Electron Conductivity Research Articles

Enhanced electrocatalytic CO2 reduction through constructing chemically homogeneous interfaces via ultrathin carbon encapsulated tin oxide

Electrocatalytic CO2 reduction to high-value chemicals has significant potential to combat environmental and energy crises. The strength and mode of adsorption of reaction species play a crucial role in determining the CO2 reduction products. Therefore, it is vital to construct catalytic interfaces with high catalytic activity, selectivity and chemically homogeneous for efficient CO2 reduction. Herein, ultra-thin carbon layer encapsulated sub-5 nm SnO2 quantum dots (SnO2@u-C) has been prepared by Sn-MOFs derivation for efficient electrocatalytic CO2 reduction. Specifically, the Faradaic efficiency of formate (FEformate) and energy efficiency of formate production (EEformate) exceed 80 % and 50 % respectively, over a wide potential range, with the highest value reaching 95.7 % for FEformate and 58.2 % for EEformate. Moreover, SnO2@u-C electrode shows excellent stability over 10 h with FEformate about 89 % at −1.17 V versus reversible hydrogen electrode. DFT calculations and experimental characterization reveal that the ultrathin carbon layer coating on the surface of SnO2 forms a chemically homogeneous catalytic interface, facilitating the adsorption and conversion of reaction species to achieve exceptional formate selectivity. Moreover, the carbon layer builds a three-dimensional rapid electron conduction network that supports electron transfer to CO2 molecules and suppressing SnO2 reduction.

High loading electrode with superior electron/ion transport network for high performance lithium-ion batteries

High loading electrode design is beneficial to increase the energy density of lithium ion batteries. Two obstacles for the high loading electrode application should be removed, including the limitation on ion/electron transport within high loading electrode and the structure stability. Here, the electron conduction on LiNi0.8Co0.1Mn0.1O2 cathodes is enhanced with evenly and tightly Ketjen Black coating via high-speed dry mixing, while carbon nanotube is added to enhance the electron conduction between LiNi0.8Co0.1Mn0.1O2 particles, thus to construct three-dimensional electron migration channel. In addition, the large amount of electrolyte adsorbed by porous Ketjen Black and carbon nanotube enhances the Li+ ion diffusivity in this network. As a result, LiNi0.8Co0.1Mn0.1O2 electrode with only 1 % Ketjen Black and 3 % carbon nanotube can achieve both high electron/Li+ ion diffusivity and high parking density (2.2 g cm−3). A thick electrode with an areal mass loading of 20 mg cm−2 shows a high specific capacity of 111.2 mA h g−1 at 4 C and capacity retention rate of 98.2 % after 100 cycles at 2 C.

Variations in flavin redox states during extracellular electron transfer and electron conduction in Shewanella oneidensis

Flavin is one of the most prevalent redox molecules utilized by electroactive bacteria. Electroactive bacteria form a three-dimensional architecture with multiple cell assemblages on electrodes in bioelectrochemical systems. This provokes the importance of unveiling the redox chemistry of flavins during electron transfer not only at the bacteria/electrode interface but also inside cell assemblages. However, it has been difficult to directly compare the redox species contributing to each electron transfer reaction. In this study, to simultaneously detect the flavin redox species at the electrode surface and those in cell assemblages, we conducted bipotentiometric cyclic voltammetry on a colony of Shewanella oneidensis MR-1. The bipotentiometric data showed that flavin mononucleotide proceeds the redox cycle at − 0.43 V (vs. standard hydrogen electrode) in the MR-1 colony assignable to the semiquinone/hydroquinone redox cycle, which was supported by experiments with semiquinone scavenger and gene deletion mutants. Notably, the peak at − 0.43 V was not detected at the electrode surface, indicating that the flavin redox cycles and redox potentials involved in the electron transfer inside MR-1 assemblages differ from those at the MR-1/electrode interface. The measurement system presented herein offers a platform to clarify the redox reactions in cell assemblages as well as at the bacteria/electrode interface.

