weight PEG in the presence of succinic acid and mercaptosuccinic acid as dicarboxylic acids. Full PEG hydrogels with elastic nanospheres as giant cross-linkers were facilely prepared by the self-assembly of esterified PEG150 segments and the oxidation of mercapto groups. The resultant full PEG hydrogels can dissipate energy by the deformation of elastic nanospheres with outstanding ductility and self-recoverability while maintaining the excellent biocompatibility owing to their full PEG components. This work provides an original strategy to fabricate full PEG hydrogels with high ductility and self-recoverability, potentially applicable in biomedical fields.