Rich Hydrogen Bonds Research Articles

Synthesis and crystal structure of a novel metal cyanide halide complex (NH4)6Fe(CN)6Cl2·0.4H2O

Hexacyanidometallates possess unique physical properties, which has been extensively studied. However, there are still a number of its derivatives that may be considered which remains unknown, such as metal cyanide halide hexacyanidometallates, especially those of transition-metal elements, but preparing such complex is hampered by the preference of the formation of compounds without halogens. Here, we report synthesis of a novel transition metal cyanide halide hexacyanidometallates derivate (NH4)6Fe(CN)6Cl2·0.4H2O through reactant ratio control. The crystal structure was studied via single-crystal X-ray diffraction, supported by elemental analysis and IR spectra. The crystal structure of (NH4)6Fe(CN)6Cl2·0.4H2O crystallizes in space group R3¯ with rhombohedral stacking behavior. Moreover, the crystal structure of (NH4)6Fe(CN)6Cl2·0.4H2O features rich hydrogen bonds, contributing to the crystal stability.

“Three birds with one stone” strategy for building easily reprocessable cellulosic thermosetting resins

Cellulose is the most abundant natural polypolysaccharide and is an ideal raw material to replace petroleum-based plastics. However, natural cellulose is difficult to be thermo-processed like conventional plastics because of the rich and strong hydrogen bonds interactions. In this study, a series of dialdehyde derivatives of cellulose (DACs) were prepared by periodate oxidation of cellulose, and cellulose covalent adaptive networks based on acetal dynamic covalent bonds (ACCs) were prepared using dipentaerythritol as a crosslinker for DAC. This strategy can introduce acetal bonds, weaken hydrogen bonds, and reduce rigidity to kill three birds with one stone. The excellent reprocessing performance of ACCs is attributed to the reconstruction of the cellulose hydrogen bond network by acetal bonds, and the reversible exchange reaction of the acetal bonds at high temperatures endows the cellulose chains with mobility, allowing ACCs to be remodeled by hot pressing at 90°C for 15 min. The excellent stability and reprocessability of ACCs hold the promise of replacing current non-renewable petroleum-based plastics and provide inspiration for the development of other types of biomass plastics.

Multi‐stimuli‐responsive chromic switching self‐assembled with polyoxometalate and copper‐viologen frameworks

AbstractChromic materials with multi‐stimuli responses have received tremendous attention from industry and academia for their potential applications in smart windows, data storage, military camouflage, molecular switches, modulators, etc. To develop multi‐stimuli‐responsive color‐changing materials with high sensitivity and high stability, a polyoxometalate‐based copper‐viologen framework, formulated as Cu2(H2O)2(L)2[PW12O40][OH−]·2H2O (HNU‐97, H2L2+ = 1,1′‐(1,4‐phenylenebis(methylene))bis(4‐carboxypyridinium)), was prepared by a mild one‐step self‐assembly strategy. Structural analysis shows that HNU‐97 presents a supramolecular structure formed by a one‐dimensional copper‐viologen framework and polyoxometalates through rich hydrogen bonds, anion‐π interactions, etc. Discoloration studies show that HNU‐97 exhibits reversible and rapid response characteristics to various external stimuli, such as 10 s to UV radiation, 5 min to heating, and 5 min to ammonium/amine vapors. This mechanism reveals that different external excitation sources lead to different preferential transfer directions of electrons, resulting in different discoloration phenomena. To construct stimuli‐chromic materials with good mechanical properties, we successfully introduced HNU‐97 into the poly(vinyl alcohol) (PVA)/glycerol (Gly) hydrogel to obtain a composite HNU‐97@PVA/Gly. Remarkably, HNU‐97@PVA/Gly combines the merits of each component and can achieve significant response discoloration behavior under both UV irradiation and ammonia atmosphere. This work will provide an idea for the construction of multiple stimuli‐responsive materials.

