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1.
Materials (Basel) ; 17(13)2024 Jun 21.
Article in English | MEDLINE | ID: mdl-38998151

ABSTRACT

This work focuses in-depth on the quantitative relationships between primary first-order microstructural parameters (i.e., volume fractions of various phases and particle size distribution) with the more complex second-order topological features (i.e., connectivity of phases, three-phase boundary length (TPBL), interfacial areas, or tortuosity). As a suitable model material, a cermet nickel/samaria-doped ceria (Ni-SDC) is used as an anode in a solid oxide fuel cell (SOFC). A microstructure description of nano-sized Ni-SDC cermets, fabricated at various sintering conditions from 1100 °C to 1400 °C, was performed using FIB-SEM nanotomography. The samples were serially sectioned employing a fully automated slicing procedure with active drift correction algorithms and an auto-focusing routine to obtain a series of low-loss BSE images. Advanced image processing algorithms were developed and applied directly to image data volume. The microstructural-topological relationships are crucial for the microstructure optimisation and, thus, the improvement of the corresponding electrode performance. Since all grains of individual phases (Ni, SDC, or pores) did not percolate, special attention was given to the visualisation of the so-called active TPBL. Based on the determined microstructure characteristics of the prepared Ni-SDC cermets, including simulations of gas flow and pressure drop, thermal treatment at 1200 °C was recognised as the most appropriate sintering temperature.

3.
Sci Rep ; 14(1): 9234, 2024 Apr 22.
Article in English | MEDLINE | ID: mdl-38649471

ABSTRACT

In this study, we introduce a novel approach using correlative analysis techniques to unravel detailed insights into the environmental influences on crystal growth. Tabular and bipyramidal wulfenite samples from the Mezica mine in north-eastern Slovenia were analysed to combine the morphological aspects of crystal growth with the atomic-resolution reconstruction of the positions of lead (Pb) and molybdenum (Mo) atoms in the parent crystal lattice. These combined data also allow us to present the formation mechanism that enables the development of bipyramidal or tabular morphologies in wulfenite. The bipyramidal and tabular crystals are chemically pure wulfenite (PbMoO4), as confirmed by various advanced diffraction and spectroscopy techniques. However, each habit includes multiple inclusions, mostly consisting of carbonates, Pb-Fe oxides, Pb oxides and, more rarely, Pb vanadate (descloizite). The differences in the morphologies can be attributed to compositional changes during precipitation from a meteoric solution and thus, we propose a growth mechanism consisting of three different phases of growth. This innovative approach emphasises the importance of understanding the origin of crystal habits, as can help to decipher how external influences can affect the crystal structure and its surface, leading to the dissolution of preferred surfaces and the selective release of Pb and Mo.

4.
Materials (Basel) ; 17(4)2024 Feb 09.
Article in English | MEDLINE | ID: mdl-38399099

ABSTRACT

In this review article, we focus on the relationship between permanent magnets and the electric motor, as this relationship has not been covered in a review paper before. With the increasing focus on battery research, other parts of the electric system have been neglected. To make electrification a smooth transition, as has been promised by governing bodies, we need to understand and improve the electric motor and its main component, the magnet. Today's review papers cover only the engineering perspective of the electric motor or the material-science perspective of the magnetic material, but not both together, which is a crucial part of understanding the needs of electric-motor design and the possibilities that a magnet can give them. We review the road that leads to today's state-of-the-art in electric motors and magnet design and give possible future roads to tackle the obstacles ahead and reach the goals of a fully electric transportation system. With new technologies now available, like additive manufacturing and artificial intelligence, electric motor designers have not yet exploited the possibilities the new freedom of design brings. New out-of-the-box designs will have to emerge to realize the full potential of the new technology. We also focus on the rare-earth crisis and how future price fluctuations can be avoided. Recycling plays a huge role in this, and developing a self-sustained circular economy will be critical, but the road to it is still very steep, as ongoing projects show.

