Synthesis Of Materials Research Articles

Toward Self-Driven Autonomous Material and Device Acceleration Platforms (AMADAP) for Emerging Photovoltaics Technologies.

ConspectusIn the ever-increasing renewable-energy demand scenario, developing new photovoltaic technologies is important, even in the presence of established terawatt-scale silicon technology. Emerging photovoltaic technologies play a crucial role in diversifying material flows while expanding the photovoltaic product portfolio, thus enhancing security and competitiveness within the solar industry. They also serve as a valuable backup for silicon photovoltaic, providing resilience to the overall energy infrastructure. However, the development of functional solar materials poses intricate multiobjective optimization challenges in a large multidimensional composition and parameter space, in some cases with millions of potential candidates to be explored. Solving it necessitates reproducible, user-independent laboratory work and intelligent preselection of innovative experimental methods.Materials acceleration platforms (MAPs) seamlessly integrate robotic materials synthesis and characterization with AI-driven data analysis and experimental design, positioning them as enabling technologies for the discovery and exploration of new materials. They are proposed to revolutionize materials development away from the Edisonian trial-and-error approaches to ultrashort cycles of experiments with exceptional precision, generating a reliable and highly qualitative data situation that allows training machine learning algorithms with predictive power. MAPs are designed to assist the researcher in multidimensional aspects of materials discovery, such as material synthesis, precursor preparation, sample processing and characterization, and data analysis, and are drawing escalating attention in the field of energy materials. Device acceleration platforms (DAPs), however, are designed to optimize functional films and layer stacks. Unlike MAPs, which focus on material discovery, a central aspect of DAPs is the identification and refinement of ideal processing conditions for a predetermined set of materials. Such platforms prove especially invaluable when dealing with "disordered semiconductors," which depend heavily on the processing parameters that ultimately define the functional properties and functionality of thin film layers. By facilitating the fine-tuning of processing conditions, DAPs contribute significantly to the advancement and optimization of disordered semiconductor devices, such as emerging photovoltaics.In this Account, we review the recent advancements made by our group in automated and autonomous laboratories for advanced material discovery and device optimization with a strong focus on emerging photovoltaics, such as solution-processing perovskite solar cells and organic photovoltaics. We first introduce two MAPs and two DAPs developed in-house: a microwave-assisted high-throughput synthesis platform for the discovery of organic interface materials, a multipurpose robot-based pipetting platform for the synthesis of new semiconductors and the characterization of thin film semiconductor composites, the SPINBOT system, which is a spin-coating DAP with the potential to optimize complex device architectures, and finally, AMANDA, a fully integrated and autonomously operating DAP. Notably, we underscore the utilization of a robot-based high-throughput experimentation technique to address the common optimization challenges encountered in extensive multidimensional composition and parameter spaces pertaining to organic and perovskite photovoltaics materials. Finally, we briefly propose a holistic concept and technology, a self-driven autonomous material and device acceleration platform (AMADAP) laboratory, for autonomous functional solar materials discovery and development. We hope to discover how AMADAP can be further strengthened and universalized with advancing development of hardware and software infrastructures in the future.

Synthesis, Characterization, and Properties of Heat-Resistant Energetic Materials Based on C-C Bridged Dinitropyrazole Energetic Materials.

Polycyclic energetic materials make up a distinctive class of conjugated structures that consist of two or more rings. In this work, 1,3-bis(3,5-dinitro-1H-pyrazol-4-yl)-4,6-dinitrobenzene (BDPD) was synthesized and investigated in detail as a polycyclic heat-resistant energetic molecule that can be deprotonated by bases to obtain its anionic (3-5) salts. All compounds were thoroughly characterized by 1H and 13C NMR, infrared spectroscopy, high-resolution mass spectrometry, and elemental analysis. The structural features of BDPD and its salts were investigated by single-crystal X-ray diffraction and analyzed by different kinds of computing software, like Multiwfn, Gaussian 09W, and so on. In addition, their thermal decomposition temperatures were evaluated by differential scanning calorimetry to be 319.8-329.0 °C, revealing that they possessed high thermal stabilities. The results of impact sensitivity and friction sensitivity analysis confirm that these energetic compounds were insensitive. The detonation properties of neutral compound BDPD and all its nonmetallic salts were calculated by the EXPLO5 v6.05.04 program. The results revealed that their detonation performances were higher than those of the widely used heat-resistant explosive 2,2',4,4',6,6'-hexanitrostilbene (HNS). Combining the above results, it is reasonable to suggest that these compounds have the potential to be heat-resistant energetic materials.