Environmental Stability Stretchable Organic Hydrogel Humidity Sensor for Respiratory Monitoring with Ultrahigh Sensitivity

AbstractReal‐time monitoring of respiration plays a very important role in human health assessment, especially in monitoring and analyzing respiration during exercise and sleep. However, traditional humidity sensors still have problems in flexibility, sensitivity, and durability, so there is an urgent need to develop humidity sensors with high sensitivity, stretchability, and environmental resistance as respiratory monitoring applications. Here, based on the double network hydrogel structure of polyvinyl alcohol and polyacrylamide, a highly sensitive, highly stretchable, and environmentally stable organic hydrogel humidity sensor has been manufactured by using the synergistic effect of lithium chloride and MXene. The hydrogel humidity sensor shows rapid response in the humidity range of 40–85% RH, and has a high sensitivity of −103.4%/% RH. In addition, it exhibits more than 3000% mechanical strain and excellent environmental resistance, which is attributed to the chemical cross‐linking in the hydrogel network and the synergistic effect of multiple hydroxyl groups in glycerol forming rich hydrogen bonds with water and polymer chains. The hydrogel humidity sensor is used for real‐time monitoring of breathing and sleep processes. This work provides a new strategy for preparing high‐performance, extensibility, and environmental stability hydrogel‐based sensors for respiratory monitoring.

A self-healing sustainable halloysite nanocomposite polyurethane coating with ultrastrong mechanical properties based on reversible intermolecular interactions

Endowing sustainable polyurethane (PU) materials with ultrastrong mechanical properties and highly efficient self-healing performancesimultaneously is extremely challenging and of great significance to dramatically extend the service life of metal materials. In this work, 4,4′-dithiodianiline (DTDA) and bio-based 2,5-Tetrahydrofurandimethanol (THFDM) were used as chain extenders to introduce hierarchical hydrogen bonds and aromatic disulfide bonds into the PU matrix, after which rich interfacial hydrogen bonds were obtained by incorporating environment-friendly polydopamine-modified halloysite nanotube (PDA@HNT) into the PU matrix. The developing PU nanocomposite exhibits record toughness (774.4 MJ m−3), outstanding tensile strength (68.3 MPa), and exceptional elongation at break (2882.7 %), as well as distinguished self-healing performance (85.4 % at 35 °C for 24 h; 95.9 % at 80 °C for 15 min). Thanks to the shielding effect of PDA@HNT fillers, the PU nanocomposite also possesses good corrosion resistance proved by its high impedance value at 0.01 Hz of 2.23 × 108 Ω cm2 after immersing in 3.5 wt% NaCl solution for 30 days. This work provides constructive guidance to create an ultra-robust self-healing sustainable PU nanocomposite with long-term corrosion resistance.

Controllable Modulation of Third‐Order NLO Properties by Polymer‐Modified MOFs Core@Shell Nanoarchitecture

AbstractThe delocalization and rearrangement of π electron clouds in space is the crucial source of regulating nonlinear optical (NLO) performance. Herein, a core‐shell metal organic framework (MOF)‐heterojunction is constructed to achieve the effect of tuning NLO properties by promoting charge transfer through multiple interactions between heterogeneous interfaces. [Cd(L)(4,4′‐bpy)(H2O)]n (Cd‐MOF) is selected to coat on polyaniline (PANI) surface to form PANI@Cd‐MOF. The constructed heterojunction displays an enhanced reverse saturation absorption (RSA) signal compared with Cd‐MOF, and it should be noted that the third‐order NLO refractive behavior changes from the self‐defocusing of Cd‐MOF to the self‐focusing of PANI@Cd‐MOF. It is proposed that high‐speed electronic communication bridges established via the rich hydrogen bond network (O… H‐N) and π–π interactions between heterogeneous interfaces can effectively modify the π electron cloud density that finally regulates the NLO properties. This work is believed to provide new avenues and insights for the design of third‐order NLO materials.

Research on the hot densification mechanism of biomass wastes based on molecular dynamics simulation and components adjustment method

The hot densification process can be used to prepare the biofuel pellets and diversified densification materials with suitable mechanical strength to overcome the natural defects of low energy density and loose structure of biomass wastes and achieve the high value utilization of the renewable resources. In this study, the two typical biomass wastes, cotton stalk (CS) and Chinese fir wood sawdust (WS) are used for the hot densification investigation (85 °C), and the microscopic evolution behavior of the biomass components during the hot densification process is explored through the combination of the component adjustment method and molecular dynamics simulation. The results show that cellulose is the key component to the mechanical strength of biomass pellet, which plays the crucial role of skeleton support in the densification process, and the strength of pellet is positively correlated with the increasing addition ratio of cellulose. Furthermore, crystalline cellulose exhibits the strongest bonding properties in the hot densification process due to the formation of rich hydrogen bonds and the increasing intermolecular attraction force. Lignin has the poorest capability for hydrogen bond formation, and its addition increases the van der Waals repulsive forces, resulting in the poorest densification performance. Hemicellulose shows the better adhesion capability than lignin due to its glassy transition (83.34 °C) and the suitable addition can greatly improve the mechanical property of the pellet, up to 14.26 MPa. There exists the strongest synergistic effect between cellulose and hemicellulose, which is beneficial to the bonding performance between particles to different extent. Hot densification process can promote the formation of hydrogen bond connections between molecules/atoms and the increase of the van der Waals repulsive force in the further compression. The densification performance of biomass is the combined effect of the physical forces, including electrostatic force and van der Waals force.