5.
Materials (Basel) ; 16(19)2023 Oct 05.
Article in English | MEDLINE | ID: mdl-37834702

ABSTRACT

The green transition initiatives and exploitation of renewable energy sources require the sustainable development of rare earth (RE)-based permanent magnets prominent technologies like wind turbine generators and electric vehicles. The recycling of RE-based permanent magnets is necessary for the future supply of critical rare-earth elements. The short-loop recycling strategies to directly reprocess Nd-Fe-B magnet waste are economically attractive and practical alternatives to conventional hydro- and pyrometallurgical processes. This study focuses on the development of a procedure to extract the (Nd, Pr)2Fe14B hard-magnetic phase from sintered Nd-Fe-B magnets. The extraction is achieved through preferential chemical leaching of the secondary, RE-rich phases using 1 M citric acid. Before the acid treatment, the magnets were pulverized through hydrogen decrepitation (HD) to increase the material's surface-to-volume ratio. The as-pulverized Nd-Fe-B powder was subsequently exposed to a 1 M citric acid solution. The effect of leaching time (5-120 min) on the phase composition and magnetic properties was studied. The results of the microstructural (SEM) and compositional (ICP-MS) analyses and the study of thermal degassing profiles revealed that the RE-rich phase is preferentially leached within 5-15 min of reaction time. Leaching of the secondary phases from the magnet's multi-phase microstructure is governed by the negative electrochemical potential of Nd and Pr. The extraction of (Nd, Pr)2Fe14B grains by the proposed acid leaching approach is compatible with the existing hydrogen processing of magnetic scrap (HPMS) technologies. The use of mild organic acid as a leaching medium makes the leaching process environmentally friendly, as the leaching medium can be easily neutralized after the reaction is completed.

6.
Materials (Basel) ; 16(14)2023 Jul 23.
Article in English | MEDLINE | ID: mdl-37512455

ABSTRACT

The green transition initiative has exposed the importance of effective recycling of Nd-Fe-B magnets for achieving sustainability and foreign independence. In this study, we considered strip-cast, hydrogenated, jet-milled Nd-Fe-B powder as a case study to explore the potential for selective chemical leaching of the Nd-rich phase, aiming to extract the Nd2Fe14B matrix phase. Diluted citric and nitric acids at concentrations of 0.01, 0.1, and 1 M were considered potential leaching mediums, and the leaching time was 15 min. Microstructural investigation, magnetic characterization, and elemental compositional analysis were performed to investigate leaching efficiency and selectivity. Based on SEM analysis, Nd/Fe ratio monitoring via ICP-MS, and the high moment/mass value at 160 emu/g for the sample leached with 1 M citric acid, 1 M citric acid proved highly selective toward the Nd-rich phase. Exposure to nitric acid resulted in a structurally damaged Nd2Fe14B matrix phase and severely diminished moment/mass value at 96.2 emu/g, thus making the nitric acid unsuitable for selective leaching. The presence of hydrogen introduced into the material via the hydrogen decrepitation process did not notably influence the leaching dynamics. The proposed leaching process based on mild organic acids is environmentally friendly and can be scaled up and adopted for reprocessing industrial scrap or end-of-life Nd-Fe-B magnets to obtain single-phase Nd-Fe-B powders that can be used for novel magnet-making.

7.
Sensors (Basel) ; 23(10)2023 May 11.
Article in English | MEDLINE | ID: mdl-37430588

ABSTRACT

Simple, low-cost methods for sensing volatile organic compounds that leave no trace and do not have a detrimental effect on the environment are able to protect communities from the impacts of contaminants in water supplies. This paper reports the development of a portable, autonomous, Internet of Things (IoT) electrochemical sensor for detecting formaldehyde in tap water. The sensor is assembled from electronics, i.e., a custom-designed sensor platform and developed HCHO detection system based on Ni(OH)2-Ni nanowires (NWs) and synthetic-paper-based, screen-printed electrodes (pSPEs). The sensor platform, consisting of the IoT technology, a Wi-Fi communication system, and a miniaturized potentiostat can be easily connected to the Ni(OH)2-Ni NWs and pSPEs via a three-terminal electrode. The custom-made sensor, which has a detection capability of 0.8 µM/24 ppb, was tested for an amperometric determination of the HCHO in deionized (DI) and tap-water-based alkaline electrolytes. This promising concept of an electrochemical IoT sensor that is easy to operate, rapid, and affordable (it is considerably cheaper than any lab-grade potentiostat) could lead to the straightforward detection of HCHO in tap water.

