Enhanced Cd2+ removal from aqueous solution using olivine and magnesite combination: New insights into the mechanochemical synergistic effect.

In this study, an efficient stabilizer material for cadmium (Cd2+) treatment was successfully prepared by simply co-milling olivine with magnesite. Several analytical methods including XRD, TEM, SEM and FTIR, combined with theoretical calculations (DFT), were used to investigate mechanochemical interfacial reaction between two minerals, and the reaction mechanism of Cd removal, with ion exchange between Cd2+ and Mg2+ as the main pathway. A fixation capacity of Cd2+ as high as 270.61 mg/g, much higher than that of the pristine minerals and even the individual/physical mixture of milled olivine and magnesite, has been obtained at optimized conditions, with a neutral pH value of the solution after treatment to allow its direct discharge. The as-proposed Mg-based stabilizer with various advantages such as cost benefits, green feature etc., will boosts the utilization efficiency of natural minerals over the elaborately prepared adsorbents.

Barrierless reactions of C2 Criegee intermediates with H2SO4 and their implication to oligomers and new particle formation.

The formation of oligomeric hydrogen peroxide triggered by Criegee intermediate maybe contributes significantly to the formation and growth of secondary organic aerosol (SOA). However, to date, the reactivity of C2 Criegee intermediates (CH3CHOO) in areas contaminated with acidic gas remains poorly understood. Herein, high-level quantum chemical calculations and Born-Oppenheimer molecular dynamics (BOMD) simulations are used to explore the reaction of CH3CHOO and H2SO4 both in the gas phase and at the air-water interface. In the gas phase, the addition reaction of CH3CHOO with H2SO4 to generate CH3HC(OOH)OSO3H (HPES) is near-barrierless, regardless of the presence of water molecules. BOMD simulations show that the reaction at the air-water interface is even faster than that in the gas phase. Further calculations reveal that the HPES has a tendency to aggregate with sulfuric acids, ammonias, and water molecules to form stable clusters, meanwhile the oligomerization reaction of CH3CHOO with HPES in the gas phase is both thermochemically and kinetically favored. Also, it is noted that the interfacial HPES- ion can attract H2SO4, NH3, (COOH)2 and HNO3 for particle formation from the gas phase to the water surface. Thus, the results of this work not only elucidate the high atmospheric reactivity of C2 Criegee intermediates in polluted regions, but also deepen our understanding of the formation process of atmospheric SOA induced by Criegee intermediates.

Gradient conducting polymer surfaces with netrin-1-conjugation promote axon guidance and neuron transmission of human iPSC-derived retinal ganglion cells.

Major advances have been made in utilizing human-induced pluripotent stem cells (hiPSCs) for regenerative medicine. Nevertheless, the delivery and integration of hiPSCs into target tissues remain significant challenges, particularly in the context of retinal ganglion cell (RGC) restoration. In this study, we introduce a promising avenue for providing directional guidance to regenerated cells in the retina. First, we developed a technique for construction of gradient interfaces based on functionalized conductive polymers, which could be applied with various functionalized ehthylenedioxythiophene (EDOT) monomers. Using a tree-shaped channel encapsulated with a thin PDMS and a specially designed electrochemical chamber, gradient flow generation could be converted into a functionalized-PEDOT gradient film by cyclic voltammetry. The characteristics of the successfully fabricated gradient flow and surface were analyzed using fluorescent labels, time of flight secondary ion mass spectrometry (TOF-SIMS), and X-ray photoelectron spectroscopy (XPS). Remarkably, hiPSC-RGCs seeded on PEDOT exhibited improvements in neurite outgrowth, axon guidance and neuronal electrophysiology measurements. These results suggest that our novel gradient PEDOT may be used with hiPSC-based technologies as a potential biomedical engineering scaffold for functional restoration of RGCs in retinal degenerative diseases and optic neuropathies.

Mechanism of overscreening breakdown by molecular-scale electrode surface morphology in asymmetric ionic liquids.

