Organic-inorganic Systems Research Articles

Cyclic Oxothiomolybdates: Building Blocks for Cyclodextrin-Based Open Frameworks.

Desolvation processes, though common in self-assembled biological structures, are rarely evidenced and utilized in the design of crystalline architectures. In this study, we introduce a novel approach using the [Mo8S8O8(OH)8(guest)]2- complex, formed by the self-condensation of four [MoV 2O2S2]2- fragments around a guest unit (MoVIO6H4 or oxalate), as a chaotropic scaffold for crystallizing hybrid organic-inorganic systems with natural cyclodextrins. Our findings reveal that β-cyclodextrin (β-CD) facilitates the formation of host-guest complexes, while α-cyclodextrin (α-CD) induces the formation of a Kagome-type structure with significant voids. These new compounds were thoroughly characterized using X-ray diffraction (both powder and single-crystal), N2 adsorption, elemental and thermogravimetric analysis. Additionally, solution studies using 1H NMR titration and small-angle X-ray scattering (SAXS) demonstrated pre-association of the building units in solution. These results enhance our understanding of the design principles for supramolecular structures composed of inorganic polyanions and cyclodextrins.

Decorated palladium nanoparticles over chitosan-agarose encapsulated Fe3O4 microspheres: Investigation of its catalytic efficiency in the Suzuki-Miaura coupling reactions

The enhanced properties of heterogeneous catalysts have led to significant interest in recent years, particularly in composite materials that incorporate organic-inorganic systems. In this particular study, a series of steps were undertaken to synthesize Fe3O4 microspheres, which were subsequently coated with chitosan and agarose. Finally, palladium nanoparticles were immobilized onto the surface of the microspheres, resulting in the formation of Fe3O4 MPs@CS-Agar/Pd NPs. To evaluate the material, advanced analytical techniques such as FT-IR, FESEM-EDS, ICP-OES, TEM, XRD, and VSM were utilized to determine its structural and physicochemical characteristics. The results shown that the Pd nanoparticles were formed in nanometer-sized particles, exhibiting a quasi-spherical shape with an average diameter ranging from 20–40 nm. Notably, the Fe3O4 MPs@CS-Agar/Pd NPs exhibited remarkable catalytic activity in Suzuki-Miyaura reaction. Importantly, the nanocatalyst could be reused up to 8 times without any decline in its activity. The exceptional catalytic performance of the Fe3O4 MPs@CS-Agar/Pd NPs in these reactions can be attributed to the distinctive nanostructure characteristics it possesses.

Enhancing phosphorus transformation in typical reddish paddy soil from China: Insights on long-term straw return and pig manure application via microbial mechanisms

Effective utilization of organic resources to activate residual phosphorus (P) in soil and enhance its availability is crucial for mitigating P resource scarcity and assessing the sustainable use of P in agricultural practices. However, the mechanisms through which organic resources affect soil P conversion via microorganisms and functional genes remain unknown, particularly in long-term organic-inorganic agricultural systems. In this study, we examined the impact of combined organic-inorganic fertilizer application on P availability, carbon (C) and P cycling genes, and microbial communities (bacterial and fungal) in reddish paddy soil based on a 42-year field experiment. The results indicated that long-term straw returning and pig manure application significantly augmented soil organic carbon (SOC), Olsen-P, microbial biomass carbon (MBC), microbial biomass phosphorus (MBP), enzyme-P, and CaCl2-P levels in paddy soils. Furthermore, these practices increased the abundance of soil C degradation genes, reduced the abundance of soil P cycling genes, and altered microbial community structure and network complexity. Notably, Module #3 ecological clusters in the fungal ecological co-occurrence network were significantly correlated with P cycling genes. Finally, our study demonstrated that long-term straw returning and pig manure application in paddy fields facilitated two robust and contrasting predictive relationships between C degradation (negative relationship) and P cycling (positive relationship) genes, respectively, and enzyme-P and HCl-P changes to improve soil P availability. This study can enhance our understanding of the role of soil microbial communities and functional genes in mediating P transformation to decipher the enhancement in P application efficiency driven by organic resources in reddish paddy soils.