Self-assembled La0.7Sr0.3Fe0.9Ni0.1O3-δ-Ce0.8Sm0.2O2-δ composite cathode with a three-dimensional ordered macroporous structure for protonic ceramic fuel cells

Self-assembled La0.7Sr0.3Fe0.9Ni0.1O3-δ-Ce0.8Sm0.2O1.9-δ (LSFN-SDC) composite cathode with a three-dimensionally ordered macroporous (3DOM) structure is synthesized using poly(methyl methacrylate) as the template for protonic ceramic fuel cells. The LSFN and SDC phases both distribute uniformly in the cathode. The SDC phase reduces the thickness of the walls of the 3DOM structure and thus hinders the bulk conduction of electrons. SDC also decreases the specific surface area and the surface oxygen reactivity of the cathode, leading to the suppression of the adsorption and dissociation of O2. However, the SDC phase provides the conduction pathway for oxygen ions and enlarges three phase boundary consequently, which facilitates the charge transfer steps. The thickness of the walls and the specific surface area of the composite cathode are both increased with the rise of the concentration of the nitrate precursor solution, resulting in the acceleration of the cathode process. Nevertheless, an excessive precursor concentration leads to the destroy of the 3DOM structure. The 3DOM composite cathode exhibits the lowest Rp of 0.039 Ω cm2, and a single cell with that cathode shows maximum power density of 1484 mW cm−2 at 700 °C. The cell exhibits a short-term stability of 120 h at 700 °C without noticeable degradation.

Balancing Ionic and Electronic Conduction at the LiFePO4 Cathode–Electrolyte Interface and Regulating Solid Electrolyte Interphase in Lithium‐Ion Batteries

AbstractRecently, in electric mobilities and stationary energy storage device applications, the development of long‐lasting, low‐cost, and high‐safety lithium‐ion batteries (LIBs) is widely studied. LiFePO4 (LFP) is a core cathode material for LIBs owing to its cost‐effectiveness and high safety. However, it exhibits low electronic conductivity and sluggish Li+ diffusion, hindering the application of LFP cathodes in high‐power battery industries. Herein, a triazole‐motivated electrolyte additive, 1‐(trimethylsilyl)−1H‐benzotriazole (TMSBTA) is presented, for mitigating iron dissolution via HF scavenging, reinforcing the robustness of the solid electrolyte interphase and constructing a cathode–electrolyte interface (CEI) to balance the ion and electron conduction of the CEI on the LFP cathode. Scanning probe microscopy performed in the conductive atomic force microscopy mode indicates that the electronically conductive CEI created by the oxidative decomposition of TMSBTA enables rapid and homogeneous lithiation and delithiation during cycling without morphological changes in the LFP particles. This study elucidates the design principles of the CEI on the LFP cathode and is expected to guide integrated electrolyte additive engineering for LFP‐containing LIBs.

Fast ionic conductor MnSe supported Micron-Si embedded in three-dimensional N-doped carbon matrix for lithium-ion batteries

Silicon is regarded as the most potential anode for the next generation lithium-ion batteries (LIBs) since its superhigh specific capacity and abundant reserves. Nonetheless, the grievous volume variation and inferior connate conductivity imped its further step on the commercial application. Herein, three-dimensional (3D) porous N-doped carbon microspheres, in which silicon is embedded and supported by MnSe, are fabricated via a simple spray drying method, named as MnSe/Si@NC. Such synergy conduces to the weaker polarization phenomenon and lower reactive barrier. Multi kind of electrochemical tests announce that the 3D network supported by MnSe and synthetical chemical bridge bonds, can remarkably ameliorate electron conductivity and structural stability. Benefit from the reasonably designed materials, the MnSe/Si@NC-10 anode expresses an outstanding cycling stability of 1030.8 mAh·g−1 at 2 A g−1 over 1000 cycles and extremely low-capacity loss rate for each cycle with about 0.27 ‰. In a word, this work can provide reference for the designing and preparation of high-performance anode materials utilized in LIBs.