The interfacial nature of the electric double layer (EDL) assumes that electrode surface morphology significantly impacts the EDL properties. Since molecular-scale roughness modifies the structure of EDL, it is expected to disturb the overscreening effect and alter differential capacitance (DC). In this paper, we present a model that describes EDL near atomically rough electrodes with account for short-range electrostatic correlations. We provide numerical and analytical solutions for the analysis of conditions for the overscreening breakdown and DC shift estimation. Our findings reveal that electrode surface structure leads to DC decrease and can both break or enhance overscreening depending on the relation of surface roughness to electrostatic correlation length and ion size asymmetry.

Se vacancies and interface engineering modulated bifunctionality prussian blue analogue derivatives for overall water splitting.

It is a challenging task to design and synthesize stable, and high-performance non-precious metals bifunctional catalysts for water-splitting. Herein, the coupling between Se vacancy and interface engineering is highlighted to synthesize a unique CoFeSe hollow nanocubes structure on MXene-modified nickel foam (NF) by in-situ phase transition from bifunctionality prussian blue analogue (PBA) derivatives (VSe-CoFeSe@MXene/NF). DFT theory reveals that the Se vacancy and interface engineering modulate the surface electronic structure and optimize the surface adsorption energy of the intermediates. Experimental data also confirm that the as-prepared CoFeSe@MF catalyst exhibits advanced electrocatalytic properties, 283 mV (OER) and 67 mV (HER) are required to drive the current density of 10 mA cm-2. Notably, it is assembled into a two-electrode system for integral water decomposition, which only requires a low cell potential of 1.57 V at current of 10 mA cm-2, together with excellent durability for 48 h. The strategy is expected to provide a new direction for the design and construction of highly efficient collaborative integrated water decomposition electrocatalysts.

Constructing multi-layer heterogeneous interfaces in liquid metal graphite hybrid powder: Towards microwave absorption enhancement.

Carbon based materials are widely used in the preparation of microwave absorption materials due to their low density, high attenuation loss and large specific surface area. However, their high conductivity usually leads to high reflection loss. In this study, multi-layer heterogeneous interfaces were constructed in liquid metal graphite hybrid powder to reduce reflection loss and enhance microwave absorption performance. Gallium oxide (Ga2O3) layer was formed in Ga coated graphite powder to improve impedance matching and attenuation constant via an annealing treatment. Specifically, the hybrid particles with 50 wt% Ga and being annealed at 120 °C for 2 h have a minimum reflection loss (RLmin) value of -42.68 dB and a maximum effective absorption bandwidth (EAB) of 4.11 GHz at a thickness of 3.3 mm. The hybrid particles not only have multi-layer structures with different electrical conductivity, but also form heterojunctions between different interfaces, which can further enhance dipole and interfacial polarization.

Construction of porous Cu/CeO2 catalyst with abundant interfacial sites for effective methanol steam reforming.

Methanol is a promising hydrogen carrier for fuel cell vehicles (FCVs) via methanol steam reforming (MSR) reaction. Ceria supported copper catalyst has attracted extensive attentions due to the extraordinary oxygen storage capacity and abundant oxygen vacancies. Herein, we developed a colloidal solution combustion (CSC) method to synthesize a porous Cu/CeO2(CSC) catalyst. Compared with Cu/CeO2 catalysts prepared by other methods, the Cu/CeO2(CSC) catalyst possesses highly dispersed copper species and abundant Cu+-Ov-Ce3+ sites at the copper-ceria interface, contributing to methanol conversion of 66.3 %, CO2 selectivity of 99.2 %, and outstanding hydrogen production rate of 490 mmol gcat-1 h-1 under 250 °C. The linear correlation between TOF values and Cu+-Ov-Ce3+ sites amount indicates the vital role of Cu+-Ov-Ce3+ sites in MSR reaction, presenting efficient ability in activation of water. Subsequently, a deep understanding of CSC method is further presented. In addition to serving as a hard template, the colloidal silica also acts as disperser between nanoparticles, enhancing the copper-ceria interactions and facilitating the generation of Cu+-Ov-Ce3+ sites. This study offers an alternative approach to synthesize highly dispersed supported copper catalysts.

Facilitating charge transfer via a Semi-Coherent Fe(PO3)2-Co2P2O7 heterointerface for highly efficient Zn-Air batteries.