ОСОБЕННОСТИ ВЗАИМОДЕЙСТВИЯ ГЕМИНА И ZnII-КОМПЛЕКСА ТЕТРА(4 ПИРИДИЛ) ПОРФИРИНА С ГЕКСАМОЛИБДЕНОНИКЕЛАТ-ПОЛИАНИОНОМ В ВОДНЫХ СРЕДАХ

This work presents a method for producing new hybrid supramolecular organic-inorganic systems based on tetrapyrrole compounds (natural and artificially synthesized porphyrins) and hexamolibdenonicelate anion to create highly ordered supramolecular complexes based on porphyrins with the possibility of using them in medicine. In particular, the reaction of natural porphyrin (hemin) and the ZnII-complex of tetra(4-pyridyl)porphyrin with the heteropoly compound sodium hexamolibdenonicelate crystalline hydrate Na4[Ni(OH)6Mo6O18]·8H2O in an aqueous medium is considered. This heteropoly compound due to its physicochemical and biological properties can be considered as a part of photochromic materials and pharmacological agent. The optical absorption spectra of the obtained hybrid supramolecular organic-inorganic systems were investigated with the help of electronic absorption spectroscopy. Both the transformation of the bands which are the characteristics of porphyrins and the appearance of new bands indicating the formation of hybrid supramolecular organic-inorganic complexes are observed in the electron absorption spectra. The work traces the role of structural features of porphyrins in the process of their interaction with the heteropolyanions. Differences in the spectral behavior of the two metalloporphyrins when interacting them with the heteropoly compound have been shown and explained by variability in their structure. The data obtained will be useful when developing new hybrid materials as antibacterial components for medical use.

Broadband Green Luminescence and Phase Transition in Low-Dimensional Organic-Inorganic Hybrid Iodate.

Organic-inorganic hybrid iodide systems, which can form highly ordered chromophores and uniformly oriented transition dipole moments, serve as optimal host-guest systems for the fabrication of micrometer-scale optical devices. In particular, those with low-dimensional structures can exhibit strong quantum-limited and highly localized charges, enabling the generation of high exciton energies and stable excitation emission. In this study, we report a novel instance of an organic-inorganic hybrid iodate, (C13H11N2)(IO3), which was synthesized by incorporating the optically active organic compound, 9-aminoacridine. Upon crystallization in the monoclinic space group P21/c, this compound exhibits a direct optical band gap of 2.66 eV. The incorporation of discrete organic units within the low-dimensional structures induces pronounced local charges, culminating in broadband green luminescence with a peak at 540 nm under UV excitation. This corresponds to the CIE coordinates (0.37, 0.56). A potential phase transition was inferred through a comprehensive analysis of the variable temperature structure and emission spectra. Furthermore, first-principles calculations revealed the pivotal role of organic cations in facilitating broadband luminescence.

Achieving synergistic improvement in dielectric and energy storage properties at high-temperature of all-organic composites via physical electrostatic effect.

In response to the increasing demand for miniaturization and lightweight equipment, as well as the challenges of application in harsh environments, there is an urgent need to explore the new generation of high-temperature-resistant film capacitors with excellent energy storage properties. In this study, we report an all-organic composite system based on two polymers with similar densities and high glass transition temperatures, achieving a synergistic effect of dielectric constant and breakdown strength. The preparation of the composite is simple, overcoming the challenge of dispersing nanoparticles in traditional organic-inorganic systems. The high polarity of polyethersulfone can modulate the polarization properties of the composites and, through a physical electrostatic effect, inhibit dipole relaxation, further reducing the current density of the composite dielectric at high temperatures, resulting in a significant improvement in insulating properties. The 9 : 1 composite dielectric at 150 °C demonstrates an energy storage density of up to 6.4 J cm-3 and an efficiency of 82.7%. This study offers a promising candidate material and development direction for the next-generation energy storage capacitors with broad application prospects.

Super-strong Zn and S atomic terminals in an organic/inorganic hybrid S-scheme polyimide based heterojunction for efficient photocatalytic treatment of mixed pollutant wastewater

Integrated oxidation and reduction reactions in the field of wastewater treatment with mixed high concentrations of sewage achieved by photocatalysis are highly desirable but still challenging. The construction of the S-scheme heterojunction system is expected to be a promising strategy to provide carriers with strong redox ability for oxidation of oxytetracycline hydrochloride (OTC) with simultaneous reduction of hexavalent chromium (Cr(VI)). Reduced graphene oxide (rGO) and ZnIn2S4 (ZIS) were successively assembled on perylene diimide polymer (PDIP) nanorods to form the S-scheme ZIS/rGO/PDIP heterojunction. The construction of organic–inorganic systems achieves wide light absorption, enhanced exciton dissociation and accelerated charge separation. A non-radiation-quenched electron transport path is formed in the ZIS/rGO/PDIP system from the conduction band of PDIP through rGO to the valence band of ZIS. The electronic energy state of the S-scheme ZIS/rGO/PDIP heterojunction was changed, and the Zn and S atomic terminals can realize strong adsorption of OTC and Cr(VI).