8.
Inorg Chem ; 62(15): 6169-6180, 2023 Apr 17.
Article in English | MEDLINE | ID: mdl-37022922

ABSTRACT

We have determined the crystal structure and the magnetic state of the CeFe9Si4 intermetallic compound. Our revised structural model (fully ordered tetragonal unit cell, I4/mcm) agrees with the previous literature report, except for some minor quantitative differences. Magnetically, the CeFe9Si4 undergoes a ferromagnetic transition at the temperature TC ≈ 94 K. Ferromagnetism in the combined Ce-Fe spin system is a result of interplay between the localized magnetism of the Ce sublattice and the Fe band (itinerant) magnetism. Ferromagnetic ordering obeys the rather general rule that the exchange spin coupling between atoms possessing more than half-full d shells with atoms possessing less than half-full d shells is antiferromagnetic (where the Ce atoms are considered as light d elements). Since in rare-earth metals from the light half of the lanthanide series, the magnetic moment is directed opposite to the spin, this results in ferromagnetism. The magnetoresistance and the magnetic specific heat show an additional temperature-dependent feature (a shoulder) deep inside the ferromagnetic phase that is considered to originate from the influence of the magnetization on the electronic band structure via the magnetoelastic coupling, which alters the Fe band magnetism below TC. The ferromagnetic phase of CeFe9Si4 is magnetically soft.

9.
Materials (Basel) ; 15(22)2022 Nov 19.
Article in English | MEDLINE | ID: mdl-36431710

ABSTRACT

The effect of Ni/Cu-coating residuals on the magnetic properties and microstructures of samarium-cobalt (SmCo5) magnets was studied. SmCo5 magnets with 0.0, 0.5, 1.0, 2.0, 3.0 and 4.0 wt.% of added Ni/Cu (85 wt.% Ni/15 wt.% Cu) were prepared using a conventional sintering route. The magnetic properties of the magnets were found to be consistent up to 2 wt.% Ni/Cu. Any further increase in the Ni/Cu content resulted in a significant reduction in the magnetic properties, to lower than values that would be commercially acceptable. SEM/EDS studies showed that two major phases, i.e., the SmCo5 matrix phase and Sm2O3 were present in all the sintered SmCo5 magnets. The presence of Sm2Co7 as a minor phase fraction was detected in the sintered SmCo5 magnets containing up to 2 wt.% Ni/Cu. A 2 wt.% Ni/Cu addition to magnets resulted in the presence of two new phases with compositions close to SmCo and Sm2Co17 in addition to SmCo5 and Sm2O3 as major phases in the SEM-observed microstructure. These newly formed phases are present in small fractions and are presumably homogenously distributed at the grain boundaries of the magnets. As they are known to act as nucleation sites for reverse magnetic domains, they effectively reduce the intrinsic grain boundary magnetic strength, leading to a drop in the coercivity. We concluded that the sintered SmCo5 magnets could be recycled with up to 2 wt.% Ni/Cu as a residual from the coating under our sintering and heat treatment conditions.

10.
Inorg Chem ; 61(23): 8823-8833, 2022 Jun 13.
Article in English | MEDLINE | ID: mdl-35635510

ABSTRACT

A binary phase with Al4Ir composition has been discovered in the Al-Ir binary system. Single-crystal X-ray diffraction analysis reveals that it crystallizes in the trigonal space group P3c1 with the unit cell parameters a = 12.8802(2) Å and c = 9.8130(2) Å. This structure is derived from the Ni2Al3 structure type. The supercell is due to the ordering of the aluminum atoms, which replace the nickel atoms in the prototype structure. The crystal structure was directly imaged by atomic-scale scanning transmission electron microscopy, and the misalignment of the Al site responsible for the supercell has been clearly evidenced. Its metastable nature has been confirmed by differential thermal analysis measurements. The atomic and electronic structures of Al4Ir have also been investigated by density functional theory. The structural optimization leads to lattice parameters and atomic positions in good agreement with the experimental ones. The compound is metallic, with a minimum in the density of states located more than 1 eV above the Fermi energy. This suggests a metastable system, in agreement with the electron count found much above 18 electrons per Ir atom, deviating from the Hume-Rothery rule and with the presence of occupied antibonding states revealed by the crystal orbital Hamiltonian population analysis. The relative stability of the compound is ensured by the hybridization between sp-Al and d-Ir states within Ir-centered clusters, while covalent-like interactions in-between the clusters are indicated by the analysis of the electron localizability function.