Developing reversible oxygen electrodes for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for achieving high-performance rechargeable Zn-air batteries (ZABs). This study introduced an nitrogen-doped carbon confined with a semi-coherent Fe(PO3)2-Co2P2O7 heterojunction for bifunctional oxygen electrocatalysis. This nanocomposite yielded an ORR half-wave potential of 0.908 V and an OER overpotential of 291 mV at 10 mA/cm2. ZABs incorporating this catalyst yielded impressive performance, including a peak power density of 203 mW/cm2, a specific capacity of 737 mAh/gZn, and promoted stability. Both experimental and theoretical simulations demonstrated that the unique electric field between Fe(PO3)2 and Co2P2O7 promoted efficient charge transport across the heterointerface. This interaction likely modulated the d-band center of the heterojunction, expedite the desorption of oxygen intermediates, thus improving oxygen catalysis and, consequently, ZAB performance. This work illustrates a significant design principle for creating efficient bifunctional catalysts in energy conversion technologies.

Interfacial modulation of nicotinamide additive enables 9700 h Zn metal batteries.

Aqueous zinc-ion batteries (AZIBs) have recently been paid great attention due to their robust safety features, high theoretical capacity, and eco-friendliness, yet their practical application is hindered by the serious dendrite formation and side reactions of Zn metal anode during cycling. Herein, a low-cost small molecule, nicotinamide (NIC), is proposed as an electrolyte additive to effectively regulate the Zn interface, achieving a highly reversible and stable zinc anode without dendrites. NIC molecules not only modify the Zn2+ solvation structure but also preferentially adsorb on the Zn surface than solvated H2O to protect the Zn anode and provide numerous nucleation sites for Zn2+ to homogenize Zn deposition. Consequently, the addition of 1 wt% NIC enables Zn||Zn symmetric cells an ultra-long lifespan of over 9700 h at 1 mA cm-2, which expands nearly 808 times compared to that without NIC. The advantages of NIC additives are further demonstrated in NaVO||Zn full cells, which exhibit exceptional capacity retention of 90.3 % after 1000 cycles with a high Coulombic efficiency of 99.9 % at 1 A/g, while the cell operates for only 42 cycles without NIC additive. This strategy presents a promising approach to solving the anode problem, fostering advancements in practical AZIBs.

Empowering lithium-ion storage: unveiling the superior performance of niobium-based oxide/perovskite heterojunction with built-in electric field.

The increasing demand for high-performance electrode materials in lithium-ion batteries has driven significant attention towards Nb2O5 due to its high working voltage, large theoretical capacity, environmental friendliness, and cost-effectiveness. However, inherent drawbacks such as poor electrical conductivity and sluggish electrochemical reaction kinetics have hindered its lithium storage performance. In this study, we introduced KCa2Nb3O10 into Nb2O5 to form a heterojunction, creating a built-in electric field to enhance the migration and diffusion of Li+, effectively promoting electrochemical reaction kinetics. Under the regulation of the built-in electric field, the charge transfer resistance of the KCa2Nb3O10/Nb2O5 anode decreased by 3.4 times compared to pure Nb2O5, and the Li+ diffusion coefficient improved by two orders of magnitude. Specifically, the KCa2Nb3O10/Nb2O5 anode exhibited a high capacity of 276 mAh g-1 under 1 C, retaining a capacity of 128 mAh g-1 even at 100 C. After 3000 cycles at 25 C, the capacity degradation was only 0.012% per cycle. Through combined theoretical calculations and experimental validation, it was found that the built-in electric field induced by the heterojunction interface contributed to an asymmetric charge distribution, thereby improving the rates of charge and ion migration within the electrode, ultimately enhancing the electrochemical performance of the electrode material. This study provides an effective approach for the rational design of high-performance electrode materials.

Efficient solar-driven: Photothermal catalytic reduction of atmospheric CO2 at the gas-solid interface by CuTCPP/MXene/TiO2.