Comprehensive Understandings of Hydrogen Bond Chemistry in Aqueous Batteries.

Aqueous batteries are emerging as highly promising contenders for large-scale grid energy storage because of uncomplicated assembly, exceptional safety, and cost-effectiveness. The unique aqueous electrolyte with a rich hydrogen bond (HB) environment inevitably has a significant impact on the electrode materials and electrochemical processes. While numerous reviews have focused on the materials design and assembly of aqueous batteries, the utilization of HB chemistry is overlooked. Herein, instead of merely compiling recent advancements, this review presents a comprehensive summary and analysis of the profound implication exerted by HB on all components of the aqueous batteries. Intricate links between the novel HB chemistry and various aqueous batteries are ingeniously constructed within the critical aspects, such as self-discharge, structural stability of electrode materials, pulverization, solvation structures, charge carrier diffusion, corrosion reactions, pH sensitivity, water splitting, polysulfides shuttle, and H2 S evolution. By adopting a vantage point that encompasses material design, binder and separator functionalization, electrolyte regulation, and HB optimization, a critical examination of the key factors that impede electrochemical performance in diverse aqueous batteries is conducted. Finally, insights are rendered properly based on HB chemistry, with the aim of propelling the advancement of state-of-the-art aqueous batteries.

A Zn(II) metal−organic framework with organic fluorescent ligands and hydrogen-bonding network for effectively sensing Al3+ and Ga3+ ions, and proton conduction

Energy shortage and environmental pollution become increasingly serious. Thus, there is urgent need to develop new functional materials to deal with these problems. Metal−organic frameworks (MOFs) are ideal candidates for fluorescence sensing pollutants and proton conduction. A benzothiadiazole-based three-dimensional (3D) Zn(II) MOF with the formula of {[(CH3)2NH2][Zn3(bbip)(BTDI)1.5(OH)]·DMF·MeOH·3H2O}n (JXUST-13, bbip = 2,6-bis(benzimidazol-1-yl)pyridine and H4BTDI = 5,5′-(benzo[c][1,2,5]thiadiazole-4,7-diyl)diisophthalic acid) with fluorescent ligands and rich hydrogen bond framework was used as a cation fluorescence sensor and proton conduction material. The fluorescence experiment revealed that JXUST-13 could detect Al3+ and Ga3+ ions by fluorescence blue shift and slight fluorescence enhancement. And it showed high sensitivity, good selectivity, anti-interference performance and cyclicity. The detection limits of JXUST-13 toward Al3+ and Ga3+ ions were 4.0 μM and 0.67 μM, respectively. Importantly, it could be rapidly detected by fluorescent test strips and naked eyes. The sensing mechanism may be due to the presence of electron transfer and the formation of exciplex. Proton conduction result indicated that the maximum conductivity value of JXUST-13 was 1.97 × 10−5 S·cm−1 at 80 °C and 98% RH. And the conductivity increased with humidity and temperature. The activation energy (Ea) value of JXUST-13 was 0.47 eV, which revealed the Vehicle mechanism. Therefore, JXUST-13 could be considered as a rare difunctional materials of blue-shifted fluorescence sensor for Al3+, Ga3+ ions and proton conduction.

Highly Flexible and Self-Healing Supercapacitor Enabled by Physically Crosslinking Polymer Hydrogel Electrolyte.