11.
Materials (Basel) ; 15(9)2022 Apr 24.
Article in English | MEDLINE | ID: mdl-35591427

ABSTRACT

The main objective of the study was to produce alternative binder materials, obtained with low cost, low energy consumption, and low CO2 production, by regenerating end-of-life (EOL) materials from mineral deposits, to replace ordinary Portland cement (OPC). The materials analyzed were ash and slag from the Turceni thermal power plant deposit, Romania. These were initially examined for morphology, mineralogical composition, elemental composition, degree of crystallinity, and heating behavior, to determine their ability to be used as a potential source of supplementary cementitious materials (SCM) and to establish the activation and transformation temperature in the SCM. The in-situ pozzolanic behavior of commercial cement, as well as cement mixtures with different percentages of ash addition, were further observed. The mechanical resistance, water absorption, sorptivity capacity, resistance to alkali reactions (ASR), corrosion resistance, and resistance to reaction with sulfates were evaluated in this study using low-vacuum scanning electron microscopy.

12.
Pharmaceutics ; 14(4)2022 Mar 22.
Article in English | MEDLINE | ID: mdl-35456523

ABSTRACT

Despite medical advances, skin-associated disorders continue to pose a unique challenge to physicians worldwide. Skin cancer is one of the most common forms of cancer, with more than one million new cases reported each year. Currently, surgical excision is its primary treatment; however, this can be impractical or even contradictory in certain situations. An interesting potential alternative could lie in topical treatment solutions. The goal of our study was to develop novel multilayer nanofilms consisting of a combination of polyhydroxyethyl methacrylate (PHEMA), polyhydroxypropyl methacrylate (PHPMA), sodium deoxycholate (NaDOC) with incorporated superparamagnetic iron-platinum nanoparticles (FePt NPs), and the potent anticancer drug (5-fluorouracil), for theranostic skin cancer treatment. All multilayer systems were prepared by spin-coating and characterised by atomic force microscopy, infrared spectroscopy, and contact angle measurement. The magnetic properties of the incorporated FePt NPs were evaluated using magnetisation measurement, while their size was determined using transmission electron microscopy (TEM). Drug release performance was tested in vitro, and formulation safety was evaluated on human-skin-derived fibroblasts. Finally, the efficacy for skin cancer treatment was tested on our own basal-cell carcinoma cell line.

13.
Nanomaterials (Basel) ; 11(4)2021 Apr 03.
Article in English | MEDLINE | ID: mdl-33916739

ABSTRACT

Photothermal therapy has always been a very attractive anti-cancer strategy, drawing a lot of attention thanks to its excellent performance as a non-invasive and pretty safe technique. Lately, nanostructures have become the main characters of the play of cancer therapy due to their ability to absorb near-infrared radiation and efficient light-to-heat conversion. Here we present the synthesis of polyethylene glycol (PEG)-stabilized hybrid ultrasmall (<20 nm) gold-silver nanotriangles (AuAgNTrs) and their application in photothermal therapy. The obtained AuAgNTrs were deeply investigated using high-resolution transmission electron microscopy (HR-TEM). The cell viability assay was performed on U-87 glioblastoma multiforme cell model. Excellent photothermal performance of AuAgNTrs upon irradiation with NIR laser was demonstrated in suspension and in vitro, with >80% cell viability decrease already after 10 min laser irradiation with a laser power P = 3W/cm2 that was proved to be harmless to the control cells. Moreover, a previous cell viability test had shown that the nanoparticles themselves were reasonably biocompatible: without irradiation cell viability remained high. Herein, we show that our hybrid AuAgNTrs exhibit very exciting potential as nanostructures for hyperthermia cancer therapy, mostly due to their easy synthesis protocol, excellent cell compatibility and promising photothermal features.

14.
Data Brief ; 32: 106203, 2020 Oct.
Article in English | MEDLINE | ID: mdl-32904307

ABSTRACT

Three phases can be distinguished in Nd‒Fe‒B permanent magnets: a Nd2Fe14B matrix grain phase, a Nd-rich grain boundary phase and a Nd-oxide phases. Common reaction models for leaching, such as the shrinking-particle model, cannot simply be applied to composite Nd‒Fe‒B permanent magnets because of the different chemical reactivities of the crystalline phases mentioned above. Etching the surface of a Nd‒Fe‒B magnet to expose its microstructure to electron microscopy is a necessary practice to correlate the microstructure itself to the specific properties of the magnets. Aqueous solutions of mineral acids are often used for etching purposes. However, these solutions are too low viscous to easily control the etching front and they show little selectivity in the etching process. In our work, the ionic liquid Cyphos IL 101 was used to etch bulk magnets instead of aqueous HCl solutions. The bulk Nd‒Fe‒B magnets were first polished, then exposed to a solution of 3 M HCl in Cyphos IL 101 for different times and at different temperatures. Afterwards, the etched Nd‒Fe‒B magnets were washed with ethanol and acetone. The results were examined via scanning-electron microscopy and image analysis. A commercial software, ImageJ®, was employed for image analysis. The latter technique was used to correlate the etched area (%area) or the grain and oxide size to the etching temperature or the etching time. The grain or the oxide size were calculated as Feret diameter. Image analysis revealed to be a necessary tool to support and correct the findings first suggested by the simple scanning-electron microscopy. The data presented in this article might be reused to corroborate a new reactivity order of the three Nd‒Fe‒B phases, different from that traditionally reported in literature, which is - from the most to the least reactive - grain boundary > oxides > the Nd2Fe14B grain phase.