Directly capturing atmospheric CO2 and converting it into valuable fuel through photothermal synergy is an effective way to mitigate the greenhouse effect. This study developed a gas-solid interface photothermal catalytic system for atmospheric CO2 reduction, utilizing the innovative photothermal catalyst (Cu porphyrin) CuTCPP/MXene/TiO2. The catalyst demonstrated a photothermal catalytic performance of 124 µmol·g-1·h-1 for CO and 106 µmol·g-1·h-1 for CH4, significantly outperforming individual components. Density functional theory (DFT) results indicate that the enhanced catalytic performance is attributed to the internal electric field between the components, which significantly enhances carrier utilization. The introduction of CuTCPP reduces free energy of the photothermal catalytic reaction. Additionally, the local surface plasmon resonance (LSPR) effect and high-speed electron transfer properties of MXene further boost the catalytic reaction rate. This well-designed catalyst and catalytic system offer a simple method for capturing atmospheric CO2 and converting it in-situ through photothermal catalysis.

Engineering S-scheme mCN@mPDIP molecular heterojunction with highly efficient interface charge transfer for photocatalytic aerobic oxidation synthesis.

The construction of S-scheme heterojunctions, which offers a promising approach for spatially separating photogenerated charge carriers with high redox potentials and multimolecular activation, represents a viable modification strategy in photocatalytic applications. However, the prevalent insufficient contact areas between two components result in low interface charge transfer efficiency, thereby impeding the photocatalytic performance of such heterostructures. Herein, we address this limitation by introducing a unique mCN@mPDIP molecular heterojunction through a pH-triggered molecule self-assembly eutectoid technique, enabling intimate interface contact and promoting highly efficient interfacial charge transfer following an S-scheme mechanism. Consequently, the mCN@mPDIP molecular heterojunction achieves significantly improved charge separation efficiency and higher concentration of active carriers compared to typical bCN-bPDIP bulk heterojunction and nCN/nPDIP nano heterojunction. Combined with the effective sulfide activation on mPDIP sites and O2 activation on mCN sites, the resulting mCN@mPDIP demonstrates outstanding activity in the photocatalytic aerobic oxidation of sulfides into sulfoxides without any redox mediators.

Interfacial study and modulation of high-voltage layered cathode based all-solid-state batteries.

Employing layered materials as the cathodes for solid-state batteries (SSBs) is vital in enhancing the batteries' energy density, whereas numerous issues are present regarding the compatibilities between cathode electrode and modified solid electrolyte (ME) in this battery configuration. By investigating the electrochemical performance and interfacial properties of SSBs using various cathodes, the fundamental reason for the poor compatibility between layered cathodes, especially LiCoO2 with ME is revealed. Because of the Li(solvent)+ intercalation environments formed in the ME, the resultant weak-interacted TFSI- could be adsorbed and destabilized by Co ions on the surface. Besides, the high energy level offsets between LiCoO2 and ME lead to Li-ion transferring from the bulk electrode to the electrolyte, resulting in a pre-formed interface on the cathode particles before the electric current is applied, affects the formation of effective cathode-electrolyte interface (CEI) film during electrochemical process and deteriorated overall battery performance. From this view, an interlayer is pre-added on the LiCoO2 surface through an electrostatic adsorption method, to adjust the energy level offsets between the cathode and ME, as well as isolate the direct contact of surface Co ions to TFSI-. The cycling properties of the SSB using modified LiCoO2 are greatly enhanced, and a capacity retention of 68.72 % after 100 cycles could be achieved, against 8.28 % previously, certifying the rationality of the understanding and the effectiveness of the proposed modification method. We believe this research could provide basic knowledge of the compatibility between layered cathodes and MEs, shedding light on designing more effective strategies for achieving SSBs with high energy density.

Superabsorbent starch protective layer modulates zinc anode interface for long-life aqueous zinc ion batteries.

Aqueous zinc ion batteries (AZIBs) have attracted much attention for their safety, low cost and high theoretical capacity. Nevertheless, Zn dendrites and the adverse reactions such as corrosion, hydrogen evolution and passivation on the anode affect the cycle life and stability of AZIBs. Herein, superabsorbent starch (SS) was employed on Zn foil to form an artificial interface protection layer, which inhibited the formation of dendrites by guiding the uniform deposition of Zn2+. SS with a large amount of oxygen-containing functional group is superabsorbent, which can attract the active water around the hydrated Zn2+, promoting the desolvation process of the hydrated Zn2+ and significantly inhibiting the occurrence of hydrogen evolution reaction. In addition, the inherent pore structure of the SS artificial interfacial layer can induce uniform nucleation of Zn2+ and inhibit the dendrites growth. Moreover, compared to bare Zn//MnO2 cell (44.1 %), the capacity retention of Zn@SS//MnO2 cell remained as high as 87.8 % after 1000 cycles at 1.5 A g-1. The simple method provided a new method for the rapid development of AZIBs.