Preparation of flexible supercapacitors with excellent mechanical properties and self-healing properties is of great significance but still remains a challenge. A self-healable conductive hydrogel based on poly N-hydroxyethyl acrylamide (PHEAA) is fabricated as electrolyte for supercapacitors. The design of the physically cross-linked dual network, and rich hydrogen bonds endow the hydrogel with robust mechanical properties and strong self-healing ability. The hydrogel exhibited an excellent stretchability (723 %) and a high ionic conductivity (21.8 mS/cm). Specially, by in situ growth of electrode film, a non-laminated supercapacitor is obtained with flexibility and self-healing ability. Due to the non-laminated structure, the supercapacitor can work stably under bending and punching. The supercapacitor possessed an areal capacitance of 253.1 mF/cm2 and the capacitance retention was 80 % after five cutting-healing cycles. The pseudo-capacitance contribution of the supercapacitor after self-healing was discussed. It is noteworthy that the supercapacitor maintains the ability to power a clock after self-healing.

Amidoxime Modified UiO-66@PIM-1 Mixed-Matrix Membranes to Enhance CO2 Separation and Anti-Aging Performance.

Mixed matrix membranes (MMMs) generally have some fatal defects, such as poor compatibility between the two phases leading to non-selective pores. In this work, PIM-1 was chosen as the polymer matrix, and UiO-66 modified with amidoxime (UiO-66-AO) was used as the filler to prepare the MMMs. In the MMMs, the amino and hydroxyl groups on UO-66-AO form a rich hydrogen bond network with the N and O atoms in the polymer PIM-1 chain to improve the compatibility between the polymer matrix and the filler. In addition, the selective adsorption of CO2 by the amidoxime group can promote the transport of CO2 in the membrane, which enhances the gas selectivity. The CO2 permeability and CO2/N2 selectivity of UiO-66-AO@PIM-1 MMMs are increased by 35.2% and 45.2% compared to pure PIM-1 membranes, reaching 7535.5 Barrer and 26.9, surpassing the Robeson Upper Bound (2008) and close to the 2019 Upper Bound. After 38 days of the aging experiment, the CO2 permeability is approximately 74% of the original. The results show that the addition of UiO-66-AO has an obvious effect on improving the aging properties of the membrane. The UiO-66-AO@PIM-1 MMMs have a bright prospect for CO2 separation in the future.

Stretchable conductive hydrogel with super resistance-strain stability and ultrahigh durability enabled by specificity crosslinking strategy for high-performance flexible electronics

Stretchable ionic conductive hydrogels (SICHs) are regarded as one of the indispensable components for flexible electronics desirable to provide stable signal transmission and functional reproducibility. However, the state-of-the-art SICHs demonstrate a narrow resistance-stability range and poor cyclical fatigue reliability due to ion migration limitations and the absence of the molecular design regime. Herein, we present a novel synthetic strategy that utilizes the dynamic Zn-carboxyl physical bonding, adjacent to B-hydroxyl chemical bonding, to realize the “specificity” cross-linking in pectin polymeric networks. This approach significantly extends the resistance-stability range of SICHs, while also providing remarkable longevity. Via “specificity” crosslinking design, the Zn-carboxyl physical bonding, bearing thermodynamically stable and dynamic exchange character, can break the resistance-strain dependence of ionic conductive hydrogel, offering an unprecedented resistance-stability under largely applied strain (300%). Moreover, the B-hydroxyl chemical bonding effectively overcomes the conductivity and mechanical strength trade-off dilemma due to its strong but dynamic feature, realizing the high durability of SICHs. In addition, the extraordinary tolerate harsh environment capacity was achieved by introducing glycerin to form rich hydrogen bonds in the SICHs network, which is crucial for the avoidance of congelation at subzero temperatures and dehydration resulting from the circuit heat. As a stretchable conductive component of deformable electronic devices, the SICH demonstrates extraordinary long life and stable operation. These observations reveal fresh stretchable conductive materials.

Flexible strain sensor with self-healing function for human motion monitoring

Flexible strain sensors with highly similar effects to human skin have been given great attention due to their potential application in personal health monitoring, human–computer interaction systems and artificial electronic skin fields. In particular, the self-healing properties of the sensors are important for their long-term and repeated use during the actual operation. Herein, a flexible strain sensor with complete self-healing function is proposed by combining self-healable PDMS film with rich hydrogen bonds and conductive ink based on recoverable liquid metal. By adjusting the contents of different components of self-healing PDMS film and the relative mass fraction of the liquid metal ink in the strain sensor, the tensile stress and resistance of flexible sensor can be changed to match different usage scenarios. The sensor can achieve a maximum tensile stress of 0.83 MPa and an elongation at break of 843%. After self-healing for 24 h at room temperature, its tensile stress can revert to 82% of the original value, while the electrical connection can instantaneously recover to initial situation after fracture surface contacts. This hints its potential advantage as wearable sensors for motion monitoring of the human body and developable applications in medical monitoring, recyclable electronics and artificial skin.