Bismuth-constructed high-speed channeled for Bi/Sb2SnO5@PCFs composite as high-rate and long-life anode for sodium-ion batteries

To cope with the charging-time and driving-range issues of the power batteries, a composite and phase modification tactics is manifested to increase the cycling stability and rate capability of the Sb2SnO5 (SSO) anode for sodium-ion batteries (SIBs). The as-fabricated Bi/SSO@PCFs composite with Bi nanocrystals homogeneously dispersed on and around the SSO surface is prepared by an electrospinning method. The excellently dispersed Bi nanocrystals realize an effective contact with SSO, which effectively lowers the electron conduction barriers and promotes the sodium ion release as well as the transport upon the desodiation/sodiation process, increasing the rate capacity and cycle stability of the SSO anode. Importantly, a high-speed ion channel is constructed through the special layered Bi, and SbBi phase. The prepared Bi/SSO@PCFs anodes deliver a high rate capacity up to 25 A g−1 and long cycle life of 5000 cycles with 83 % capacity retention rate, sustaining an average capacity loss of 0.0034 % for each cycle. Particularly, the intercalation of Na+ between layer-structure Bi and SbBi galleries provides a good basis for excellent cycle performance due to small volume change and unobstructed ion channels. This finding provides an effective strategy to establish ion transport highways, which essentially increase the rate-capacity and cycle-life of the SSO-based anodes for SIBs.

Differences in Brain Region Mitochondrial Bioenergetics Detected Using CK Clamp

The brain is a non-uniform organ comprised of discrete structures of varying function and cell composition. The differing function of brain regions ostensibly would necessitate disparate energetic demands, thereby suggesting brain bioenergetics would be different among brain regions. This study aimed to address whether brain regions indeed have different bioenergetics by evaluating substrate preference, fuel-specific mitochondrial function at physiologically relevant energy demands as well as associated membrane potential and electron conductance using high-resolution respirometry (Oroboros O2k) in the frontal cortex, hypothalamus, and hippocampus. We hypothesize there will be different bioenergetics among brain regions. Substrate preference was established using a substrate-uncoupler-inhibitor-titration (SUIT) with additions, in order: ADP, Pyruvate/Malate, UK5099, Octanoylcarnitine, Rotenone, Succinate, and Antimycin A. There was no statistically significant interaction between region and substrate (p=0.15) nor a main effect of region (p=0.91), however, there was a main effect of substrate in which pyruvate/malate (+275%) and succinate/rotenone (+170%) had significantly greater respiration than octanoylcarnitine, independent of region (p<0.001). Given the results of the SUIT test, pyruvate/malate was used for subsequent tests. The SUIT method relies upon saturating ADP levels and non-physiological ATP:ADP concentration ratios, the extent to which this test obscures the interpretation of brain region respiration is unclear. Instead, an alternative approach that leverages the enzymatic reaction of creatine kinase and phosphocreatine to assess mitochondrial respiration and membrane potential at clamped physiological ATP:ADP ratios, “CK Clamp,” was used. Function of mitochondria with a pyruvate fuel was then evaluated in all three brain regions in which energetic demand was clamped at ΔGATP = -12.87 (high demand), -14.08, -14.5, and -14.85 (low demand). There was a statistically significant interaction between brain region and clamped ΔGATP values (p = 0.02). Frontal cortex displayed higher respiration than hippocampus at -12.87 ΔGATP (33%). There was no statistically significant interaction between region and clamp for mitochondrial membrane potential assessed during the CK clamp (p=0.16), however there was a significant main effect of clamped ΔGATP (p<0.001) in which membrane potential increased (i.e., hyperpolarized) as energetic demand decreased. This agrees with the bioenergetic model that a decrease in energetic demand increases the proton motive force (aka, hyperpolarization), thereby applying a backpressure on the electron transport chain, slowing respiration. Electron conductance was then assessed by calculating the slope of respiration versus clamped ΔGATP. Electron conductance was greater in the frontal cortex than hypothalamus (+70%, p = 0.015). The conclusion of this study is there are differences in mitochondrial bioenergetics among brain regions and the CK clamp was more sensitive at detecting these differences than the SUIT method. None. This is the full abstract presented at the American Physiology Summit 2024 meeting and is only available in HTML format. There are no additional versions or additional content available for this abstract. Physiology was not involved in the peer review process.

