Carbonaceous Electrodes Research Articles

Performance Evaluation of Desalination Battery Systems based on Synthesis Method of Carbon Nanotube-Carbon Felt Composite Electrodes

To enhance chlorine ion removal and increase the current charging capacity of a desalination battery system, carbon nanotubes were applied to a carbonaceous electrode. Two types of composite electrodes were fabricated by attaching multiwalled carbon nanotubes (MWCNTs) to a carbon felt (CF) electrode via dip coating (D-CNT@CF) and electrophoresis (E-CNT@CF). These composite electrodes were then tested within a desalination battery system to evaluate their chlorine ion removal efficiency and current charging performance during the charging process. Microflocs of MWCNTs were observed on the surface of D-CNT@CF, whereas a uniform coating of MWCNTs was achieved on the surface of E-CNT@CF. Performance evaluations revealed that chlorine ion removal rates improved by 3.5% for D-CNT@CF and by 19.4% for E-CNT@CF compared to that of CF. Furthermore, the time required to reach maximum current charge was 40.0% for D-CNT@CF and E-CNT compared to CF. @CF decreased by 60.0%. These findings suggest that surface modification of carbonaceous electrodes through electrophoresis can result in a more stable coating and improve the performance of desalination battery systems.

Covalent Carbide Interconnects Enable Robust Interfaces and Thin SEI for Graphite Anode Stability under Extreme Fast Charging.

Carbonaceous and carbon-coated electrodes are ubiquitous in electrochemical energy storage and conversion technologies due to their electrochemical stability, lightweight nature, and relatively low cost. However, traditional reliance on conductive additives and binders leads to impermanent electrical pathways. Here, a general approach is presented to fabricate robust electrodes with a progressive failure mechanism by introducing carbide-based interconnects grown via carbothermal conversion of (5 wt%) titanium hydride nanoparticles. This method concurrently enhances both electrical and mechanical properties within the electrode architecture. The resulting chemical bonding between active materials establishes a novel mechanism to maintain stable electrical pathways during cycling. Employed as Li-ion battery anodes, these electrodes exhibit improved cyclability, achieving 80% capacity retention after 800 fast-charge cycles at moderate loading (1 mAh cm- 2). High loading cells with areal capacity of 3 mAh cm-2 show significantly improved cycle lifeover the same number of cycles. This performance improvement is attributed to the absence of significant impedance growth and a thinner solid electrolyte interphase (SEI) layer formed at high current densities (4C) as demonstrated by X-ray photoelectron spectroscopy and transmission electron microscopy studies. The enhanced conductivity facilitates SEI formation, lowering ionic impedance and mitigating lithium plating, ultimately leading to the reported extended cycle life.

Carbon Nitride Nanosheets as an Adhesive Layer for Stable Growth of Vertically-Ordered Mesoporous Silica Film on a Glassy Carbon Electrode and Their Application for CA15-3 Immunosensor.

Vertically ordered mesoporous silica films (VMSF) are a class of porous materials composed of ultrasmall pores and ultrathin perpendicular nanochannels, which are attractive in the areas of electroanalytical sensors and molecular separation. However, VMSF easily falls off from the carbonaceous electrodes and thereby impacts their broad applications. Herein, carbon nitride nanosheets (CNNS) were served as an adhesive layer for stable growth of VMSF on the glassy carbon electrode (GCE). CNNS bearing plentiful oxygen-containing groups can covalently bind with silanol groups of VMSF, effectively promoting the stability of VMSF on the GCE surface. Benefiting from numerous open nanopores of VMSF, modification of VMSF's external surface with carbohydrate antigen 15-3 (CA15-3)-specific antibody allows the target-controlled transport of electrochemical probes through the internal silica nanochannels, yielding sensitive quantitative detection of CA15-3 with a broad detection range of 1 mU/mL to 1000 U/mL and a low limit of detection of 0.47 mU/mL. Furthermore, the proposed VMSF/CNNS/GCE immunosensor is capable of highly selective and accurate determination of CA15-3 in spiked serum samples, which offers a simple and effective electrochemical strategy for detection of various practical biomarkers in complicated biological specimens.

Accounting for the Quantum Capacitance of Graphite in Constant Potential Molecular Dynamics Simulations.