Inorganic hydrogen-bonded SnO(OH)2as molecular springs boosted the piezocatalytic degradation of contaminants

SnO(OH)2is the first highly active hydrogen-bonded inorganic piezocatalyst due to its rich hydrogen bonds and high valence band.

High-value copolyamide 6 materials with colorless transparent and low water absorption upgraded from upcycled and biomass comonomers

Polyamide 6 (PA6) is a semicrystalline polymer with excellent wide application for filament and packing materials. However, the use in filament and packing materials of PA6 with high crystallinity and rich hydrogen bonds is limited because of its low optical properties and poor anti-water absorption. In this work, a series of partially sustainable PA6 copolymers with high value were synthesized by melt polycondensation from fatty dimer acid (FDA) and upcycled chemical bis(6-aminohexyl) terephthalamide (BAHT). The chemical structure of partially sustainable PA6 copolymers was characterized by 1 H NMR, FT IR, relative viscosity, and amine value. The mechanical properties, optical properties, and anti-water absorption of high-value PA6 copolymers depended on the BAHT salt loading and the chain length of aliphatic dicarboxylic acids. The tensile strength of PA6 copolymers was decreased, but the tensile toughness, optical transmittance, and anti-water absorption of that were significantly improved. Overall, this easy method opens up new avenues for devising excellent optical transmittance and low water absorption of polyamide materials, whereas providing the new strategy for carbon-neutral through rPET upcycling and biomass use, and these PA6 copolymers have the potential and economy to be widely applied. • Combining both upcycling and biomass segments in polycaprolactam copolymers (CoPAs). • Bis(6-aminohexyl) terephthalamide (BAHT) upcycled from rPET bottle to promote spherulite shrinkage of CoPAs. • Fatty dimer acid influenced the optical behavior of the polyamide (transparency level > 80% and haze level < 10%). • Fatty dimer acid increased the anti-water absorption of CoPAs. • CoPAs prepared transparent monofilaments and films by twin-screw extrusion and hot-pressing.

Casein micelles embedded composite organohydrogel as potential wound dressing

Excellent mechanical and tissue adhesive properties, long-lasting environmental suitability and reliable biocompatibility are essential factors for the hydrogels to be applied as wound dressing in the clinical fields. Based on the self-assembly micelle structures, a new type of casein micelles (CEs)/polyvinyl alcohol (PVA) GW (glycerol-water) organohydrogel was designed and synthesized by a simple one-pot method. Through a unique “load sharing” effect, the CEs which own suitable adhesion abilities and drug loading capacities simultaneously were embedded into the PVA networks by rich hydrogen bonds, so that to obtain the composite organ hydrogel with not only excellent adhesive abilities, but also enhanced mechanical properties. Benefited from the unique GW binary solvent system, the organohydrogel showed long-lasting moisture lock-in capacity and extreme temperature tolerance (in the range of ‐−20 °C ~ 60 °C). Particularly, after loading the model antibacterial drugs (allicin) within the CEs, the as-developed CEs/PVA GW gel exhibited a prominent long-lasting (>100 h) antibacterial properties (>90%). Furthermore, the organohydrogel was confirmed with prominent biocompatibility to support fibroblast cell proliferation and migration. This work proposed a new strategy to build CEs-based gel system, which have a great potential application in terms of prevent bacterial infection, accelerate tissue proliferation and wound healing.

Study of the interfacial adhesion properties of a novel Self-healable siloxane polymer material via molecular dynamics simulation

The reported outstanding adhesive and self-healing properties of a novel siloxane polymer – DOSS, have made it a promising candidate as polymer matrix of thermal interface materials (TIM). To explore its potential use in TIM, here we conduct systematic investigations on the interfacial properties of the DOSS/NiO interfaces at microscopic-scale using molecular dynamics (MD) simulations. MD can provide atomic-scale information which can hardly be obtained using experimental techniques. NiO presents at the surface of the plating layer of copper heat spreader in electronic packaging. DOSS is found to form rich hydrogen bonds with NiO, resulting in stronger adhesion to NiO compared to polydimethylsiloxane (PDMS), a conventional TIM matrix. The greater strength and ductility of DOSS compared to PDMS is ascribed to its rich hydrogen bonds and star-like topology. The strength changes with tensile rate, and is attributed to different strength and relaxation time of the bonded and non-bonded interactions. For ductility, an optimal temperature is found at 375 K. The DOSS has good self-healing ability, which is characterized by an 85% recovery of hydrogen bonds at 450 K. The microscopic insights provided by current work may shed lights on the design of DOSS as future potential polymer matrix to be used in TIM.

