Potential of novel iron 1,3,5-benzene tricarboxylate loaded on biochar to reduce ammonia and nitrous oxide emissions and its associated biological mechanism during composting.

In this study, a novel iron 1,3,5-benzene tricarboxylate loaded on biochar (BC-FeBTC) was developed and applied to kitchen waste composting. The results demonstrated that the emissions of NH3 and N2O were significantly reduced by 57.2% and 37.8%, respectively, compared with those in control group (CK). Microbiological analysis indicated that BC-FeBTC addition altered the diversity and abundance of community structure as well as key functional genes. The nitrification genes of ammonia-oxidizing bacteria were enhanced, thereby promoting nitrification and reducing the emission of NH3. The typical denitrifying bacterium, Pseudomonas, and critical functional genes (nirS, nirK, and nosZ) were significantly inhibited, contributing to reduced N2O emissions. Network analysis further revealed the important influence of BC-FeBTC in nitrogen transformation driven by functional microbes. These findings offer crucial scientific foundation and guidance for the application of novel materials aimed at mitigating nitrogen loss and environmental pollution during composting.

High-Temperature Polymer Dielectrics Designed Using an Invertible Molecular Graph Generative Model.

Generating new molecules with the desired physical or chemical properties is the key challenge of computational material design. Deep learning techniques are being actively applied in the field of data-driven material informatics and provide a promising way to accelerate the discovery of innovative materials. In this work, we utilize an invertible graph generative model to generate hypothetical promising high-temperature polymer dielectrics. A molecular graph generative model based on the invertible normalizing flow is trained on a data set containing 250k polymer molecular graphs (mostly generated by an RNN-based generative model) to learn the invertible transformations between latent distributions and molecular graph structures. When generating molecular graphs, a sample vector is drawn from the latent space, and then an adjacency tensor and node attribute matrix are generated through two invertible flows in two steps and assembled into a molecular graph. The model has the merits of exact likelihood training and an efficient one-shot generation process. The learned latent space is used to generate polymers with a high glass-transition temperature (Tg) and a wide band gap (Eg) for the application of high-temperature energy storage film capacitors. This work contributes to the efficient design of high-temperature polymer dielectrics by using deep generative models.

A Bilayer High-Temperature Dielectric Film with Superior Breakdown Strength and Energy Storage Density.

The further electrification of various fields in production and daily life makes it a topic worthy of exploration to improve the performance of capacitors for a long time, including thin-film capacitors. The discharge energy density of thin-film capacitors that serves as one of the important types directly depends on electric field strength and the dielectric constant of the insulation material. However, it has long been a great challenge to improve the breakdown strength and dielectric constant simultaneously. Considering that boron nitride nanosheets (BNNS) possess superior insulation and thermal conductivity owing to wide band gap and 2-dimensional structure, a bilayer polymer film is prepared via coating BNNS by solution casting on surface of polyethylene terephthalate (PET) films. By revealing the bandgap and insulating behavior with UV absorption spectrum, leakage current, and finite element calculation, it is manifested that nanocoating contributes to enhance the bandgap of polymer films, thereby suppressing the charge injection by redirecting their transport from electrodes. Worthy to note that an ultrahigh breakdown field strength (~ 736 MV m-1), an excellent discharge energy density (~ 8.77 J cm-3) and a prominent charge-discharge efficiency (~ 96.51%) are achieved concurrently, which is ascribed to the contribution of BNNS ultrathin layer. In addition, the modified PET films also have superior comprehensive performance at high temperatures (~ 120 °C). The materials and methods here selected are easily accessible and facile, which are suitable for large-scale roll-to-roll process production, and are of certain significance to explore the methods about film modification suitable for commercial promotion.

Alternating [1.1.1]Propellane-(Meth)Acrylate Copolymers: A New Class of Dielectrics with High Energy Density for Film Capacitors.

Polymer dielectrics with high energy density are of urgent demand in electric and electronic devices, but the tradeoff between dielectric constant and breakdown strength is still unsolved. Herein, the synthesis and molar mass control of three alternating [1.1.1]propellane-(meth)acrylate copolymers, denoted as P-MA, P-MMA, and P-EA, respectively, are reported. These copolymers exhibit high thermal stability and are semi-crystalline with varied glass transition temperatures and melting temperatures. The rigid bicyclo[1.1.1]pentane units in the polymer backbone promote the orientational polarization of the polar ester groups, thus enhancing the dielectric constants of these polymers, which are 4.50 for P-EA, 4.55 for P-MA, and 5.11 for P-MMA at 10 Hz and room temperature, respectively. Moreover, the high breakdown strength is ensured by the non-conjugated nature of bicyclo[1.1.1]pentane unit. As a result, these copolymers show extraordinary energy storage performance; P-MA exhibits a discharge energy density of 9.73 J cm-3 at 750 MV m-1 and ambient temperature. This work provides a new type of promising candidates as polymer dielectrics for film capacitors, and offers an efficient strategy to improve the dielectric and energy storage properties by introducing rigid non-conjugated bicyclo[1.1.1]pentane unit into the polymer backbone.