Oxidative stress in the remaining muscle after volumetric muscle loss contributes to impaired mitochondrial bioenergetics and is attenuated by SS-31

Volumetric muscle loss (VML) injury results in the non-recoverable loss of muscle mass and function. Our previous studies indicate mitochondrial dysfunction in the remaining muscle fibers after VML injury, marked by changes in mitochondrial respiration, membrane potential, and enzyme activities. In particular, mitochondrial membrane potential is hyperpolarized during the first 14-days post-injury, a condition that could lead to the production of reactive oxygen species (ROS). When ROS emissions exceed the antioxidant buffering capacity, cellular damage can ensue. The primary objective of this study was to determine ROS production, ROS emission, and antioxidant buffering capacity of remaining muscle fibers after VML injury in the first month after injury. The secondary objective of this study was to determine if a mitochondrial antioxidant (SS-31) could mitigate mitochondrial dysfunction after VML injury. We hypothesized that VML injury will alter the redox status of the remaining muscle. Study 1: Male C57BL/6J mice (n=40) were randomized to Uninjured or VML-injured cohorts. ROS (H2O2) emission/production and endogenous antioxidant buffering capacity were analyzed fluorometrically during live muscle fiber respiration (Oroboros O2k) at 3-, 7-, 14-, 21-, and 30-days post-injury. Study 2: Male C57BL/6J mice (n=32) were randomized into two groups: VML and VML+SS-31. SS-31 is a mitochondrial-targeted peptide with ROS-scavenging properties. VML+SS-31 received SS-31 (8mg/kg/day) for 14 days, and the VML received equal volume saline injections. At 14- and 28-days post-VML, mitochondrial respiration and electron conductance, ROS emission, and antioxidant buffering capacity were assessed in permeabilized gastrocnemius muscle fibers from the muscle remaining after the initial injury. Group differences were detected through ANOVA and unpaired t-test. ROS emission and antioxidant buffering capacity were different between VML-injured and Uninjured mice through 14-days post-injury, specifically at 3-, 7-, and 14-days, mitochondrial ROS emission was significantly higher (+28%, p<0.001), and antioxidant buffering capacity was less (-28%, p=0.002) in VML mice compared to Uninjured mice. Two weeks of SS-31 treatment lead to greater muscle fiber respiration and electron conductance (p≤0.008) at both 14- and 28-days post-VML. Importantly, at 14-days post-injury, mitochondrial ROS emission was 71% lower in VML+SS-31 than VML. At both 14- and 28-days post-injury, antioxidant buffering capacity was 12% greater in VML+SS-31 (p≤0.003) compared to VML. Oxidative stress is a feature of early VML pathophysiology marked by greater ROS emission and less antioxidant buffering capacity. Attenuating oxidative stress during the first two-weeks post-VML injury improves mitochondrial respiration. W81XWH-20-1-0885 and R01AR078903 to SG and JC. This is the full abstract presented at the American Physiology Summit 2024 meeting and is only available in HTML format. There are no additional versions or additional content available for this abstract. Physiology was not involved in the peer review process.

Thermoelectric properties of undoped and Bi-doped GeS monolayers: A first-principles study

Different from the extensive experimental investigations into the thermoelectric (TE) properties of the bulk IV–VI compounds, less attention has been paid to the TE properties of the monolayer IV–VI compounds. Here, we consider the TE transport properties including the Seebeck coefficient, electronic conductance, thermal conductance, power factor, and figure of merit ZT of the undoped and Bi-doped GeS monolayers. Our results show that for both the undoped and Bi-doped monolayers the anisotropy is widely observed in all their TE properties, and the maximum ZT at a certain temperature along the armchair direction is much greater than that along the zigzag direction. Moreover, Bi doping can lead to an increase of the maximum ZT, and there are more ZT peaks appearing near the zero chemical potential. This indicates that the Bi-doped GeS monolayer can work as a TE material at a lower bias voltage, and especially along the armchair direction it can work at zero bias voltage, which obviously strengthens the reliability of the TE devices. As the temperature increases, the maximum ZT will be uniformally increased along the armchair and zigzag directions for both the undoped and Bi-doped GeS monolayers. In the temperature scope from 300 to 800 K, the maximum ZT along the armchair direction of the Bi-doped GeS monolayer will increase from 3.39 to 4.85, which indicates that this Bi-doped GeS monolayer is a promising TE material in a wide-temperature zone. As an application, we have designed the GeS-based TE couples and found that their efficiencies can be greater than 27% at large temperature differences. This research should be an important guidance for designing a low-voltage, wide-temperature-scope, and high-stability TE device.