Effect of Copper(II) Ion Binding by Porin P1 Precursor Fragments from Fusobacterium nucleatum on DNA Degradation.

Fusobacterium nucleatum is one of the most notorious species involved in colorectal cancer. It was reported that numerous outer membrane proteins (OMP) are actively involved in carcinogenesis. In this paper, the structure and stability of certain complexes, as well as DNA cleavage and ROS generation by fragments of OMP, were investigated using experimental and theoretical methods. Mass spectrometry, potentiometry, UV-Vis, CD, EPR, gel electrophoresis and calculations at the density functional theory (DFT) level were applied. Two consecutive model peptides, Ac-AKGHEHQLE-NH2 and Ac-FGEHEHGRD-NH2, were studied. Both of these were rendered to form a variety of thermodynamically stable complexes with copper(II) ions. All of the complexes were stabilized, mainly due to interactions of metal with nitrogen and oxygen donor atoms, as well as rich hydrogen bond networks. It was also concluded that these complexes in the presence of hydrogen peroxide or ascorbic acid can effectively produce hydroxyl radicals and have an ability to cleave the DNA strands. Surprisingly, the second studied ligand at the micromolar concentration range causes overall DNA degradation.

Hybrid Nafion Membranes of Ionic Hydrogen-Bonded Organic Framework Materials for Proton Conduction and PEMFC Applications.

As the high-power density and environmentally friendly energy resources, proton exchange membrane fuel cells (PEMFCs) have a promising future in portable power generation. Herein, the hybrid Nafion membranes of ionic hydrogen-bonded organic frameworks (iHOFs) for PEMFC applications are demonstrated. By adjusting the position of sulfonic groups on naphthalene disulfonic acid compounds, four iHOFs with different types of hydrogen bonds were synthesized successfully based on 1,1'-diamino-4,4'-bipyridylium and naphthalene disulfonic acid. The formation of hydrogen bond interactions between amino and sulfonate groups provides a rich hydrogen bond network, which makes such iHOFs have high conductivity, and the maximum value is 2.76 × 10-3 S·cm-1 at 100 °C and 98% RH. Besides, composite membrane materials were obtained by mixing Nafion and iHOFs, and the maximum proton conductivity values can achieve 1.13 × 10-2 S·cm-1 for 6%-iHOF-3/Nafion and 2.87 × 10-3 S·cm-1 for 6%-iHOF-4/Nafion membranes at 100 °C under 98% RH. Through the H2/O2 fuel cell performance test by using iHOF/Nafion as the solid electrolyte, the maximum power and current density values of hybrid membranes are 0.36 W·cm-2 and 1.10 A·cm-2 for 6%-iHOF-3/Nafion and 0.42 W·cm-2 and 1.20 A·cm-2 for 6%-iHOF-4/Nafion at 80 °C and 100% RH. This work provides a practicable approach for establishing high-performance proton exchange hybrid membranes by doping high proton-conducting iHOFs into the Nafion matrix.

Lanthanide‐Hypophosphite Frameworks with Guanidinium Guest Showing High Proton Conductivity

Main observation and conclusionProton‐conductive metal‐organic frameworks (MOFs) have attracted great attention for their promising application in membrane fuel cells. To explore proton‐conductive MOFs with high performance, here we present four lanthanide‐hypophosphite frameworks with distinct amine guests. These complexes possess a general formula [AH][Gd2(H2PO2)7] (AH = protonated amines). Due to the rich hydrogen bond networks, complex 1 with guanidinium as guest shows high proton conductivity of 1.75 × 10–2 S·cm–1 at a relative humidity of 97% (368 K). We also studied the magnetic properties of complex 1 and reveal that the hypophosphite ligand transfers weak antiferromagnetic interactions between Gd3+ ions.