3D printing of highly conductive and strongly adhesive PEDOT:PSS hydrogel-based bioelectronic interface for accurate electromyography monitoring.

PEDOT: PSS hydrogel-based bioelectronic interfaces have gained significant attention in various fields including biomedical devices, wearable devices, and epidermal electronics. However, the development of high-performance bioelectronic interfaces that integrate excellent conductivity, strong adhesion, and advanced processing compatibility remains a challenge. Herein, we develop a high-performance bioelectronic interface by 3D printing of a novel poly(vinyl alcohol-formaldehyde) (PVAF)-PEDOT:PSS composite ink. Such a PEDOT:PSS-PVAF ink exhibits favorable rheological properties for direct-ink-writing 3D printing, enabling the fabrication of high-resolution patterns and three-dimensional structures with high aspect ratios. Hydrogel bioelectronic interface printed by such PEDOT:PSS-PVAF ink simultaneously achieves high conductivity (over 100 S m-1), strong adhesion (31.44 ± 7.07 kPa), as well as stable electrochemical performance (charge injection capacity of 13.72 mC cm-2 and charge storage capacity of 18.80 mC cm-2). We further integrate PEDOT:PSS-PVAF hydrogel bioelectronic interface to fabricate adhesive skin electrodes for electromyography (EMG) signal recording. The resultant EMG skin electrodes demonstrate superior performance and stability compared to commercial products, maintaining high signal-to-noise ratio of > 10 dB under varying weights and repetitive motions. These advantageous performance of PEDOT:PSS-PVAF based hydrogel bioelectronic interfaces may be helpful for diverse bioelectronic applications like healthcare monitoring and epidermal bioelectronics.

Large scale investigation of the effect of gender on mu rhythm suppression in motor imagery brain-computer interfaces.

The utmost issue in Motor Imagery Brain-Computer Interfaces (MI-BCI) is the BCI poor performance known as 'BCI inefficiency'. Although past research has attempted to find a solution by investigating factors influencing users' MI-BCI performance, the issue persists. One of the factors that has been studied in relation to MI-BCI performance is gender. Research regarding the influence of gender on a user's ability to control MI-BCIs remains inconclusive, mainly due to the small sample size and unbalanced gender distribution in past studies. To address these issues and obtain reliable results, this study combined four MI-BCI datasets into one large dataset with 248 subjects and equal gender distribution. The datasets included EEG signals from healthy subjects from both gender groups who had executed a right- vs. left-hand motor imagery task following the Graz protocol. The analysis consisted of extracting the Mu Suppression Index from C3 and C4 electrodes and comparing the values between female and male participants. Unlike some of the previous findings which reported an advantage for female BCI users in modulating mu rhythm activity, our results did not show any significant difference between the Mu Suppression Index of both groups, indicating that gender may not be a predictive factor for BCI performance.

Advancements in Flexible Electronics Fabrication: Film Formation, Patterning, and Interface Optimization for Cutting-Edge Healthcare Monitoring Devices.

Flexible electronics can seamlessly adhere to human skin or internal tissues, enabling the collection of physiological data and real-time vital sign monitoring in home settings, which give it the potential to revolutionize chronic disease management and mitigate mortality rates associated with sudden illnesses, thereby transforming current medical practices. However, the development of flexible electronic devices still faces several challenges, including issues pertaining to material selection, limited functionality, and performance instability. Among these challenges, the choice of appropriate materials, as well as their methods for film formation and patterning, lays the groundwork for versatile device development. Establishing stable interfaces, both internally within the device and in human-machine interactions, is essential for ensuring efficient, accurate, and long-term monitoring in health electronics. This review aims to provide an overview of critical fabrication steps and interface optimization strategies in the realm of flexible health electronics. Specifically, we discuss common thin film processing methods, patterning techniques for functional layers, interface challenges, and potential adjustment strategies. The objective is to synthesize recent advancements and serve as a reference for the development of innovative flexible health monitoring devices.