Metastable Charged Dimers in Organometallic Species: A Look into Hydrogen Bonding between Metallocene Derivatives.

Multiply charged complexes bound by noncovalent interactions have been previously described in the literature, although they were mostly focused on organic and main group inorganic systems. In this work, we show that similar complexes can also be found for organometallic systems containing transition metals and deepen in the reasons behind the existence of these species. We have studied the structures, binding energies, and dissociation profiles in the gas phase of a series of charged hydrogen-bonded dimers of metallocene (Ru, Co, Rh, and Mn) derivatives isoelectronic with the ferrocene dimer. Our results indicate that the carboxylic acid-containing dimers are more strongly bonded and present larger barriers to dissociation than the amide ones and that the cationic complexes tend to be more stable than the anionic ones. Additionally, we describe for the first time the symmetric proton transfer that can occur while in the metastable phase. Finally, we use a density-based energy decomposition analysis to shine light on the nature of the interaction between the dimers.

Evidence for Hybrid Inorganic–Organic Transitions at the WS2/Terrylene Interface

The realization of the potential of hybrid inorganic organic systems requires an understanding of the coupling between the constituents: its nature and its strength. The observation of hybrid optical transitions in the monolayer WS2/terrylene hybrid is reported. The first‐principle calculations, linear optical, and transient absorption spectroscopy are employed to investigate the optical spectrum of the hybrid, which exhibits a new transition that does not appear in the constituents’ spectra. The calculations indicate type II level alignment, with the highest occupied level of terrylene in the gap of WS2. Exploiting state‐resolved transient absorption, the response of the hybrid interface to optical excitation is selectively probed. The dynamics reveal rapid hole transfer from WS2 to the terrylene layer, with a decay time of 88 ps. This hole transfer induces a bleach of the hybrid transition, which indicates that terrylene contributes to its initial state. Based on this, the hybrid resonance energy, and on our calculations, we assign the hybrid feature to a transition from the highest occupied molecular orbital of terrylene to the conduction band of WS2 close to the Γ point. The results indicate that the conditions for strong electronic coupling are met in this hybrid system.

Significantly Enhanced Poling Efficiency of Piezocomposites by Tuning Resistivity of a Polymer Matrix.

Although the ability to convert biomechanical vibrations into electric energy has been demonstrated in organic-inorganic piezocomposites, it is challenging to improve their piezoelectric properties owing to insufficient electric field poling. Here, we propose a facile and effective approach to enhance the poling efficiency of a barium calcium zirconate titanate/polydimethylsiloxane (BCZT/PDMS) composite by introducing copper nanowires (Cu NWs) to tune the resistivity of the PDMS matrix. The Cu NW-modified PDMS weakens the resistivity mismatch between the BCZT filler and the PDMS matrix, allowing a higher poling electric field to be applied to the BCZT filler during poling. As a result, the BCZT/Cu-PDMS piezocomposite exhibited a high piezoelectric quality factor (d33 × g33) of 2.58 pm2/N, which was about 7 times higher than that of BCZT/PDMS (d33 × g33 = 0.38 pm2/N). Moreover, BCZT/Cu-PDMS showed a much higher power density (3.18 μW/cm2) and a faster charging capability. This composite approach of introducing metal nanowires can be considered as a generic poling-improvement method that can be extended to other organic-inorganic piezocomposite systems.