Ultrafast In-Situ synthesis of flexible MoO3 anode in five seconds for High-Performance aqueous zinc ion hybrid capacitor

The efficient synthesis of high-performance α-MoO3 on flexible conductive substrates is crucial for enhancing its value in the field of energy storage. However, traditional synthesis methods currently employed often suffer from slow heating rates, intricate reaction processes involving multiple steps, sluggish reaction kinetics, high energy consumption, and prolonged preparation times, thereby hindering efficient production. Presented herein is a facile, ultrafast, and versatile approach utilizing microwave carbon thermal shock, a one-step reaction synthesis of α-MoO3 on carbon substrates within 5 s. During microwave carbon thermal shock, the precursor salt experiences an extremely rapid heating rate, swiftly decomposing to form small-sized α-MoO3 crystals. Simultaneously, this process promotes the oxidation of adjacent carbon sites, thereby imparting multi-scale defects and oxygen-containing functional groups to the resulting carbon cloth (CC). The exceptionally low reaction energy barriers and superior Gibbs free energy (ΔG) further substantiate the advantages of the microwave carbon thermal shock strategy over traditional synthesis methods in terms of both kinetics and thermodynamics. The air-assisted transient microwave carbonthermal shock (AMCTS) process circumvents high energy requirements, multistep reactions, and extended preparation times, endowing AMCTS-CC@MoO3 with remarkable flexibility and processability. In demonstrating its practical utility within zinc-ion hybrid micro capacitors, it exhibits outstanding specific capacitance (up to 2300mF cm−2) and mechanical stability. This air-assisted transient microwave thermal shock process provides an efficient route for ultrafast and low-cost synthesis of flexible zinc-ion anode materials.

Uncovering the Recent Progress of CNC-Derived Chirality Nanomaterials: Structure and Functions.

Cellulose nanocrystal (CNC), as a renewable resource, with excellent mechanical performance, low thermal expansion coefficient, and unique optical performance, is becoming a novel candidate for the development of smart material. Herein, the recent progress of CNC-based chirality nanomaterials is uncovered, mainly covering structure regulations and function design. Undergoing a simple evaporation process, the cellulose nanorods can spontaneously assemble into chiral nematic films, accompanied by a vivid structural color. Various film structure-controlling strategies, including assembly means, physical modulation, additive engineering, surface modification, geometric structure regulation, and external field optimization, are summarized in this work. The intrinsic correlation between structure and performance is emphasized. Next, the applications of CNC-based nanomaterials is systematically reviewed. Layer-by-layer stacking structure and unique optical activity endow the nanomaterials with wide applications in the mineralization, bone regeneration, and synthesis of mesoporous materials. Besides, the vivid structural color broadens the functions in anti-counterfeiting engineering, synthesis of the shape-memory and self-healing materials. Finally, the challenges for the CNC-based nanomaterials are proposed.

Over all Benefits of Gift of Nature (Microbial Communities) to Sustainable Environmental Health

Background: Microorganisms are widespread in nature and are beneficial to life in producing oxygen in environment, decomposing organic material, medicine, providing nutrients for plants, and maintaining human health. The effects of microbes on their environment can be beneficial or harmful with regard to human observation. Microbes also regulates environmental health through interactions with plant microbiota, which actively participate in substance cycling (particularly the carbon and nitrogen cycles) and influence the overall energy flow in the biosphere. Review Results: The most significant effect of the microbes on earth is their ability to recycle the primary elements that make up all living systems, especially carbon, oxygen, and nitrogen (N). Primary production involves photosynthetic organisms which take up CO2 from the atmosphere and convert it to organic (cellular) material. The process is also called CO2 fixation, and it accounts for a very large portion of organic carbon available for synthesis of cell material. Decomposition or biodegradation results in the breakdown of complex organic materials to other forms of carbon that can be used by other Organisms. Microorganisms are also highly involved in degradation, eradication, immobilization, or Detoxification of diverse chemical wastes and physical hazardous materials from the surrounding and transforming pollutants such as hydrocarbons, oil, heavy metal, pesticides, dye’s and so on through enzymatic way and contributed to solve many environmental problems. Conclusion: Thus, along with all these benefits, microbes greatly contribute in maintaining sustainability of environment. This review mainly focuses on beneficial impacts of microbes on environment and their role to maintain quality, health, and sustainability of environment and also encourage further efforts to study microbial ecology and protect the natural environment.

