Charge Transfer Process Research Articles

Factors Affecting the Population of Excited Charge Transfer States in Adenine/Guanine Dinucleotides: A Joint Computational and Transient Absorption Study

There is compelling evidence that the absorption of low-energy UV radiation directly by DNA in solution generates guanine radicals with quantum yields that are strongly dependent on the secondary structure. Key players in this unexpected phenomenon are the photo-induced charge transfer (CT) states, in which an electric charge has been transferred from one nucleobase to another. The present work examines the factors affecting the population of these states during electronic relaxation. It focuses on two dinucleotides with opposite orientation: 5′-dApdG-3′ (AG) and 5′-dGpdA-3′ (GA). Quantum chemistry calculations determine their ground state geometry and the associated Franck–Condon states, map their relaxation pathways leading to excited state minima, and compute their absorption spectra. It has been shown that the most stable conformer is anti-syn for AG and anti-anti for GA. The ground state geometry governs both the excited states populated upon UV photon absorption and the type of excited state minima reached during their relaxation. Their fingerprints are detected in the transient absorption spectra recorded with excitation at 266 nm and a time resolution of 30 fs. Our measurements reveal that in the large majority of dinucleotides, chromophore coupling is already operative in the ground state and that the charge transfer process occurs within ~120 fs. The competition among various relaxation pathways affects the quantum yields of the CT state formation in each dinucleotide, which are estimated to be 0.18 and 0.32 for AG and GA, respectively.

Rational design of 1, 2, 4, 5-tetraphenyl-1H-imidazole-based AIEgens with tunable intramolecular charge transfer and restricted intramolecular rotation processes for multifunctional sensing

Aggregation-induced emission fluorogens (AIEgens) with intramolecular charge transfer (ICT) characteristic are widely used in the detection of various analytes owing to their highly tunable fluorescence emission properties. However, facilely synthesis of AIEgens with ICT characteristic for multiple sensing is still rare and limited in use. In this work, two new AIEgens of 1,2-bis(4-alkoxycarbonylphenyl)-4,5-bis(4-methoxyphenyl)-1H-imidazole (AMI) and its hydrolyzed derivative 1,2-bis(4-carboxylphenyl)-4,5-bis(4-methoxyphenyl)-1H-imidazole (CMI) were facilely synthesized with donor-π-acceptor (D-π-A) structures. The tunable ICT and restricted intramolecular rotation (RIR) processes endow them multifunctional sensing performances. AMI could serve as a reversible fluorescent thermometer, in which a positive linear correlation between fluorescence intensities and temperatures from 20 °C to 60 °C was obtained. Meanwhile, owning to the specific interaction between carboxyl groups and Al(III) ions, CMI was successfully served as a “turn-on” fluorescent chemosensor for detecting Al(III) in aqueous solutions under a neutral condition with high sensitivity and selectivity. Mechanism study showed that the formation of aggregation states of coordination polymers between CMI and Al(III) was responsible for the fluorescence enhancement. What is more, the sensing process could be applied for detecting Al(III) in real water samples and on solid test papers, which implied its potential application values. Furthermore, the aggregation-induced emission (AIE) characteristic also made fluorescence emissions of CMI suitable for specific pH sensing. This work provides an efficient strategy for the construction of multifunctional fluorescence chemosensors based on AIEgens.