Exploring the Impact of In Situ-Formed Solid-Electrolyte Interphase on the Cycling Performance of Aluminum Metal Anodes.

Unwanted processes in metal anode batteries, e.g., non-uniform metal electrodeposition, electrolyte decomposition, and/or short-circuiting, are not fully captured by the electrolyte bulk solvation structure but rather defined by the electrode-electrolyte interface and its changes induced by cycling conditions. Specifically, for aluminum-ion batteries (AIBs), the role of the solid-electrolyte interphase (SEI) on the Al0 electrodeposition mechanism and associated changes during resting or cycling remain unclear. Here, we investigated the current-dependent changes at the electrified aluminum anode/ionic liquid electrolyte interface to reveal the conditions of the SEI formation leading to irreversible cycling in the AIBs. We identified that the mechanism of anode failure depends on the nature of the counter electrode, where the areal capacity and cycling current for Al0 electrodeposition dictates the number of successful cycles. Notwithstanding the differences behind unstable aluminum anode cycling in symmetrical cells and AIBs, the uniform removal of electrochemically inactive SEI components, e.g., oxide-rich or solvent-derived organic-rich interphases, leads to more efficient cycling behavior. These understandings raise the importance of using specific conditioning protocols for efficient cycling of the aluminum anode in conjugation with different cathode materials.

Reinforced interfacial coupling effect of NiO/Ni2P by Fe doping for boosting water splitting.

Nickel-based catalysts are suitable for water splitting to generate hydrogen. However, the low conductivity and weak stability have always been urgent issues to be addressed in nickel-based catalysts. Fe-doped nickel oxide/nickel phosphide (Fe-NiO/Ni2P) was prepared as a bifunctional electrocatalyst by doping metal and constructing heterogeneous interface. The introduction of Fe contributed to the reinforced interfacial coupling effect of NiO/Ni2P to promote charge transfer and accelerate reaction kinetics. The heterojunction regulated the interfacial charge density between NiO and Ni2P to improve the electronic environment of Ni2+ and enhance conductivity. The O-Fe-P bond at the heterogeneous interface induced the directional transfer of electrons and ensured the structure stability. The synergistic effect of Fe doping and heterogeneous interface increased the adsorption energy of *O and coordinated the adsorption energy of *H, advancing the catalytic performance. Fe-NiO/Ni2P exhibited the overpotential of 242 mV and 141 mV at 10 mA cm-2 for oxygen and hydrogen evolution, respectively.

A(CoFe)(S2)2/CoFe heterostructure constructed in S, N co-doped carbon nanotubes as an efficient oxygen electrocatalyst for zinc-air battery.

Transition metal alloys can exhibit synergistic intermetallic effects to obtain high activities for oxygen reduction/evolution reactions (ORR/OER). However, due to the insufficient stability of active sites in alkaline electrolytes, conventional alloy catalysts still do not meet practical needs. Herein, by using polypyrrole tubes and cobalt-iron (CoFe) Prussian blue analogs as precursors, CoFe sulfides is in-situ formed on CoFe alloys to construct (CoFe)(S2)2/CoFe heterostructure in sulfur (S) and nitrogen (N) co-doped carbon nanotubes (CoFe@NCNTs-nS) via a low-temperature sulfidation strategy. The as-marked CoFe@NCNTs-12.5S exhibits a comparable ORR activity (half-wave potential of 0.901 V) to Pt/C (0.903 V) and a superior OER activity (overpotential of 272 mV at 10 mA cm-2) to RuO2 (299 mV). CoFe@NCNTs-12.5S also exhibits ultralow charge transfer resistances (ORR-6.36 Ω and OER-0.21 Ω) and an excellent potential difference of 0.617 V. The sulfidation-induced (CoFe)(S2)2/CoFe heterojunctions can accelerate interfacial charge transfer process. Tubular structure not only disperses the (CoFe)(S2)2/CoFe heterostructure, but also reduces the corrosion of active-sites to enhance catalysis stability. Zinc-air battery with CoFe@NCNTs-12.5S achieves a high specific capacity (718.1 mAh g-1), maintaining a voltage gap of 0.957 V after 400 h. This work reveals the potential of interface engineering for boosting ORR/OER activities of alloys via in-situ heterogenization.