Spiking neural networks compensate for weight drift in organic neuromorphic device networks

Organic neuromorphic devices can accelerate neural networks and integrate with biological systems. Devices based on the biocompatible and conductive polymer PEDOT:PSS are fast, require low amounts of energy and perform well in crossbar simulations. However, parasitic electrochemical reactions lead to self-discharge and the fading of the learned conductance states over time. This limits a neural network’s operating time and requires complex compensation mechanisms. Spiking neural networks (SNNs) take inspiration from biology to implement local and always-on learning. We show that these SNNs can function on organic neuromorphic hardware and compensate for self-discharge by continuously relearning and reinforcing forgotten states. In this work, we use a high-resolution charge transport model to describe the behavior of organic neuromorphic devices and create a computationally efficient surrogate model. By integrating the surrogate model into a Brian 2 simulation, we can describe the behavior of SNNs on organic neuromorphic hardware. A biologically plausible two-layer network for recognizing pixel MNIST images is trained and observed during self-discharge. The network achieves, for its size, competitive recognition results of up to 82.5%. Building a network with forgetful devices yields superior accuracy during training with 84.5% compared to ideal devices. However, trained networks without active spike-timing-dependent plasticity quickly lose their predictive performance. We show that online learning can keep the performance at a steady level close to the initial accuracy, even for idle rates of up to 90%. This performance is maintained when the output neuron’s labels are not revalidated for up to 24 h. These findings reconfirm the potential of organic neuromorphic devices for brain-inspired computing. Their biocompatibility and the demonstrated adaptability to SNNs open the path towards close integration with multi-electrode arrays, drug-delivery devices, and other bio-interfacing systems as either fully organic or hybrid organic-inorganic systems.

Organic-inorganic heterojunction photocatalysts: From organic molecules to frameworks

The clean and abundant solar energy has been proven to be a promising alternative energy source for traditional fossil fuel. Inspired by natural biological photosynthesis, global scientists developed numerous artificial photocatalytic systems to converted solar energy into chemical energy (including degradation, CO2 reduction, N2 fixation, water splitting, etc.). Nevertheless, current photocatalytic activity is hindered by various factors such as severe recombination of photogenerated charges, insufficient reduction/oxidation potentials, inadequate light-harvesting, and photocorrosion. Thus, it is urgent to design more efficient and stable photocatalysis systems. This review main focuses on recent advances in organic-inorganic heterojunction photocatalysts, based on organic semiconductors from molecules to frameworks. The synergistic effect between organic and inorganic components, and meaningful heterojunctions (like S-scheme or Z-scheme) are emphasized in this work. Finally, the outlooks and challenges for efficient inorganic-organic composites systems are also proposed.

New Carbamoyl Surface-Modified ZrO2 Nanohybrids for Selective Au Extraction from E-Waste

Efficient and selective extractions of precious and critical metal ions such as Au(III) and Pd(II) were investigated using zirconia nanoparticles surface modified with different organic mono- and di-carbamoyl phosphonic acid ligands. The modification is made on the surface of commercial ZrO2 that is dispersed in aqueous suspension and was achieved by optimizing the Bronsted acid-base reaction in ethanol/H2O solution (1:2), resulting in inorganic-organic systems of ZrO2-Ln (Ln: organic carbamoyl phosphonic acid ligand). The presence, binding, amount, and stability of the organic ligand on the surface of zirconia nanoparticles were confirmed by different characterizations such as TGA, BET, ATR-FTIR, and 31P-NMR. Characterizations showed that all the prepared modified zirconia had a similar specific surface area (50 m2.g-1) and the same amount of ligand on the zirconia surface in a 1:50 molar ratio. ATR-FTIR and 31P-NMR data were used to elucidate the most favorable binding mode. Batch adsorption results showed that (i) ZrO2 surface modified with di-carbamoyl phosphonic acid ligands had the highest adsorption efficiency to extract metals than mono-carbamoyl ligands, and (ii) higher hydrophobicity of the ligand led to better adsorption efficiency. The surface-modified ZrO2 with di-N,N-butyl carbamoyl pentyl phosphonic acid ligand (ZrO2-L6) showed promising stability, efficiency, and reusability in industrial applications for selective gold recovery. In terms of thermodynamic and kinetic adsorption data, ZrO2-L6 fits the Langmuir adsorption model and pseudo-second-order kinetic model for the adsorption of Au(III) with maximum experimental adsorption capacity qmax = 6.4 mg.g-1.