Eletrochemical evaluation of a sensor modified with tucumã biochar for analysis of environmental samples

In this study, a carbon paste electrode modified with tucumã biochar (EPCM/TB) was produced for the determination of pyridine in industrial effluents. To develop the methodology, different paste proportions were evaluated, and a proportion of 40:30:30 (m/m/m) of graphite:tucumã biochar:binder was selected. Cyclic voltammetry was used to characterize the charge and mass transfer process of the electrochemical system; the reaction occurred with the transfer of two electrons. The reaction was irreversible and controlled by diffusion. The experimental variables such as the supporting electrolyte, pH and instrumental parameters of the differential pulse voltammetry (DPV) technique were evaluated. After the optimization of these parameters, four analytical curves were constructed using DPV to calculate the matrix effect (ME). The analytical curves in the presence of the matrix showed good linearity for the three effluents, with R2 values of 0.991, 0.997 and 0995. The limits of detection (LODs) for effluents 1, 2 and 3 were 34.9, 5.5 and 36.8 nmol/L, respectively. The limits of quantification (LOQs) for effluents 1, 2 and 3 were 116.6 nmol/L, 18.4 nmol/L and 122.6 nmol/L, respectively. The MEs of the three effluent samples showed values above 50.0 %, indicating strong MEs; therefore, the quantification of pyridine was performed using the matrix curves. The method had recoveries close to 100 % for the three effluents. The repeatability and reproducibility studies of the method provided RSD% values below 5 %; therefore, the method has potential application in the quantification of pyridine in textile effluents.

Turning Waste into Treasure: Utilizing Environment-Pollutant Graphite Tailings as Photocatalyst for Photocatalytic Building Materials

Graphite tailings, as solid waste residuals from graphite extraction and refinement, pose serious risks to the surrounding ecological environment and the safety of residents’ lives. However, it is desirable but challenging how to rationalize the utilization of graphite tailings and further to develop their functionality. Herein, we demonstrate a "turning waste into treasure" strategy: capitalizing on the characteristics of graphite tailings in visible light absorption and rich metal catalytic sites, graphite tailings are employed as photocatalysts and fine aggregates to manufacture photocatalytic building materials, achieving sustainable use. Tailings powder from Luobei, Heilongjiang Province is selected as the photocatalyst, we discover that it exhibits photocatalytic degradation capability for methylene blue (MB) in water under visible-light irradiation: the degradation rates reach 70% within one hour and near-complete degradation within two hours, accompanying good recyclability. Structural analysis reveals that the graphite tailings are enriched with Fe2O3 and TiO2. They are capable of forming type-II heterojunction that enable efficient charge separation and transfer processes, transmitting photogenerated electrons to the active catalytic site to accomplish the photocatalytic degradation of MB. Moreover, other tailings, such as those from Jixi, also achieve photocatalytic degradation of MB, and cement specimens made with graphite tailings also bespoke photocatalytic degradation performance. This work is to provide solutions for the reuse of graphite tailings in the field of functional building materials, and to explore the feasibility of transforming graphite tailings from industrial solid waste to photocatalytic building materials.

A novel electrochemical high-performance non-enzymatic glucose sensing based on face-centred cubic FeCoNiMnCr high entropy nano alloys encapsulated in NCNTs

Here, we report a novel approach for non-enzymatic glucose sensing, utilizing a FeCoNiMnCr High Entropy Nano Alloy (HENA) encapsulated within N-doped carbon nanotubes (NCNT). The encapsulation of HENA within NCNT offers multiple advantages such as high sensitivity, low Limit of Detection (LOD), and fast response time. A step forward, the practical viability of the sensor has been demonstrated by detecting glucose in saliva medium. This non-invasive method for monitoring blood sugar levels highlights the potential of HENA@NCNT for wearable or portable glucose monitoring devices. The material also serves as a highly effective electrocatalyst for the oxygen evolution reaction (OER), with performance comparable to state-of-the-art catalyst RuO2. This makes HENA@NCNT a promising candidate for fuel cell applications and other energy storage systems. Density Functional Theory (DFT) analysis provides a deeper understanding of the advantages conferred by NCNT encapsulation. The encapsulation enhances the stability, efficiency, and durability of HENA by optimizing electronic structure and charge transfer processes making it more effective for both glucose sensing and OER

Jackfruit waste derived oxygen-self-doped porous carbon for aqueous Zn-ion supercapacitors