15.
Materials (Basel) ; 13(8)2020 Apr 22.
Article in English | MEDLINE | ID: mdl-32331388

ABSTRACT

A sustainable solution for the global construction industry can be partial substitution of Ordinary Portland Cement (OPC) by use of supplementary cementitious materials (SCMs) sourced from industrial end-of-life (EOL) products that contain calcareous, siliceous and aluminous materials. Candidate EOL materials include fly ash (FA), silica fume (SF), natural pozzolanic materials like sugarcane bagasse ash (SBA), palm oil fuel ash (POFA), rice husk ash (RHA), mine tailings, marble dust, construction and demolition debris (CDD). Studies have revealed these materials to be cementitious and/or pozzolanic in nature. Their use as SCMs would decrease the amount of cement used in the production of concrete, decreasing carbon emissions associated with cement production. In addition to cement substitution, EOL products as SCMs have also served as coarse and also fine aggregates in the production of eco-friendly concretes.

16.
Sensors (Basel) ; 21(1)2020 Dec 29.
Article in English | MEDLINE | ID: mdl-33383812

ABSTRACT

Polyaniline (PANI) is a conducting polymer, widely used in gas-sensing applications. Due to its classification as a semiconductor, PANI is also used to detect reducing ammonia gas (NH3), which is a well-known and studied topic. However, easier, cheaper and more straightforward procedures for sensor fabrication are still the subject of much research. In the presented work, we describe a novel, more controllable, synthesis approach to creating NH3 PANI-based receptor elements. The PANI was electrochemically deposited via cyclic voltammetry (CV) on screen-printed electrodes (SPEs). The morphology, composition and surface of the deposited PANI layer on the Au electrode were characterised with electron microscopy, Fourier-transform infrared spectroscopy and profilometry. Prior to the gas-chamber measurement, the SPE was suitably modified by Au sputtering the individual connections between the three-electrode system, thus showing a feasible way of converting a conventional three-electrode electrochemical SPE system into a two-electrode NH3-gas detecting system. The feasibility of the gas measurements' characterisation was improved using the gas analyser. The gas-sensing ability of the PANI-Au-SPE was studied in the range 32-1100 ppb of NH3, and the sensor performed well in terms of repeatability, reproducibility and sensitivity.

17.
Inorg Chem ; 59(1): 360-366, 2020 Jan 06.
Article in English | MEDLINE | ID: mdl-31859489

ABSTRACT

A new ternary phase with a composition Al1+xV2Sn2-x (x = 0.19) has been found during investigation of the Al-V-Sn ternary system. Single-crystal X-ray diffraction measurements reveal that this ternary phase crystallizes with an orthorhombic structure with a = 5.5931(1) Å, b = 18.8017(5) Å, and c = 6.7005(2) Å (space group Cmce). This compound is thus isostructural to the GaV2Sn2 structure type, showing a layered structure composed of vanadium cluster bands formed with pentagonal faces intercalated by Sn atom layers. High-resolution transmission electron microscopy measurements confirm the orthorhombic structure. Regarding lattice perfection, no dislocation could be identified within the probed Al1.19V2Sn1.81 single-crystal lamella. Ab initio calculations reveal a reduction of the density of states at the Fermi level, which could be attributed to both a Hume-Rothery effect combined with strong spd hybridization.