Simultaneous Interface Engineering and Phase Tuning of CeO2-Decorated Catalysts for Boosted Oxygen Evolution Reaction.

Heterogeneous catalysts have attracted extensive attention among various emerging catalysts for their exceptional oxygen evolution reaction (OER) capabilities, outperforming their single-component counterparts. Nonetheless, the synthesis of heterogeneous materials with predictable, precise, and facile control remains a formidable challenge. Herein, a novel strategy involving the decoration of catalysts with CeO2 is introduced to concurrently engineer heterogeneous interfaces and adjust phase composition, thereby enhancing OER performance. Theoretical calculations suggest that the presence of ceria reduces the free energy barrier for the conversion of nitrides into metals. Supporting this, the experimental findings reveal that the incorporation of rare earth oxides enables the controlled phase transition from nitride into metal, with the proportion adjustable by varying the amount of added rare earth. Thanks to the role of CeO2 decoration in promoting the reaction kinetics and fostering the formation of the genuine active phase, the optimized Ni3FeN/Ni3Fe/CeO2-5% nanoparticles heterostructure catalyst exhibits outstanding OER activity, achieving an overpotential of just 249mV at 10mAcm-2. This approach offers fresh perspectives for the conception of highly efficient heterogeneous OER catalysts, contributing a strategic avenue for advanced catalytic design in the field of energy conversion.

Advancement in Fabrication and Characterization Techniques of Nanocomposites.

Advancements in the field of materials research have unveiled numerous unparalleled features, such as mechanical properties, clinical advances, interfacial strengthening, and porosities, providing a wide range of applications. The employment of any material begins with fabrication and characterization, demanding expertise for the effective execution of the investigation. This review encompasses the details of the working principles of some significant and frequently used fabrication and characterization techniques for various material categories, including pellets and coatings. The discussion begins with techniques for fabricating materials for various applications. A brief overview of coating synthesis methods can provide intriguing information for researchers in the field of coating fabrication. The report highlights the portrayal of morphological and physiochemical analysis techniques, followed by the estimation of the elastic modulus using nanoindentation and dynamic modulus mapping testing for the materials. Additionally, the review covers theoretical models for observing the elastic moduli of the materials. The review depicts tribological investigations of the materials, aiming to provide insight into fretting wear, pin-on-disc, and microscratch testing. The fundamentals of electrochemical characterization are presented, including the appraisal of linear polarization and potentiodynamic polarization as well as electrochemical impedance spectroscopy. Furthermore, the magnetic behavior was examined by using a vibrating sample magnetometer (VSM), and the estimation of magnetic domains in the materials was conducted through magnetic force microscopy. Thus, the report suggests that readers, especially beginners, can gain a comprehensive understanding of the extensive prospects associated with the fundamental principles of material synthesis and characterization.

Topological regulations of Stone-Wales graphene

Designed synthesis of graphene-based materials containing Stone-Wales defects represents a promising strategy for graphene modification, because of their highly diverse structures and tunable properties. In graphene-based materials, Stone-Wales defects are caused by the in-plane atomic rearrangement and re-linkage of graphene's honeycomb structure. The resultant Stone-Wales graphene's are topoisomers of graphene. Topology is naturally a major factor in regulating the structures and properties of Stone-Wales graphene, but the regulation rules are mostly unclear. In this study, 478 low-energy Stone-Wales graphene allotropes with diverse topology are predicted using topology-based global optimization, for which the thermodynamic, electronic, and elastic properties are evaluated using the first-principles calculations. The dependencies of the predicated physical properties on topological quantities and patterns are explicitly determined. The current study may lay the groundwork for design, synthesis, and property tuning of graphene-based materials.