To fully harness the benefits of high energy density, strategic fabrication of hierarchical porous carbon (PC) materials is essential and highly impactful. In this study, oxygen-self-doped PC materials are synthesized from jackfruit waste (JK) through pyrolysis combined with chemical activation. The resulting material (JKPC-4) features abundant interfacial active sites and a short ions/electrons transfer distance, enhancing the ion adsorption capacity and kinetic behavior of the cathode. Additionally, the oxygen-rich functional groups contribute to increased pseudocapacitance and enhance the wettability and conductivity of the material. Consequently, the assembled JKPC-4//JKPC-4 symmetric supercapacitor in 2M Na2SO4 electrolyte exhibits a high energy density of 36.06 Wh kg−1 at 647.94 W kg−1. Furthermore, the JKPC-4//Zn device demonstrates a notable capacity of 225 mAh g−1 at 0.1 A g−1, exceptional rate capability (93 mAh g−1 at 10 A g−1), high energy density (154 Wh kg−1), and impressive cycle stability, retaining 97 % of its capacity after 10,000 cycles at 10 A g−1. The electrochemical process is studied using ex-situ characterization. Mechanistic studies have shown that the outstanding energy storage capability and charge-transfer processes of JKPC-4 stem from the synergistic interplay between oxygen heteroatoms and suitable pore structure.

Plasma Power Effect to the Structure and Morphology of Strontium Stannate Thin Film

Hybrid p-n heterojunction requires a suitable n-type material to support the charge transfer process in photodiode or solar cell applications. Numerous materials have been researched in terms of wet and dry processes. This paper investigated the effect of varied plasma power levels of 50 W, 80 W and 100 W at room temperature on the structure and morphology of an alkaline-earth-based perovskite oxide thin film. Strontium stannate (SrSnO3) thin films are deposited on an indium tin oxide (ITO) substrate using radio frequency (RF) magnetron sputtering at various power levels. The crystallographic orientation of the thin films was examined and it was observed that the (102) plane exhibited dense growth at low power, while the (002) plane showed increased intensity at higher power levels. Additionally, the increase in RF power resulted in larger crystallite and grain sizes, along with modified grain boundaries. Contrarily, surface roughness, resistivity, macrostrain and work adhesion were reduced. The nearly zero W-H linear fitting plot observed at 80 W can serve as a valuable reference for the fabrication of preferred films. These findings provide valuable insights for optimising the growth conditions of alkaline-earth-based perovskite oxide thin films for various applications.

A theoretical comprehension of photophysical processes in Cu2+ sensing by 1,7-di(2-pyridyl)bispyrazolo[3,4-b:4′,3′-e]pyridines

Due to its simplicity and sensitivity, metal ion sensing by fluorescent probes has a high biological and ecological impact, and several preliminary applications for Cu2+ have been found. However, the poor understanding of photophysical phenomena by which probes work has led to the growth of unhelpful literature. In this way, 4-aryl-1,7-di(pyridin-2-yl)bispyrazolo[3,4-b:4′,3′-e]pyridines Py2BP2a-c were studied as tridentate ligands in developing the probe Py2BP2a (Ar = Ph, LODCu2+ = 26 nM); thus, this previous work is completed herein by DFT/TD-DFT studies to understand the sensing process. The basal and first excited state of Py2BP2a-c (Ar: Ph, 4-An, 4-Py) and the parent l,4,7-triphenylbispyrazolo[3,4-b:3′,4′-e]pyridine Ph3BP2 were optimised. Results suggest that the probes' fluorescence is due to a twisted intramolecular charge transfer (TICT) and ICT processes around the 4-aryl and 1,7-dipyridin-2-yl groups; likewise, the fluorescence turn-off in the presence of Cu2+ by probe Py2BP2b is due to a photoinduced electron transfer (PET) process, favouring a ligand-to-metal charge transfer (LMCT). These findings enhance our understanding of the sensing process and open new possibilities for its applications in various fields.