Transcriptomic analysis reveals extensive modulation of mitochondrial gene expressions after volumetric muscle loss injury

Volumetric muscle loss (VML) is characterized by the unrecoverable loss of muscle tissue and function. Therapeutic modalities remain elusive in part because the etiology of the pathology remains unclear. Past RNA-sequencing analyses shed light on transcriptional regulation, but differential gene expression and gene set enrichment analysis (GSEA) results are often dominated by the robust inflammatory and fibrotic response to the injury. The primary objective of this study was to leverage past datasets and interrogate transcriptional regulation of cellular metabolism because our group has previously reported that VML injury disrupts mitochondrial function in the remaining muscle after VML injury. We hypothesized that a metabolic GSEA analysis will identify several differentially expressed mitochondrial gene sets. Utilizing a publicly-available rat species RNAseq dataset, we transformed that data from transcripts per million (TPM) to a Z-score with respect to the uninjured group. Since TPM is not compatible with cross-sample comparisons, we opted for a single-sample GSEA that permits phenotype comparisons. Visualizing the normalized enrichment scores (NES) into heatmaps allowed us to select the top-25 enriched gene sets. The majority of the top-25 could be split into three groups: electron transport chain (ETC, n=8), substrate metabolism (SM, n=5), and mitochondrial maintenance (MM, n=2). The NES at each day post-VML injury (dpi) was compared to its respective uninjured group using a two-tailed t-test. We found that all ETC-related pathways were significantly enriched and downregulated at 7-, 14-, and 28-dpi (p ≤ 0.039). For example, the percent change in NES of ‘complex 1’ was- 436%, -419%, and -816%, respectively (p≤0.002). SM-related pathways followed a similar downward trend (p≤0.044). For example, ‘TCA’ -149%, -303%, and -697%, respectively (p≤0.028). Interestingly, within the MM-related gene sets, mitochondrial ‘fusion’ was significant down at 7- and 28-dpi (-319%, -414%, p≤0.009) while ‘fission’ was significantly down at 3-, 7-, and 14-dpi (-157%, -319%, and -797%, p≤0.030). We next analyzed a publicly-available mouse species scRNAseq data set. To examine the muscle-specific transcriptional response we combined the counts for myonuclei and satellite cells. GSEA revealed six significantly enriched gene sets, notably ‘all metabolism genes’ (NES = 1.33, FDR q = 0.050), and the remaining four were related to the ETC (NES ≥ 1.81, FDR q ≤ 0.050). This retrospective, comprehensive analysis confirms dynamic changes in the expression of mitochondrial-related genes in response to VML injury in both rats and mice. The modulation of genes related to the electron transport chain, mitochondrial maintenance, and substrate metabolism agree with physiological outcomes of impaired mitochondrial carbohydrate metabolism, hyperpolarized mitochondria, and slowed electron conductance from previous mouse studies. R01AR078903 to SG and JC. This is the full abstract presented at the American Physiology Summit 2024 meeting and is only available in HTML format. There are no additional versions or additional content available for this abstract. Physiology was not involved in the peer review process.