Tunable Ammonia Adsorption within Metal-Organic Frameworks with Different Unsaturated Metal Sites.

Ammonia (NH3) emissions during agricultural production can cause serious consequences on animal and human health, and it is quite vital to develop high-efficiency adsorbents for NH3 removal from emission sources or air. Porous metal-organic frameworks (MOFs), as the most promising candidates for the capture of NH3, offer a unique solid adsorbent design platform. In this work, a series of MOFs with different metal centers, ZnBTC, FeBTC and CuBTC, were proposed for NH3 adsorption. The metal centers of the three MOFs are coordinated in a different manner and can be attacked by NH3 with different strengths, resulting in different adsorption capacities of 11.33, 9.5, and 23.88 mmol/g, respectively. In addition, theoretical calculations, powder XRD patterns, FTIR, and BET for the three materials before and after absorption of ammonia were investigated to elucidate their distinctively different ammonia absorption mechanisms. Overall, the study will absolutely provide an important step in designing promising MOFs with appropriate central metals for the capture of NH3.

A Combined Experimental and Computational Study on the Adsorption Sites of Zinc-Based MOFs for Efficient Ammonia Capture.

Ammonia (NH3) is a common pollutant mostly derived from pig manure composting under humid conditions, and it is absolutely necessary to develop materials for ammonia removal with high stability and efficiency. To this end, metal-organic frameworks (MOFs) have received special attention because of their high selectivity of harmful gases in the air, resulting from their large surface area and high density of active sites, which can be tailored by appropriate modifications. Herein, two synthetic metal-organic frameworks (MOFs), 2-methylimidazole zinc salt (ZIF-8) and zinc-trimesic acid (ZnBTC), were selected for ammonia removal under humid conditions during composting. The two MOFs, with different organic linkers, exhibit fairly distinctive ammonia absorption behaviors under the same conditions. For the ZnBTC framework, the ammonia intake is 11.37 mmol/g at 298 K, nine times higher than that of the ZIF-8 framework (1.26 mmol/g). In combination with theoretical calculations, powder XRD patterns, FTIR, and BET surface area tests were conducted to reveal the absorption mechanisms of ammonia for the two materials. The adsorption of ammonia on the ZnBTC framework can be attributed to both physical and chemical adsorption. A strong coordination interaction exists between the nitrogen atom from the ammonia molecule and the zinc atom in the ZnBTC framework. In contrast, the absorption of ammonia in the ZIF-8 framework is mainly physical. The weak interaction between the ammonia molecule and the ZIF-8 framework mainly results from the inherent severely steric hindrance, which is related to the coordination mode of the imidazole ligands and the zinc atom of this framework. Therefore, this study provides a method for designing promising MOFs with appropriate organic linkers for the selective capture of ammonia during manure composting.

Recent Progress and Future Prospects on All-Organic Polymer Dielectrics for Energy Storage Capacitors.

With the development of advanced electronic devices and electric power systems, polymer-based dielectric film capacitors with high energy storage capability have become particularly important. Compared with polymer nanocomposites with widespread attention, all-organic polymers are fundamental and have been proven to be more effective choices in the process of scalable, continuous, and large-scale industrial production, leading to many dielectric and energy storage applications. In the past decade, efforts have intensified in this field with great progress in newly discovered dielectric polymers, fundamental production technologies, and extension toward emerging computational strategies. This review summarizes the recent progress in the field of energy storage based on conventional as well as heat-resistant all-organic polymer materials with the focus on strategies to enhance the dielectric properties and energy storage performances. The key parameters of all-organic polymers, such as dielectric constant, dielectric loss, breakdown strength, energy density, and charge-discharge efficiency, have been thoroughly studied. In addition, the applications of computer-aided calculation including density functional theory, machine learning, and materials genome in rational design and performance prediction of polymer dielectrics are reviewed in detail. Based on a comprehensive understanding of recent developments, guidelines and prospects for the future development of all-organic polymer materials with dielectric and energy storage applications are proposed.

All-Organic Dielectrics with High Breakdown Strength and Energy Storage Density for High-Power Capacitors.

Polymer-based film capacitors with high breakdown strength and excellent flexibility are crucial in the field of advanced electronic devices and electric power systems. Although massive works are carried to enhance the energy storage performances, it is still a great challenge to improve the energy density of polymer composites under the premise of large-scale industrial production. Herein, a general strategy is proposed to improve the intrinsic breakdown strength and energy storage performances by blending core-shell structured methyl methacrylate-butadiene-styrene (MBS) rubber particles into a polymer matrix. Good compatibility and uniform dispersion state of MBS particles are observed in the matrix. Polarizing microscopy images show that blended films exhibit clear reduction of crystalline grains with the addition of MBS particles. Accordingly, an increased breakdown strength of 515 MV m-1 and discharged energy density of 12.33 J cm-3 are observed in poly(vinylidene fluoride-co-hexafluoropropylene)-based composite films. Through comprehensive characterizations, it is believed that the superior energy storage performance of composite films is attributed to decreased crystalline grains, improved mechanical properties, and restriction on carrier motion. These results provide a novel design of dielectric polymers for high breakdown strength and discharged energy density applications.