Effect of Alkali Source on Crystal Regulation and Ethanol Gas Sensing Properties of Nano-ZnO

This study investigates the ethanol gas-sensing mechanisms of ZnO nanocrystals with distinct morphologies, synthesized via a hydrothermal method using various alkali sources. Significant differences in the gas-sensing performance and morphology of ZnO samples synthesized with ammonium carbonate (Na2CO3), hexamethylenetetramine (HMTA), ammonia solution (NH3·H2O), and sodium hydroxide (NaOH) were observed. ZnO were confirmed to be impurity-free through XRD analysis, and their morphological features were characterized by SEM. TEM, XPS, and FTIR were employed to further analyze the crystal structure and binding energy of ZnO. To elucidate the underlying mechanisms, density functional theory (DFT) calculations combined with electron depletion layer theory were applied to assess charge transfer processes and identify the most sensitive ZnO crystal planes for ethanol detection. Experimental gas-sensing tests, conducted across 5–1000 ppm ethanol concentrations within a 150–350 °C range, showed that ZnO prepared with Na2CO3, HMTA, and NaOH was responsive at high ethanol concentrations as low as 100 °C, while ZnO synthesized with ammonia required 250 °C to exhibit sensitivity. All ZnO samples demonstrated excellent recovery at low concentrations at 250 °C. By integrating experimental findings with theoretical insights, this study provides a comprehensive understanding of ethanol gas-sensing mechanisms in ZnO, highlighting the role of crystal plane engineering and charge transfer dynamics as critical factors influencing gas response.

Improving charge transfer efficiency in CCDs: A SILVACO-based numerical study

In this study, we investigate the charge transfer efficiency (CTE) of a radiation-damaged charge-coupled device (CCD) subjected to proton radiation levels typical of space-borne experiments, nuclear imaging, and particle detection. The primary factor affecting CTE in such damaged CCDs is the trapping of charge carriers by bulk states. Our analysis examines CTE as a function of temperature, and radiation-created traps (trap levels). We employed a two-dimensional numerical model using the SILVACO semiconductor simulation software to simulate the dynamic transfer process in a buried-channel CCD (BCCD) with a three-phase clock pulse driver. After setting the appropriate physical models and the suggested deep traps levels in the channel region. The simulations demonstrate that the CTE shows a nonlinear dependence on temperature, with a charge transfer inefficiency (CTI) peaking at 7x10-6 at 135 K and reaching a minimum value of 2x10-6 around 200 K. These simulated results closely match the experimental data found in the literature, providing a comprehensive understanding of the impact of radiation-induced traps on the dynamic charge transfer processes in CCDs.

Analytical theoretical framework for closed bipolar electrochemical cells under homogeneous molecular catalysis: Implications for electrochemiluminescence applications

A novel analytical framework has been formulated to describe the current-potential-time response in systems with two polarized interfaces where one charge transfer process follows a catalytic mechanism, as found in co-reactant electrochemiluminescence (ECL) systems. The developed theory provides mathematical expressions for electrochemical and ECL signals, concentrations, and interfacial potentials upon the application of a constant potential pulse. Theoretical analysis reveals that the chemical regeneration of the redox reactant within the catalytic cycle has a remarkable impact on the chronoamperometric, voltammetric, and ECL responses, thereby providing means to estimate the catalytic rate constant and to optimize light emission. The system's behaviors are rationalized through the influence of catalysis on the interfacial concentrations and potentials. Also, the primary theoretical predictions have been experimentally validated using the [Ru(bpy)₃]²⁺/oxalate ECL system.