Quaternary Ammonium Assisted Synthesis of Melanin-like Poly(l-DOPA) Nanoparticles with a Boosted Photothermal Effect.

Poly(levodopa) nanoparticles (P(l-DOPA) NPs) are another kind of melanin mimetic besides well-established polydopamine nanoparticles (PDA NPs). Due to the presence of carboxyl groups, the oxidative polymerization of l-DOPA to obtain particles was not as efficient as that of dopamine. Several established methods toward P(l-DOPA) NP fabrication do not combine convenience, morphological regularity, size controllability, low cost, and adaptability to metal-free application scenarios. In this work, P(l-DOPA) NPs were successfully prepared in hot water with the assistant of organic quaternary ammonium, due to the extra physical cross-linking mediated by cations. The employed physical interactions could also be affected by quaternary ammonium structure (i.e., number of cation heads, length of alkyl chain) to achieve different polymerization acceleration effects. The obtained P(l-DOPA) NPs retained superior photothermal properties and outperformed PDA-based melanin materials. Furthermore, P(l-DOPA) NPs were used in photothermal tumor therapy and showed better efficacy. This study offers new insights into the synthesis of melanin-like materials, as well as new understanding of the interaction between quaternary ammonium and bioinspired polyphenolic materials.

Lattice engineering of high-entropy olivine-type lithium metal phosphate as high-voltage cathodes

Engineering of high-entropy cathode materials for lithium-ion batteries has been actively pursued owing to the outstanding conductivity of high-entropy materials benefited from the maximum entropy and unique antisite disordering structure. Olivine lithium metal phosphates such as LiMnPO4 and LiNiPO4 feature high working voltages but low capacities due to their insulation nature. In this work, the synthesis of the high-entropy lithium metal phosphate materials (HELMPs) is realized by combining mechanochemistry with a calcination method. By regulating lattice of HELMPs, the high-entropy Li(Mn0.35Fe0.35Co0.1Mg0.1Ca0.1)PO4 reveals three typical high-voltage plateaus in charge–discharge curves corresponding to the redox of Fe, Mn, and Co in the voltage range of 2.0–4.9 V vs Li+/Li, and a much higher initial capacity than LiMnPO4 (104 vs 15 mAh g−1).

Synthesis of hybrid materials containing H-ZSM-5 and CeO2 for green butadiene production

Synthesis of hybrid materials combining two or more components with different properties is a commonly used strategy to obtain high-performance materials for a wide range of different applications, including catalytic reactions with a complex reaction network. In this work, two synthesis approaches are investigated to prepare hybrid materials containing two well-defined phases, i.e. H-ZSM-5 and CeO2. By dispersing nano-sized H-ZSM-5 on CeO2, and by synthesizing a core-shell catalyst with a nano H-ZSM-5 core and a ceria shell, a high intimacy between H-ZSM-5 and CeO2 was obtained, while keeping the characteristic properties of each phase. The dehydration of 1,3-butanediol is used as a test reaction to explore the potential of these materials. A ratio between the selectivities of the desired product and intermediates, i.e. 1,3-butadiene (BD), 3-buten-2-ol (3B2OL), and 2-buten-1-ol (2B1OL) to the undesired product propylene (PP) was defined: (BD+3B2OL+2B1OL)/PP. Dispersing H-ZSM-5 zeolites on a CeO2 surface was the optimal synthesis route to enhance the 1,3-butadiene selectivity, and a (BD+3B2OL+2B1OL)/PP selectivity ratio was obtained (3.9) compared to its parent material (2.1).

Solution-Processable and Printable Two-Dimensional Transition Metal Dichalcogenide Inks.

Two-dimensional (2D) transition metal dichalcogenides (TMDs) with layered crystal structures have been attracting enormous research interest for their atomic thickness, mechanical flexibility, and excellent electronic/optoelectronic properties for applications in diverse technological areas. Solution-processable 2D TMD inks are promising for large-scale production of functional thin films at an affordable cost, using high-throughput solution-based processing techniques such as printing and roll-to-roll fabrications. This paper provides a comprehensive review of the chemical synthesis of solution-processable and printable 2D TMD ink materials and the subsequent assembly into thin films for diverse applications. We start with the chemical principles and protocols of various synthesis methods for 2D TMD nanosheet crystals in the solution phase. The solution-based techniques for depositing ink materials into solid-state thin films are discussed. Then, we review the applications of these solution-processable thin films in diverse technological areas including electronics, optoelectronics, and others. To conclude, a summary of the key scientific/technical challenges and future research opportunities of solution-processable TMD inks is provided.