Activation of peroxymonosulfate (PMS) by rGO supported Co3O4 catalyst for iohexol degradation

Sulphate radical (SO4·-) -based advanced oxidation process (SR-AOP) is a promising sewage treatment technology. Reduced graphene oxide (rGO) supported Co3O4 composites were synthesized by a hydrothermal method for the degradation of iohexol (IOH) in the rGO/Co3O4/peroxymonosulfate (PMS) system. Experimental results show that rGO/Co3O4 possessed much better PMS activated ability than pure GO or Co3O4, which is ascribed to the summation of rGO and Co3O4. The efficiency of rGO/Co3O4 composite, single GO and Co3O4 nanocrystals for the degradation of IOH were 98.7%, 15.8% and 79.8% at 15 min, and their corresponding reaction rate constants (kapp) were 0.21 min−1, 0.0077 min−1 and 0.080 min−1, respectively. The results of active species capture experiment and electron paramagnetic resonance (EPR) experiment, showed that singlet oxygen is the main active species, which is non-radical degradation. rGO is conducive to the electron conduction of Co3O4, thus improving the efficiency of PMS activation. The system is simple and efficient, which is an effective technology to remove IOH.

Dual ligands and crosslinking atoms relayed MOF anode for tetracycline hydrochloride electrocatalytic decontamination: Efficiency and mechanism

MOF anodes were especially prepared with dual-ligand and S/N crosslinking atoms for tetracycline hydrochloride (TCH) electrocatalytic degradation. Results showed S(HTTP)-Ni-N(HAB) and N(HITP)-Ni-S(BHT) exhibited high electrocatalytic performance with 100% TCH degradation in 10 min, which were superior to that of S(HTTP)-Ni-S(BHT) and N(HITP)-Ni-N(HAB). The experimental and DFT calculation results jointly unraveled that the electron delocalization created by adjacent S/N crosslinking atoms facilitated the electron conduction and produced positive-charged Ni sites for the improved generation of ·O2− and ·OH radicals. The positive contributions of ·O2− and ·OH radicals then proved the degradation pathways of TCH. In addition, extended experiments on various conditions and pollutions highlighted the application potential of S/N hybrid MOF anodes. The final results provided new insight into MOF anode design and preparation via large cardinal ligand and crosslinking atom adjustment for environmental application.

A comprehensive quantitative DFT procedure to evaluate rate-capability and electron conduction of intercalation electrode materials: Assessment of novel Li[Mi]1/3[Mj]1/3[Mk]1/3O2 electrodes as case studies

This paper uses comprehensive approach to propose quantitative evaluations of the electrode materials’ electronic rate-capability calculated by density functional theory (GGA/GGA + U). Here, a novel approach is introduced to evaluate electrical rate-capability by calculating electronic conductivity (σ) for the case studies. Application of the evaluated materials as electrodes of Li-ion battery is taken into account. Also, thermal conductivity and Seebeck coefficient for the materials are calculated. Here, three novel alternatives for LiNi1/3Co1/3Mn1/3O2 (NCM111), in which introduced by substitution of transition metals, are LiNi1/3Mn1/3Fe1/3O2(NMF), LiMn1/3Fe1/3Co1/3O2(MFC), and LiFe1/3Co1/3Ni1/3O2(FCN). The evaluated materials are compared with each other and other relevant electrodes, based on structural, electrochemical, and electrical properties. The voltage reaction of the cathode materials is calculated by two approaches, namely internal and Fermi energy methods. According to the obtained results, MFC and NMF have superior properties on NCM. It is concluded that the NMF can be the best alternative for NCM conditionally.

Ultrathin High-Entropy Fe-Based Spinel Oxide Nanosheets with Metalloid Band Structures for Efficient Nitrate Reduction toward Ammonia.

Spinel oxides with tunable chemical compositions have emerged as versatile electrocatalysts, however their performance is greatly limited by small surface area and low electron conductivity. Here, ultrathin high-entropy Fe-based spinel oxides nanosheets are rationally designed (i.e., (Co0.2Ni0.2Zn0.2Mg0.2Cu0.2)Fe2O4; denotes A5Fe2O4) in thickness of ≈4.3nm with large surface area and highly exposed active sites via a modified sol-gel method. Theoretic and experimental results confirm that the bandgap of A5Fe2O4 nanosheets is significantly smaller than that of ordinary Fe-based spinel oxides, realizing the transformation of binary spinel oxide from semiconductors to metalloids. As a result, such A5Fe2O4 nanosheets manifest excellent performance for the nitrate reduction reaction (NO3 -RR) to ammonia (NH3), with a NH3 yield rate of ≈2.1mmol h-1 cm-2 at -0.5V versus Reversible hydrogen electrode, outperforming other spinel-based electrocatalysts. Systematic mechanism investigations reveal that the NO3 -RR is mainly occurred on Fe sites, and introducing high-entropy compositions in tetrahedral sites regulates the adsorption strength of N and O-related intermediates on Fe for boosting the NO3 -RR. The above findings offer a high-entropy platform to regulate the bandgap and enhance the electrocatalytic performance of spinel oxides.