Molecular dynamics (MD) simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite the numerous advances in the simulation of electrodes, they fail to accurately represent the electronic structure of materials such as graphite. In this work, a simple parameterization method that allows to tune the metallicity of the electrode based on a quantum chemistry calculation of the density of states (DOS) is introduced. As a first illustration, the interface between graphite electrodes and two different liquid electrolytes, an aqueous solution of NaCl and a pure ionic liquid, at different applied potentials are studied. It is shown that the simulations reproduce qualitatively the experimentally-measured capacitance; in particular, they yield a minimum of capacitance at the point of zero charge (PZC), which is due to the quantum capacitance (QC) contribution. An analysis of the structure of the adsorbed liquids allows to understand why the ionic liquid displays a lower capacitance despite its large ionic concentration. In addition to its relevance for the important class of carbonaceous electrodes, this method can be applied to any electrode materials (e.g. 2D materials, conducting polymers, etc), thus enabling molecular simulation studies of complex electrochemical devices in thefuture.

Understanding the Wettability of C1N1 (Sub)Nanopores: Implications for Porous Carbonaceous Electrodes.

Understanding how water interacts with nanopores of carbonaceous electrodes is crucial for energy storage and conversion applications. A high surface area of carbonaceous materials does not necessarily need to translate to a high electrolyte-solid interface area. Herein, we study the interaction of water with nanoporous C1N1 materials to explain their very low specific capacity in aqueous electrolytes despite their high surface area. Water was used to probe chemical environments, provided by pores of different sizes, in 1H MAS NMR experiments. We observe that regardless of their high hydrophilicity, only a negligible portion of water can enter the nanopores of C1N1, in contrast to a reference pure carbon material with a similar pore structure. The common paradigm that water easily enters hydrophilic pores does not apply to C1N1 nanopores below a few nanometers. Calorimetric and sorption experiments demonstrated strong water adsorption on the C1N1 surface, which restricts water mobility across the interface and impedes its penetration into the nanopores.

Stable Lithium Metal Batteries Enabled by Dilute Cationic Additives

Conventional Li-ion electrolytes consist of carbonate solvents and Li-ion salts that were made for carbonaceous negative electrodes. When the electrolytes are used with metallic lithium anodes, carbonate electrolytes lead to low charge-discharge cycle stability due to adverse reactive species at the anode surface.1-4 This reactive species are called the solid electrolyte interface (SEI).1 SEI instabilities/inhomogeneities result in its continuous thickening and formation of electronically non-active dead lithium.2 SEI composition and structure are affected by both solvent and electrolyte chemistry in bulk solution and, more importantly, at the electrode-electrolyte interface.4 Current research studies suggest that X-rich (where X is a halogen) SEI yields superior performance compared to halogen-free SEI.1,5 Electrolytes that have large volume fractions of halogenated species have statistically higher probability to be reduced at the electrode surface and yield X-rich SEI layers.6 Therefore, the use of halogenated solvent and/or high concentrated (> 1 M) lithium salt with halogenated anions has been actively explored for LiMBs. However, the high cost of Li salts and high viscosity of the electrolyte at high salt concentration make the concentrated electrolytes unrealistic for commercial battery applications. In search of a cost-effective solution for high performance LiMBs, halogenated electrolyte additives could serve as an ideal approach since only a small amount of the additive would be potentially required to induce similar X-rich interface that can be seen in the case of the halogenated ether electrolyte. In this meeting abstract, we present a new concept that leverages favorable electrostatic interactions with the electrolyte additive to drive the formation of robust SEI layers even at low additive content. Specifically, custom-designed additives can be electrostatically attracted to the negatively charged electrode, creating a high population of halogenated species at the anode surface even at a dilute Li salt concentration. Effective SEI formation with a low-concentration additive circumvents the challenges associated with the current state-of-the-art approach of using halogenated species at high concentration (i.e., unfavorably high solution viscosity and high cost). Reference 1 Louli, A. J. et al. Diagnosing and correcting anode-free cell failure via electrolyte and morphological analysis. Nature Energy 5, 693-702, (2020).2 Chen, K.-H. et al. Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes. Journal of Materials Chemistry A 5, 11671-11681, (2017).3 Lin, D. et al. Three-dimensional stable lithium metal anode with nanoscale lithium islands embedded in ionically conductive solid matrix. Proc Natl Acad Sci U S A 114, 4613-4618, (2017).4 Lin, D., Liu, Y. & Cui, Y. Reviving the lithium metal anode for high-energy batteries. Nat Nanotechnol 12, 194-206, (2017).5 Yu, Z. et al. Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries. Nature Energy 5, 526-533, (2020).6 Yamada, Y., Wang, J., Ko, S., Watanabe, E. & Yamada, A. Advances and issues in developing salt-concentrated battery electrolytes. Nature Energy 4, 269-280, (2019).