Synthesis of Bio-Based Polyester Resins for Vat Photopolymerization 3D Printing.

Driven by environmental considerations, the scientific community has directed great effort towards the synthesis of new materials derived from renewable resources. However, for photocurable resins, most commercially available building blocks still rely on petroleum-based precursors. Herein, we present a simple synthesis route for bio-based acrylate-modified polyester resins, whose viscosity is sufficiently low for processing them with vat photopolymerization 3D printing. The established synthesis route enables the gradual substitution of fossil-based raw materials with bio-based alternatives. The acid number, color and viscosity of the bio-based acrylic resins are characterized and photocurable formulations are prepared by adding a radical photoinitiator. The photopolymerization kinetics, and thermomechanical and mechanical properties of the photopolymers are investigated as a function of the resin structure and benchmarked against a commercially available petroleum-based counterpart. Finally, the processability of the new bio-based resins via digital light processing 3D printing is demonstrated and test specimens are successfully 3D printed with a resolution in the millimeter range.

Electrochemical Generation of Te Vacancy Pairs in PtTe for Efficient Hydrogen Evolution.

Two-dimensional (2D) van der Waals materials are increasingly seen as potential catalysts due to their unique structures and unmatched properties. However, achieving precise synthesis of these remarkable materials and regulating their atomic and electronic structures at the most fundamental level to enhance their catalytic performance remain a significant challenge. In this study, we synthesized single-crystal bulk PtTe crystals via chemical vapor transport and subsequently produced atomically thin, large PtTe nanosheets (NSs) through electrochemical cathode intercalation. These NSs are characterized by a significant presence of Te vacancy pairs, leading to undercoordinated Pt atoms on their basal planes. Experimental and theoretical studies together reveal that Te vacancy pairs effectively optimize and enhance the electronic properties (such as charge distribution, density of states near the Fermi level, and d-band center) of the resultant undercoordinated Pt atoms. This optimization results in a significantly higher percentage of dangling O-H water, a decreased energy barrier for water dissociation, and an increased binding affinity of these Pt atoms to active hydrogen intermediates. Consequently, PtTe NSs featuring exposed and undercoordinated Pt atoms demonstrate outstanding electrocatalytic activity in hydrogen evolution reactions, significantly surpassing the performance of standard commercial Pt/C catalysts.

Synthesis, electricaland structural characterization of a composite material based on powdered magnetite and high density polyethylene

Garzón Posada A.O., F.E. Fajardo Tolosa, D.A. Landínez Téllez, J. Roa-Rojas, G. Peña Rodríguez. Synthesis, electrical and structural characterization of a composite material based on powdered magnetite and high density polyethylene. Rev. Acad. Colomb. Cienc., 37 (1): 55-59, 2013. ISSN 0370-3908. This work describes the synthesis and characterization of a composite material based on magnetite filled HDPE, which is comrnonly known for its magnetic properties. Composites of this kind are used in different applica­tions such as magnetic and microwave absorption, transducers manufacturing, and biomedical applications like targeted drug delivery, organs tagging, etc. The samples were produced according to different volume ratios of magnetite and HDPE. The samples structure was analyzed through X-ray diffraction tests and the crystallinity degree was calculated. Then, the samples were electrically characterized through volume resistivity measure­ments. The results showed that for ratios less than the 20% of magnetite there is not a substantial reduction in the resistivity ofthe composite compared to the unfilled HDPE. For magnetite ratios above the 30% the com­posite shows a substantial reduction of six orders of magnitude in its electrical resistivity.

Spent Lithium-Ion Batteries Derived Co3O4 for Electrocatalytic Polyethylene Terephthalate Plastic Recycling.