Toward a critical social theory of AI: Knowledge, information, and intelligence in the later works of André Gorz

In his last scholarly work, L’Immatériel, André Gorz grapples with the emergence of the new cognitive capitalism based on immaterial labor and capital and, crucially, he seeks to comprehend how advanced technologies—such as nanotechnology, biotechnology, ICTs, and specifically, AI—reshape the very nature of the human subject. Despite its vital contributions, his conventional form of humanism—one that draws clear lines between organic human culture and inorganic machinic systems—is questioned and challenged by the increasingly complex and pervasive interplay between the two domains. Focusing on his later writings, this essay critically examines Gorz’s social theory of cognitive capitalism with particular reference to knowledge, information and intelligence. In doing so, the essay draws out some theoretical implications of Gorz’s defense of the humanities against post-human civilization for the development of a critical social theory of AI.

Recent Progress in Chitosan-Containing Composite Materials for Sustainable Approaches to Adsorption and Catalysis

In recent years, composite materials including organic–inorganic systems have drawn special attention due to their enhanced properties such as adsorbents and heterogeneous catalysts. At the same time, large-scale production of environmentally benign functionalized biopolymers, such as chitosan (CS), allows for constantly developing new materials, since CS reveals remarkable properties as a stabilizing agent for metal-containing compounds and enzymes and as an adsorbent of organic molecules. This review is focused on CS-based materials and on the composite systems including CS-oxide and CS-metal composites in particular for application as adsorbents and supports for catalytically active metal nanoparticles and enzymes.

Direct CO2 Capture by Alkali-Dissolved Cellulose and Sequestration in Building Materials and Artificial Reef Structures.

Current carbon capture and utilization (CCU) technologies require high energy input and costly catalysts. Here, an effective pathway is offered that addresses climate action by atmospheric CO2 sequestration. Industrially relevant highly reactive alkali cellulose solutions are used as CO2 absorption media. The latter lead to mineralized cellulose materials (MCM) at a tailorable cellulose-to-mineral ratio, forming organic-inorganic viscous systems (viscosity from 102 to 107 mPas and storage modulus from 10 to 105 Pa). CO2 absorption and conversion into calcium carbonate and associated minerals translate to maximum absorption of 6.5gCO2 gcellulose -1 , tracking inversely with cellulose loading. Cellulose lean gels are easily converted into dry powders, shown as a functional component of ceramic glazes and cementitious composites. Meanwhile, cellulose-rich gels are moldable and extrudable, yielding stone-like structures tested as artificial substrates for coral reef restoration. Life Cycle Assessment (LCA) suggests new CCU opportunities for building materials, as demonstrated in underwater deployment for coral reef ecosystem restoration.

Nanocrystalline CaWO4 and ZnWO4 Tungstates for Hybrid Organic-Inorganic X-ray Detectors.

Hybrid materials combining an organic matrix and high-Z nanomaterials show potential for applications in radiation detection, allowing unprecedented device architectures and functionality. Herein, novel hybrid organic-inorganic systems were produced using a mixture of tungstate (CaWO4 or ZnWO4) nanoparticles with a P3HT:PCBM blend. The nano-tungstates with a crystallite size of 43 nm for CaWO4 and 30 nm for ZnWO4 were synthesized by the hydrothermal method. Their structure and morphology were characterized by X-ray diffraction and scanning electron microscopy. The hybrid systems were used to fabricate direct conversion X-ray detectors able to operate with zero bias voltage. The detector performance was tested in a wide energy range using monochromatic synchrotron radiation. The addition of nanoparticles with high-Z elements improved the detector response to X-ray radiation compared with that of a pure organic P3HT:PCBM bulk heterojunction cell. The high dynamic range of our detector allows for recording X-ray absorption spectra, including the fine X-ray absorption structure located beyond the absorption edge. The obtained results suggest that nanocrystalline tungstates are promising candidates for application in direct organic-inorganic X-ray detectors.