Polyphenol-Derived Carbonaceous Frameworks with Multiscale Porosity for High-Power Electrochemical Applications.

With the escalating global demand for electric vehicles and sustainable energy solutions, increasing focus is placed on developing electrochemical systems that offer fast charging and high-power output, primarily governed by mass transport. Accordingly, porous carbons have emerged as highly promising electrochemically active or supporting materials due to expansive surface areas, tunable pore structures, and superior electrical conductivity, accelerating surface reaction. Yet, while substantial research has been devoted to crafting various porous carbons to increase specific surface areas, the optimal utilization of the surfaces remains underexplored. This review emphasizes the critical role of the fluid dynamics within multiscale porous carbonaceous electrodes, leading to substantially enhanced pore utilization in electrochemical systems. It elaborates on strategies of using sacrificial templates for incorporating meso/macropores into microporous carbon matrix, while exploiting the unique properties of polyphenol moieties such as sustainable carbons derived from biomass, inherent adhesive/cohesive interactions with template materials, and facile complexation capabilities with diverse materials, thereby enabling adaptive structural modulations. Furthermore, it explores how multiscale pore configurations influence pore-utilization efficiency, demonstrating advantages of incorporating multiscale pores. Finally, synergistic impact on the high-power electrochemical systems is examined, attributed to improved fluid-dynamic behavior within the carbonaceous frameworks, providing insights for advancing next-generation high-power electrochemical applications.

Renewable Musa Sapientum derived porous nano spheres for efficient energy storage devices

Biomass-based carbonaceous materials derived from Musa Sapientum have gained much attention in recent years for their application in energy storage devices, especially supercapacitors. In the present work, we synthesized carbonaceous material from banana peel as the biomass precursor by using a pyrolysis method carried out at various temperatures (600, 800, and 1000 °C). The characterization of the prepared carbonaceous materials BP600, BP800 and BP1000 was done by using different characterization techniques such as FTIR, XRD, FE-SEM, and TEM, studies. The electrochemical study of the synthesized material was carried out by cyclic voltammetry (CV), galvanostatic charge–discharge (GCD) electrochemical impedance spectroscopy (EIS). The supercapacitive performance of the material was studied using a 3-electrode system with 3M KOH as an electrolyte. As a result, the BP600 exhibited a better specific capacitance with higher energy and power densities along with a maximum cyclic stability of 16,000 cycles. To show the practical applicability of the material BP 600, two electrode system studies were carried out as well, which showed preferentially good values for specific capacitance with appreciable power and energy density values. The study provides us with a green approach for the fabrication of non-toxic, low-cost, and environmentally friendly potential porous carbonaceous electrode materials by converting bio-waste into a clean and renewable source of energy.

Carbon nanotubes as efficient anode current collectors for stationary aqueous Zn–Br2 batteries

Static Zn–Br2 batteries are considered an attractive option for cost-effective and high-capacity systems for large energy storage. Yet, the corrosive nature of the Zn–Br2 electrolytes entails a careful selection of all cells' ingredients to avoid rapid degradation of the batteries upon cycling. Thanks to their high chemical resistance and excellent conductivity, carbonaceous electrodes are typically utilized as current collectors for the cathode side, while thin Zn or Ti foils are most widely used as the anodes' current collectors. However, these metals tend to corrode fast, thus undermining the desirable performance of the cells as durable and stable rechargeable batteries. We demonstrate the effective utilization of carbon nanotubes (CNT) films as highly stable anode current collector for Zn–Br2 batteries. Dispersion of the CNT beforehand in slurries containing anionic, cationic, or neutral surfactants yielded distinct chemical and physical characteristics of these carbonaceous electrodes. This, in turn, led to significant differences in the morphology of the deposited Zn, consequently affecting the electrochemical performance of the Zn anodes. These findings provide insight into the interactions between Zn cations and the surface of CNTs, offering opportunities for further surface modifications of CNTs as effective anodes’ substrates for Zn–Br2 batteries.