Spent lithium-ion batteries (LIBs) are an essential secondary resource containing valuable metal elements. Transforming spent LIBs into efficient catalysts through a simple process presents a promising strategy to address both metal resource scarcity and clean energy challenges. Herein, a deep eutectic solvent-assisted synthesis of Co3O4 material from spent LIBs is proposed. The obtained Co3O4 material possesses efficient and stable electrocatalytic activity for converting raw polyethylene terephthalate (PET) bottles into high-purity formic acid and terephthalic acid products under ambient conditions. As expected, the Co3O4 catalyst exhibits a high FE of 92 % with a concentration of produced potassium formate of 23.6 mM under alkaline conditions. This study presents a waste-treating-waste strategy for the simultaneous recovery of spent LIBs and PET waste in a greener manner.

Solution combustion synthesis of zinc and calcium aluminate spinel phase materials: optical and structural properties

Solution combustion synthesis of zinc and calcium aluminate spinel phase materials: optical and structural properties

Synthesis of near-infrared-activated YF3:Yb3+, Tm3+/Bi2MoO6 upconversion photocatalytic materials for the photocatalytic degradation of antibiotics based on fluorescence resonance energy transfer

Photocatalytic degradation of pollutants, an ecofriendly technology, is widely used for environmental remediation. However, the design and synthesis of photocatalytic materials for near-infrared light photocatalysis are challenging. In this study, an upconversion photocatalyst with fluorescence resonance energy transfer (FRET), YF3:Yb3+, Tm3+/Bi2MoO6 (YFYT/BMO), was developed and synthesised based on rare-earth upconversion luminescence. YFYT converted near-infrared (NIR) light into blue–violet light via upconversion. The rapid decay of the fluorescence lifetime of YFYT/BMO at 478 nm (Tm3+:1G4-3H6) verified that FRET efficiently occurred between YFYT and BMO. The degradation rate of tetracycline by YFYT/BMO was 2.6 times higher than that by BMO under NIR light. A great enhancement of 42.1 % on the tetracycline degradation efficiency was achieved in YFYT/BMO compared with pure BMO within 90 min of visible-NIR irradiation. This study provides a basis for developing and designing rare-earth upconversion photocatalytic materials that can achieve excellent photocatalytic degradation of antibiotics using NIR light for environmental remediation.

Using industrial waste in porous building materials for indoor humidity control

This study uses waste bricks and waste catalyst as raw materials in the synthesis of humidity control building materials with high structural strength. This paper explores the feasibility of producing porous humidity control materials (PHCM) through the billet sintering of waste brick with various quantities of waste catalyst (0 %–40 %) for indoor construction. N2 adsorption and desorption isotherms revealed that PHCM exhibits Type-IV adsorption with H3 hysteresis loops, indicating a network of interconnected mesopores with diameters ranging from 3 to 17 nm. Humidity control analysis revealed that increasing the waste catalyst content significantly enhanced the equilibrium moisture content and moisture adsorption and desorption capacity. This study determined that the adsorption of moisture within the PHCM relies on capillary condensation within the mesopores. Under 95 % relative humidity (RH), the highest equilibrium moisture content (2.97 kg/kg) and 12-h moisture adsorption capacity (72.41 g/m2) were obtained in specimens prepared at a sintering temperature of 1000 °C with a 40 % spent catalyst. This excellent adsorption capacity can be attributed to the high surface area of the waste catalyst, which increased the surface area of PHCM from 0.013 to 8.529 m2/g. This study demonstrates the benefits of synthesizing PHCM using waste bricks and catalysts in terms of porous properties, mechanical properties, and humidity control performance.

Magnetostatic waves in metallic rectangular waveguides filled with uniaxial negative permeability media

The propagation characteristics of magneto-quasistatic waves, more commonly, known as magnetostatic waves in a long, metallic rectangular waveguide filled with a metamaterial slab are comprehensively investigated. The metamaterial slab consists of split-ring resonators as an anisotropic uniaxial medium with transversal negative effective permeability. Some analytical relations and numerical validations on the characteristics of these waves are presented. The results include the dispersion relations, mode patterns (field distributions) that can be supported by such media, and their corresponding cutoff frequencies, group velocities, power flows, and storage energies of magnetostatic waves. The findings from the present research study can be advantageous to advance the synthesis and development of negative permeability materials with peculiar features in guiding structures.