Exploring electronic structure and photophysical properties of metalloporphyrin-based metal–organic frameworks for photocatalysis: A quantum chemistry study

Hydrogen production is gaining interest as a clean energy source, with photocatalytic water-splitting being a key method due to its eco-friendly nature. Metalloporphyrins-based MOFs (TCPP(M)-MOFs), due to their tunable optical properties, are excellent materials for hydrogen evolution via water-splitting using sunlight. In this research, TCPP(M)-MOFs containing nodes based on metal ion d10 Zn2+ and TCPP(M) as linkers (M = Fe2+, Ni2+, Co2+and Cu2+) has been studied using theoretical approach. The electronic structure and optical properties of all Zn-TCPP(M)-MOFs were investigated using the density functional theory (DFT) and periodic-DFT calculations. The study revealed a bandgap reduction related to the open-shell metals in the TCPP linker, with an optimal value for the photocatalytic process under sunlight. TD-DFT calculations show that the inclusion of open shell ions enhances the linker-centered ligand-to-metal charge transfer process. Finally, it was suggested some directions for the design of new melloporphyrine-based MOFs, potentially leading to new materials for photocatalytic water-splitting.

N-doped Z-scheme heterojunctions on cobalt foam for enhanced photocatalytic degradation of levofloxacin and reduction of hexavalent chromium: Insights into charge separation and catalytic mechanisms

The transfer of photoelectrons across heterogeneous materials stands as a cornerstone process within the domain of photocatalysis. Elucidating the mechanisms underlying electron transfer at heterojunction interfaces provides profound insights that are crucial for the rational design of efficient catalysts. In this study, we employ a hierarchical synthesis approach to fabricate N-doped Z-scheme heterojunctions directly on the surface of cobalt foam (CoF). Both experimental observations and density functional theory (DFT) calculations reveal that N-doped CoS2 nanosheets exhibit asymmetric charge distribution, functioning as localized electron traps. Further analysis of differential charge density elucidates that positive charges are predominantly concentrated in proximity to N-CoS2, whereas negative charges accumulate near ZnO, indicating substantial charge exchange between these two phases. The integration of a potent built-in electric field upon illumination facilitates the splitting of photogenerated carriers in both transverse and longitudinal directions, thereby enabling their effective separation and migration. The CoF@N-CS@ZO composites demonstrated a remarkable capacity for simultaneous degradation and reduction, achieving a 93.6 % degradation of levofloxacin (LEV) and a 96.9 % reduction of hexavalent chromium (Cr(VI)) under visible light irradiation for 85 min. Furthermore, due to the active species being anchored on the surface of the CoF, which serves as a recyclable substrate, the composites could be directly recycled post-use. Notably, CoF@N-CS@ZO maintained an efficiency of over 80 % for both LEV degradation and Cr(VI) reduction even after undergoing more than ten cycles. This research elucidates the intricate interplay of the synergistic N-doped built-in electric field on the charge transfer process, offering profound insights into the targeted design of charge-modulated materials for enhanced photocatalytic performance.

Nitrous oxide abatement and valorization in an ammonia-fueled SOFC stack – Nitric oxide and electricity production

Nitrous oxide (N2O) is a harmful gas that strongly impacts climate change. Several strategies for denitrification have been addressed, where the use of solid oxide fuel cells (SOFCs) has been demonstrated to be attractive for N2O reduction and simultaneous electricity production. The reduction of N2O to N2 is studied for the first time at the cathode of an SOFC, where ammonia is supplied to the anode as fuel. A diluted ammonia stream is particularly interesting since it is normally available in HNO3 plants – the most important concentrated source of N2O emission – and is carbon-free. The combined reduction of N2O with the oxidation of NH3 allows the production of nitric oxide (NO) at the anode, a valuable precursor for HNO3 production.This work uses a commercial SOFC stack comprehending six cells, equipped with membrane electrode assemblies of LSM-CGO ‖ yttria-stabilized zirconia (YSZ) ‖ YSZ-NiO. Electrochemical Impedance Spectroscopy (EIS) was successfully employed to characterize the stack performance. Data were analyzed by combining a Distribution Function of Relaxation Times (DFRT) and Equivalent Circuit Models (ECMs), for different operating conditions, namely in terms of temperature and fuel feed composition. Three major processes were identified at the anode: one related to the adsorption/desorption of reactants on the surface of the electrocatalyst, a diffusion process of charge carriers/intermediate species to the triple phase boundary (TPB), and a charge-transfer process at the TPB. The electrochemical production of nitric oxide (NO) was investigated, and a 20 % selectivity towards NO production and an energy stack efficiency of 88 % was obtained. Overall, the current work provides a critical first step toward using SOFC to perform efficient N2O electroreduction using diluted ammonia as fuel.