Ultrahigh Salt Adsorption Capacity of Carbonaceous Electrode in a Rocking-Chair Capacitive Deionization through Surface Charge Modulation

Ultrahigh Salt Adsorption Capacity of Carbonaceous Electrode in a Rocking-Chair Capacitive Deionization through Surface Charge Modulation

A novel MXene coated liquid crystal display anode derived from a futile computer monitor for microbial fuel cell application

A Ti3C2Tx MXene nanosheet-coated liquid crystal display (LCD) anode is meticulously crafted through precision waterjet cutting, salvaging a discarded LCD monitor. This technique, preserving structural integrity and enhanced electrical conductivity, sets it apart from conventional methods. The resulting MXene-coated LCD anode is well-suited for microbial fuel cell (MFC) applications. Comparative assessments against costlier carbonaceous electrodes like graphite felt and carbon cloth, emphasize that the water-jet cut LCD anode with Ti3C2Tx MXene coating is 3.79 and 2.51 times more cost-effective, with an approximate total cost of $38/m2. Substituting Ti3C2Tx MXene-coated LCD for carbon cloth and graphite felt anodes reduces MFC unit fabrication costs by 19 and 10.45 %, respectively. Notably, the Ti3C2Tx MXene LCD anode-based MFC unit boasts a power density per unit cost of 0.008 W/m2/$, underscoring economic viability. This research highlights waterjet cutting's pivotal role in crafting Ti3C2Tx MXene LCD anodes, opening avenues for scalable, cost-effective electrode production in renewable energy applications.

Integration of Carbon-Based Nanomaterials for Hybrid Energy Storage in Lithium-Ion Batteries

Hybrid energy storage systems benefit significantly from incorporating nanoparticles containing metallic oxides, potassium phosphate, chemical compounds, and sulfides. The current technological problem is to increase the device’s electrical capacity without decreasing its energy capacity. The energy storage capacity of lithium-ion cells has been greatly improved by the use of tiny carbon particles owing to their conductive qualities, extensive specific surface area, customizable form, and intrinsic resilience. Further biologically active layouts, thinner ion-diffusion dimensions, and increased aboard carrier-/charge-transport motion are all made possible by incorporating effective bi-dimensional nanomaterials into future-oriented battery packs. For applications like lithium-ion batteries and electrochemical capacitors, this research presents carbon-based energy storage (CES) using a support vector machine (SVM) incorporating Particle Swarm Optimization (CES-SVM) to investigate the long-term stability of nanoparticle alloy forms of a specific shape and chemical makeup. This paper provides a potential improvement to the intermittent particle swarm optimization technique and its accompanying algorithmic architecture. Hybrid nanocomposites have been successfully synthesized, allowing the easy synthetic pathway and unique growth of nanostructuring technology to be used for electrodes with outstanding electrochemical effectiveness in conventional lithium-ion batteries. This paper shows how the cell’s conductivity, the electrode/electrolyte contact, and ion diffusion all affect impedance performance. Carbonaceous electrodes for lithium-ion battery systems, electrochemical storage units, and related combination devices are examined as a final area.

Algal biomass-based zero-waste biorefinery for producing optically pure (R)-γ-valerolactone and carbonaceous electrodes applicable for energy storage devices

Mankind is facing a severe climate crisis caused by fossil fuel-derived CO2 emissions. Although biorefineries utilizing biomass have been considered the best option for carbon-neutrality, most biorefinery-derived products have not yet been promising for economic feasibility; various strategies have been developed to increase economic competitiveness, and zero-waste biorefineries are challenging options. Herein, we aim to develop an algal biomass-based zero-waste biorefinery for producing enantioselective (R)-γ-valerolactone ((R)-GVL) and carbonaceous electrodes applicable for Li-ion batteries (LiBs). Various algal biomasses were hydrothermally oxidized to produce levulinic acid (LA) as an intermediate for producing (R)-GVL, resulting that Gracilaria verrucosa was selected as feedstock. For the hydroxylation of G. verrucosa-derived LA to 4-hydroxyvaleric acid (4-HV), 3-hydroxybutyrate dehydrogenase (HBDH) was explored through genome mining and further engineered. The engineered HBDH successfully converted G. verrucosa-derived LA to 4-HV, which was subsequently lactonized under acidic conditions, resulting in optically pure (R)-GVL. To our knowledge, this is the first report of the production of an algal biomass-derived enantioselective (R)-GVL with a perfect enantiomeric excess (>99.99 %) that can be used as a precursor for more valuable biopharmaceuticals and bioplastics than biofuels. Furthermore, residual G. verrucosa after hydrothermal oxidation was used as a carbonaceous anode material for LIBs for the first time; hard carbon anodes, which were prepared through simple heat treatment (800 ℃, 3 h, argon atmosphere), exhibit good capacities of 231, 191, 133, 108, 97 and 86 mAh/g at 0.05, 0.1, 0.5, 1, 1.5, and 2 A/g, respectively. The results discussed herein can provide insights into zero-waste biorefineries applicable for diverse industrial fields (e.g., biopolymer, biopharmaceutical and energy storage) and contribute to the construction of closed-carbon-loops for coping with climate change.