18.
ChemSusChem ; 12(21): 4754-4758, 2019 Nov 08.
Article in English | MEDLINE | ID: mdl-31529776

ABSTRACT

Recycling of end-of-life Nd-Fe-B magnets is an important strategy for reducing the environmental dangers associated with rare-earth mining and overcoming the supply risks associated with the rare-earth elements. In this study, a novel concept for recycling of sintered Nd-Fe-B magnets by directly recovering the matrix Nd2 Fe14 B grains is presented. The procedure is based on the anodic etching of sintered Nd-Fe-B magnets in a nonaqueous dimethylformamide (DMF)/0.3 mol L-1 FeCl2 bath. Selective recovery of Nd2 Fe14 B grains was realized within the applied current density <5 mA cm-2 based on the etching priority of phases: metallic Nd > intergranular NdFe4 B4 > matrix Nd2 Fe14 B. The total energy consumption of the proposed recycling route is estimated to be 2.99 kWh kg-1 , which is comparable to the state-of-the-art methods. However, the proposed recycling route is currently the only procedure that enables repeated recycling of sintered Nd-Fe-B magnets in a closed-loop system.

19.
Materials (Basel) ; 12(9)2019 May 08.
Article in English | MEDLINE | ID: mdl-31071992

ABSTRACT

The magnetic properties of the recycled hydrogenation disproportionation desorption recombination (HDDR) Nd-Fe-B powder, doped with a low weight fraction of DyF3 nanoparticles, were investigated. Spark plasma sintering (SPS) was used to consolidate the recycled Nd-Fe-B powder blends containing 1, 2, and 5 wt.% of DyF3 grounded powder. Different post-SPS sintering thermal treatment conditions (600, 750, and 900 °C), for a varying amount of time, were studied in view of optimizing the magnetic properties and developing characteristic core-shell microstructure in the HDDR powder. As received, recycled HDDR powder has coercivity (HCi) of 830 kA/m, and as optimally as SPS magnets reach 1160 kA/m, after the thermal treatment. With only 1-2 wt.% blended DyF3, the HCi peaked to 1407 kA/m with the thermal treatment at 750 °C for 1 h. The obtained HCi values of the blend magnet is ~69.5% higher than the starting recycled HDDR powder and 17.5% higher than the SPS processed magnet annealed at 750 °C for 1 h. Prolonging the thermal treatment time to 6 h and temperature conditions above 900 °C was detrimental to the magnetic properties. About ~2 wt.% DyF3 dopant was suitable to develop a uniform core-shell microstructure in the HDDR Nd-Fe-B powder. The Nd-rich phase in the HDDR powder has a slightly different and fluorine rich composition i.e., Nd-O-F2 than in the one reported in sintered magnets (Nd-O-F). The composition of reaction zone-phases after the thermal treatment and Dy diffusion was DyF4, which is more abundant in 5 wt.% doped samples. Further doping above 2 wt.% DyF3 is ineffective in augmenting the coercivity of the recycled HDDR powder, due to the decomposition of the shell structure and formation of non-ferromagnetic rare earth-based complex intermetallic compounds. The DyF3 doping is a very effective single step route in a controlled coercivity improvement of the recycled HDDR Nd-Fe-B powder from the end of life magnetic products.

20.
Chem Sci ; 10(38): 8735-8743, 2019 Oct 14.
Article in English | MEDLINE | ID: mdl-32133124

ABSTRACT

With Liquid-Cell Transmission Electron Microscopy (LCTEM) we can observe the kinetic processes taking place in nanoscale materials that are in a solvated environment. However, the beam-driven solvent radiolysis, which results from the microscope's high-energy electron beam, can dramatically influence the dynamics of the system. Recent research suggests that radical-induced redox chemistry can be used to investigate the various redox-driven dynamics for a wide range of functional nanomaterials. In view of this, the interplay between the formation of various highly reactive radiolysis species and the nanomaterials under investigation needs to be quantified in order to formulate new strategies for nanomaterials research. We have developed a comprehensive radiolysis model by using the electron-dose rate, the temperature of the solvent, the H2 and O2 gas saturation concentrations and the pH values as the key variables. These improved kinetic models make it possible to simulate the material's specific radical-induced redox reactions. As in the case of the Au model system, the kinetic models are presented using Temperature/Dose-rate Redox potential (TDR) diagrams, which indicate the equilibrium [Au0]/[Au+] concentration ratios that are directly related to the temperature-/dose-rate-dependent precipitation or dissolution regions of the Au nanoparticles. Our radiolysis and radical-induced redox models were successfully verified using previously reported data from low-dose experiments with γ radiation and experimentally via TDR-dependent LCTEM. The presented study represents a holistic approach to the radical-induced redox chemistry in LCTEM, including the complex kinetics of the radiolysis species and their influence on the redox chemistry of the materials under investigation, which are represented here by Au nanoparticles.

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