Perspectives on the highly selective oxidation of copper-mediated C3N4-BiVO4 organic-inorganic hybrid catalysts and the efficient generation of reactive oxygen species

Singlet oxygen (1O2) is a kind of reactive oxygen species (ROS) with both oxidizability and selectivity. The construction of 1O2 is the key to improve the selectivity of various organic reactions. In this study, Cu/C3N4-BiVO4 (CCN-BVO) ternary system significantly improved the catalytic effect of selective oxidation of glycerol to prepare high value chemical dihydroxyacetone (DHA). At the same time, CCN-BVO also has a strong environmental catalytic effect, and the decomposition effect of liquid phase organic pollutants can reach more than 90 % within 2 h. The superior ROS production capacity of CCN-BVO, particularly its ability to produce 1O2, has been confirmed by electron spin resonance (ESR) and quenching experiments as the reason for its excellent catalytic effect. Electrochemical characterization and X-ray photoelectron spectroscopy (XPS) proved that Cu can be used as an intermediary to accelerate electron conduction, and can also effectively construct defects to improve oxygen absorption efficiency, thus effectively increasing ROS yield. This study also theoretically confirmed the reaction path of glycerol catalysis through DFT calculation, which provided a theoretical basis for the subsequent design of efficient catalytic materials.

Enhancing proton exchange membrane water electrolysis by building electron/proton pathways

Proton exchange membrane water electrolysis (PEMWE) plays a critical role in practical hydrogen production. Except for the electrode activities, the widespread deployment of PEMWE is severely obstructed by the poor electron-proton permeability across the catalyst layer (CL) and the inefficient transport structure. In this work, the PEDOT:F (Poly(3,4-ethylenedioxythiophene):perfluorosulfonic acid) ionomers with mixed proton-electron conductor (MPEC) were fabricated, which allows for a homogeneous anodic CL structure and the construction of a highly efficient triple-phase interface. The PEDOT:F exhibits strong perfluorosulfonic acid (PFSA) side chain extensibility, enabling the formation of large hydrophilic ion clusters that form proton-electron transport channels within the CL networks, thus contributing to the surface reactant water adsorption. The PEMWE device employing membrane electrode assembly (MEA) prepared by PEDOT:F-2 demonstrates a competitive voltage of 1.713 ​V under a water-splitting current of 2 ​A ​cm−2 (1.746 ​V at 2A cm−2 for MEA prepared by Nafion D520), along with exceptional long-term stability. Meanwhile, the MEA prepared by PEDOT:F-2 also exhibits lower ohmic resistance, which is reduced by 23.4 ​% and 17.6 ​% at 0.1 ​A ​cm−2 and 1.5 ​A ​cm−2, respectively, as compared to the MEA prepared by D520. The augmentation can be ascribed to the superior proton and electron conductivity inherent in PEDOT:F, coupled with its remarkable structural stability. This characteristic enables expeditious mass transfer during electrolytic reactions, thereby enhancing the performance of PEMWE devices.