Efficient Charge Transfer Driven Electrochemiluminescence in Heteroatom-Involved Cocrystal Engineering for Detection of Uranyl Ions.

Embracing strategies that circumvent the complexities and disordered structures of electrochemiluminescence (ECL) emitters to improve charge transfer efficiency is crucial for advancing ECL technology to the forefront. Here, heteroatom-involved cocrystal engineering was introduced, constructing an ECL system with controllability of the charge transfer process. Through the mutual recognition and coassembly between functional monomers, highly ordered cocrystal superstructures are formed. The layered donor-acceptor arrays in cocrystals accelerated charge transfer, producing a remarkable ECL performance. Furthermore, distinct heteroatoms possess the capability to modulate the charge distribution of monomers by either pushing or pulling electrons. This modulation ultimately affects the charge transfer pathways within cocrystals, enabling ECL emissions of varying intensities and wavelengths. Notably, the presence of UO22+ would significantly inhibit the charge transfer in cocrystals, causing a quenching of ECL signal. This unique characteristic enables precise and selective detection of UO22+. The heteroatom-involved cocrystals hold immense potential to construct next-generation ECL emitters and create fresh opportunities for the advancement of ECL technology.

Spontaneous detection of F− and viscosity using a multifunctional tetraphenylethene-lepidine probe: Exploring environmental applications

Excessive fluoride ions (F−) in drinking water and food is harmful for human health and the environment. Therefore, a fluorescent probe tetraphenylethylene-quinoline (P-1) is developed with multiple sensing properties for the sequential detection of tert-butyldiphenylsilyl chloride (TBDS), F−, and viscosity. Sensor P-1 first recognized TBDS and then observed an intramolecular charge transfer process, which produced an intermediate sensor P-2 in addition to fluorescence quenching at 576 nm. Following this, P-2 revealed a concentration-related quantitative analysis by tracking F− and reproducing sensor P-1 reversibly with the fluorescence amplification at 496 nm when the SiN bond of P-2 was broken. A comparable sensing mechanism was noted in monitoring F− and viscosity through a synthetically developed P-2 sensor. The characterizations (nuclear magnetic resonance-NMR, high resolution-mass-HR-MS, and high-performance liquid chromatography-HPLC) and density functional theory (DFT) confirmed the sensing mechanism of sensors P-1 and P-2. The proposed method was used to measure the viscosity of living cells and to measure F− in food, water, and living cell samples. According to research results, quantitative emission characteristics versus F− can offer insights into designing effective molecular probes with beneficial applications in healthcare and the environment.

Pyrene Derived Donor-Acceptor as a Host for Fullerene Unveils the Crystallinity in Semiconducting Nanostructures.

Donor-acceptor in linear π-conjugated systems elicits the intramolecular charge transfer which improves the optical and electronic characteristics. Nevertheless, linear arrangement of electron donor and acceptor finely tune the charge or electron transfer process divulges the device performance. Therefore, molecular engineering of appropriate D-A with precise spacer is indeed challenging. Herein, we synthesized two bispyrene derivatives and attached with benzothiadazole and phenyl group through imidazole spacer (PyBTD and PyBz). PyBTD has shown solvatochromism demonstrates the intramolecular charge transfer (ICT) from pyrene to benzothiadiazole while PyBz remains as pristine spectra. Microscopic images reveal that network-type structures for PyBTD and elongated nanorods from self-assemblies of PyBz. Subsequently, host-guest interactions suggest that C60 was encapsulated in concave shaped bispyrene controls their crystallinity in nanostructures leads short nanosheets. Impedance analyses depict ICT assisted nanowires facilitate improved conductivity than host-guest complex. Therefore, imidazole spacer between D-A systems paves the way to design such type of molecules for future generated optoelectronics.