Stability of Metal Hydroxide Organic Frameworks for Oxygen Evolution

The oxygen evolution reaction (OER) is central to storing electrical energy via chemical bonds in energy carriers and fuels through reactions such as electrochemical water splitting to produce hydrogen, CO2 reduction for CO and liquid hydrocarbons, and nitrogen to ammonia. While there has been considerable work towards the engineering of inexpensive yet highly active OER catalysts, current state-of-the-art materials are still at least an order of magnitude less active than oxygen evolving complexes found in biological systems that intricately combine inorganic metal-oxo clusters with organic ligands.1 As a result, metal organic frameworks (MOFs) have drawn considerable attention as hybrid organic-inorganic systems that can potentially mimic the unique structure of biological oxygen evolving complexes. Recently, metal hydroxide organic frameworks (MHOFs),2 a new class of MOFs that combine layered hydroxides with aromatic carboxylate linkers that stabilize the structure via π-π interactions, have been shown to display three times the tunability of layered hydroxides, offering extensive opportunities for further engineering of its electrochemical properties for numerous applications. However, the long-term stability of these material during OER is still unclear, which would be paramount to understand for further rational design of this class of material.In this study, we investigated Ni-based MHOFs with carboxylate linkers of varying π-π interaction strengths to understand how these differences affect the electrochemical stability of these materials during OER. We observed that the MHOFs all undergo activation during OER leading to two orders of magnitude increase in OER activity, where the MHOFs with weaker π-π interaction strengths tend to transform at a faster rate than the MHOFs with stronger π-π interaction strengths. We further characterized the MHOFs using a wide range of analytical techniques, including scanning transmission electron microscopy, Raman spectroscopy, x-ray photoelectron spectroscopy, and hard x-ray absorption spectroscopy, before and after extended OER cycling and galvanostatic tests to understand the transformed phase, which suggested that while the bulk structure largely remains unchanged, the surface undergoes significant restructuring into a Ni(OH)2-like phase during OER. Using operando UV-vis and Raman spectroscopy measurements on the MHOFs during OER to understand the factors that induce the transformation process, we found that there was a clear link between the Ni2+/3+, 4+ redox couple observed around 1.4 VRHE and a loss in the carboxylate organic linkers for the linkers with weak π-π interactions. However, for the MHOFs synthesized with linkers exhibiting strong π-π interaction strengths, there were smaller changes to the overall material during OER, suggesting that the bulk stability of these materials is largely dictated by the linker interaction strength and activation are primarily only surface transformations. These results directly demonstrate that linker selection also plays a key role in the stability MOFs under electrochemical conditions and are pertinent for rational design and understanding of the stability and activity of hybrid organic-inorganic materials as electrocatalysts.

Green and efficient production of functionalized graphene to achieve soybean meal-based adhesive enhancement

Designing organic-inorganic nanohybrid systems have exhibited considerable potential in fabricating high-performance protein-based adhesives. However, the simplicity of the strategy, renewability, cost and effective dispersion of inorganic nanofillers in a hybrid framework remains challenging. This study proposed a simple, cost-effective, and sustainable design strategy to fabricate soybean meal (SM)-based hybrid adhesives using sodium lignosulfonate-functionalized graphene (SLS@G). SLS@G was simultaneously produced and functionalized via a dry ball milling method from graphite without using toxic reagents and tedious fabrication procedures. SLS@G had stable water dispersion and good compatibility with the SM adhesive matrix. The synergistic hydrogen bonding and hydrophobic interaction between SLS@G and the protein chains remarkedly improved the strength and water resistance of the SM-based adhesive. With minimal addition of the SLS@G (0.10 wt% of SM), the modified adhesive dry and wet shear strengths increased to 2.19 MPa and 1.15 MPa, which were 32.7% and 248.5% higher than the pristine adhesive, respectively. Moreover, the construction of the organic-inorganic nanohybrid structure also contributed to the thermal stability of the SM-based adhesives, leading to the increase in carbon residue rate from 26.6% to 28%. Overall, this facile and green strategy offers a new design pathway for developing advanced and multifunctional bio-adhesives for engineered wood-based composites.

Two-Dimensional Organic-Inorganic Room-Temperature Multiferroics.

Organic-inorganic multiferroics are promising for the next generation of electronic devices. To date, dozens of organic-inorganic multiferroics have been reported; however, most of them show a magnetic Curie temperature much lower than room temperature, which drastically hampers their application. Here, by performing first-principles calculations and building effective model Hamiltonians, we reveal a molecular orbital-mediated magnetic coupling mechanism in two-dimensional Cr(pyz)2 (pyz = pyrazine) and the role that the valence state of the molecule plays in determining the magnetic coupling type between metal ions. Based on these, we demonstrate that a two-dimensional organic-inorganic room-temperature multiferroic, Cr(h-fpyz)2 (h-fpyz = half-fluoropyrazine), can be rationally designed by introducing ferroelectricity in Cr(pyz)2 while keeping the valence state of the molecule unchanged. Our work not only reveals the origin of magnetic coupling in 2D organic-inorganic systems but also provides a way to design room-temperature multiferroic materials rationally.