A novel ε-MnO2/MXene composite as an electrode with excellent conductivity and ultrahigh capacitive deionization

Manganese dioxide (MnO2) holds great promise as an electrode material for capacitive deionization (CDI); but its low electrical conductivity considerably restricts its desalination capacity. Nevertheless, its electrochemical performance can be enhanced by augmenting its conductivity. Hence, we propose a novel strategy for constructing a strongly coupled ε-MnO2/MXene composite, in which, MXene (Ti3C2Tx) serves as a network of electron conduction highways that enhance the charge transfer of ε-MnO2 and activates the underutilized electrochemically active sites of ε-MnO2. Based on these advantages, an ε-MnO2/MXene composite is prepared for the first time, comprising spherical ε-MnO2 nanoparticles grown on MXene layers. As demonstrated, ε-MnO2/MXene composite demonstrates exceptional desalination performance, exhibiting a maximum deionization rate of 17.54 mg g−1 min−1 and an ultrahigh desalination capacity of 114.66 mg g−1 in 1000 mg/L NaCl solution at 1.2 V, which is considerably higher than those observed for ε-MnO2 (74.93 mg g−1), MXene (29.26 mg g−1) and recently reported electrode materials. Such an outstanding CDI performance can be ascribed to a considerably high specific capacitance ε-MnO2/MXene composite of approximately 337.2F g−1 at a specific current of 1 A/g, which is approximately 2.16 times that of an ε-MnO2 electrode.The excellent performance of ε-MnO2/MXene composite makes it a potential practical application of CDI.

Assembly of Amorphizing Porous Bimetallic Metal‐Organic Frameworks Spheres with Zn─O─Fe Cluster and Coordination Deficiency via Ligand Competition for Efficient Electro‐Fenton Catalysis

AbstractElectro‐Fenton process stands out as a highly promising approach for generating reactive oxygen‐containing radicals to address the escalating issue of environmental pollution. However, the long‐term goal of application necessitates ongoing pursuit of high‐quality catalysts with both sufficient activity and stability. Herein, a general route is reported for large‐scale synthesis of amorphizing porous bimetallic metal‐organic framework (MOF) spheres with Zn─O─Fe structure and coordination deficiency through facile and low‐cost synthesis of ligand competition. Assisted by a coordination modulator, deprotonation of terephthalic acid is accelerated and rapid synthesis of amorphous bimetallic MOF spheres is successfully achieved at room temperature. As inactive metal Zn is introduced into metal clusters of MOFs, the cycling efficiency of Fe3+/Fe2+ is improved and a secondary building unit of Zn─O─Fe is constructed, greatly accelerating electron conduction rate. Compared to crystalline spindle cMIL‐88B(Fe2Zn) by traditional solvothermal route, amorphous aMIL‐88B(Fe2Zn) has a unique spherical porous structure with larger surface area, higher conductivity, and more exposed active sites. Endowed with unique textural and surface chemistry, aMIL‐88B(Fe2Zn) exhibits superior catalytic activity in the degradation of refractory organic pollutants. The progress offers a feasible way to rational design of iron‐based hybrid MOF materials with tunable structures and enhance properties for various applications.

Highly Conductive Carbon/Carbon Composites as Advanced Multifunctional Anode Materials for Structural Lithium‐Ion Batteries

AbstractCurrently, structural lithium‐ion batteries (LIBs) typically use carbon fibers (CFs) as multifunctional anode materials to provide both Li+ storage and high mechanical strength. However, due to the obvious volume expansion of CFs in lithiation process, the fiber structure suffers rapid degradation during cycling. Herein, CFs‐reinforced carbon matrix (C/C) composites are proposed as multifunctional anodes for structural LIBs for the first time. The C/C composite presents distinctive core/shell structure, in which CF as the core supplies a fast and continuous electron conduction pathway along with excellent mechanical strength, while the layered pyrolytic carbon shell accommodates the volume change of CF and provides additional ion storage. The impact of the C/C microstructure on the ion/electron transport and the Li+ storage mechanism behind such a unique hybrid structure are explored. Owing to the structural advantages of the C/C composite, the LiFePO4||C/C full cell exhibits surprising electrochemical performances at high electrode mass loadings, which are far superior to those of the present structural LIBs and even surpass the commercial LIBs at the same mass loadings. Moreover, the pouch cell presents excellent mechanical strength and mechanical‐electrochemical coupling characteristics. This work demonstrates great potential of the C/C composites as new multifunctional anodes for high‐performance structural batteries.