Delayed luminescence and thermoluminescence in laboratory-grown diamonds

The “blue-green” phosphorescence/thermoluminescence is most commonly observed in diamonds following excitation at or above the indirect band gap and has been explained by a substitutional nitrogen-boron donor-acceptor pair recombination model. “Orange” and “red” phosphorescence have also been frequently observed in laboratory-grown near-colorless high-pressure high-temperature diamonds following optical excitation and their luminescence mechanisms are shown to be different from that of the blue-green phosphorescence. The physics of the orange and red luminescence and phosphorescence bands including the optical-excitation dependency (UV-NIR), temperature dependency (20K–573K), and related charge transfer process are investigated by a combination of self-built time-resolved imaging/spectroscopic techniques. In this paper, an alternative model for long-lived phosphorescence based on charge trapping is proposed to explain the orange phosphorescence/thermoluminescence band. Additionally, the red phosphorescence band is attributed to point defect, which possibly has a three-level phosphorescence system. Published by the American Physical Society 2024

Surface oxygen vacancy regulation strategy enhances the electrochemical catalytic activity of CoFe2O4 cathode for solid oxide fuel cells

Oxygen vacancies are crucial for enhancing oxygen ion transport in solid-state materials. Therefore, an approach was established to efficiently adjust the surface oxygen vacancy concentration in the solid oxide fuel cell (SOFC) cathodes. This method employs NaBH4 solution to capture lattice oxygen on the cathode surface, enabling precise control over both the surface oxygen vacancy concentration and the transition metal ion valence states in spinel CoFe2O4 (CFO) by modulating the NaBH4 treatment duration. The results indicate that CFO-10, treated with NaBH4 solution for 10 min, exhibits optimal electrochemical catalytic activity. This enhancement is primarily attributed to the improved oxygen adsorption-dissociation and charge transfer processes. At 750 °C, CFO-10 shows a polarization resistance (Rp) of 0.032Ω cm2, representing a reduction of 42.8 % compared to CFO. Additionally, CFO-10 achieves a peak power density (PPD) of 923 mW·cm−2, representing a 78.5 % increase compared to CFO. This study provides new insights for optimizing SOFC spinel oxide cathode performance and opens a promising avenue for the development of other high-performance catalytic materials.

Engineering Heterointerface to Synergistically Regulate Kinetics and Stress of Copper-Cobalt Selenide toward Reversible Magnesium/Lithium Hybrid Batteries.

Metal chalcogenide-based cathodes are crucial for the development of rechargeable magnesium batteries, yet the strong electrostatic interactions of Mg2+ result in slow ion transport and high polarization. The Mg2+/Li+ hybrid battery holds promise for enhancing the energy storage capability. Herein, we establish a system that utilizes (Co,Cu)Se2/CoSex heterostructure grown on carbon cloth as the cathode and APC-LiCl as a dual-salt electrolyte to achieve high reversible capacity, enhanced cyclic stability, and impressive rate performance. First-principles calculations and kinetic analyses are employed to uncover that constructing the heterointerface stimulates the formation of an intrinsic electric field and high-density electron flows, thereby accelerating charge transfer and ion diffusion processes. Finite element simulations further demonstrate that the heterostructure effectively alleviates stresses associated with magnesiation/lithiation to enhance the structural integrity of the material. Moreover, the multistep reaction unveils a stepwise structural transformation pathway. This study initiates a new chapter in designing heterointerface strategies for advanced energy storage devices.