Endowing turbostratically porous carbon with rich edge nitrogen active sites for efficient capacitive removal of phosphate

The mitigation of phosphate in water is a pivotal concern for the prevention of eutrophication and enhancement of water quality. Capacitance deionization (CDI) technique possesses the merits of high removal efficacy, facile operation, and environmental friendliness, rendering it a promising strategy for phosphate elimination. Herein, the nitrogen-rich laminar porous carbon composites (NTPCs) prepared by direct pyrolysis of supermolecular precursor were utilized as phosphate capture electrodes. The resulting NTPC800 features a high nitrogen content turbostratically amorphous carbon framework, which facilitates efficient ion diffusion pathways and electron transfer. The abundant presence of edge nitrogen (pyridine and pyrrole nitrogen) optimizes the electronic structure of the carbon system and provides more active sites, thus leading to the boosted electrochemical activity and dephosphorization efficiency. Consequently, NTPC800 demonstrates a rapid phosphate removal capacity, achieving 73.51 mg g−1 within a mere 10 min at 1.2 V condition, which is nearly 6 times more efficient than that of the commercial activated carbon electrode. Moreover, it exhibited consistent phosphate removal efficiency across various pH ranges, coexisting ion interferences, and cyclic stability assessments. This study provides theoretical support for the utilization of edge nitrogen decorated carbonaceous electrodes to enhance charge transfer and provide additional active sites for efficient capacitive dephosphorization.

Dip-coated graphene nanoplatelets and multiwall carbon nanotubes composite ink electrode for metal-free paper-based flexible heating device

A paper-based flexible heating device (PFHD - paper-based flexible heating device) composed of a cellulose paper substrate and a carbonaceous functional electrode is reported. The functional composite electrodes containing graphene nanoplatelets (GNP - graphene nanoplatelets) and multi-walled carbon nanotubes (MWCNT) in various compositional ratios were prepared by dip-coating the oxygen plasma-treated paper substrate into the composite ink, and subsequently dried at 110 ℃ for 30 min to prepare PFHDs. The electrochemical characteristics and heat generation properties of PFHDs indicated that the GNP component in the functional electrode enhanced the electrical conductivity of the electrode, and the physical stability was enhanced mainly by the MWCNT component. Accordingly, PFHD0.33 which contains 33 % GNP and 67 % MWCNT in the functional electrode shows excellent heating performance with high stability and areal rated power of 0.68 W cm−2 (specific rated power = 45 W g−1). The measured sensitivity of PFHD0.33 is 31.50 ℃ V−1 at the applied DC voltage of 0.1–2.0 V.

Nitrogen-doped carbonaceous electrode modified by biological metal-organic framework for vanadium redox flow batteries

The biological metal-organic framework (Bio-MOF) is utilized to modify the carbonaceous electrode for the vanadium redox flow batteries. The microwave solvothermal method prepared the cobalt-based Bio-MOF on a graphite felt (GF) surface. Then, the nitrogen-doping graphite and porous structure formation were completed simultaneously during the carbonization process. Finally, electrochemical activation was conducted to remove cobalt metal from the GF electrode and raise the concentration of oxygen-containing functional group active sites. By in-situ Raman spectroscopy, the increase of disordered graphitic lattices could be observed by raising the potential from 0.6 V to 1.6 V. The microwave solvothermal method and electrochemical activation can effectively shorten the treatment time compared with the traditional solvothermal method and acidic etching processes. Among the carbonization parameters for Bio-MOF-covered GFs, maintaining the temperature at 900 °C for 2 h under an argon atmosphere is the most suitable. The annealed sample after electrochemical activation (BMDGF-900EA) displays 73.7 % energy efficiency at 120 mA cm−2 and possesses a 90 % retention rate of efficiency after 250 cycles at 180 mA cm−2. The superior performance results from more catalytic active sites, hydrophilic surface features, and larger specific surface area prove that this modification method derived from Bio-MOF indeed provides a novel and potential way to improve the VRFB performance.

Sensitive Electrochemical Detection of Carcinoembryonic Antigen Based on Biofunctionalized Nanochannel Modified Carbonaceous Electrode.

The convenient construction of carbon-based electrochemical immunosensors with high performance is highly desirable for the efficient detection of tumor biomarkers. In this work, an electrochemical immunosensor was fabricated by integrating a biofunctionalized mesoporous silica nanochannel film with a carbon-based electrode, which can enable the sensitive determination of carcinoembryonic antigen (CEA) in serum. The commonly used carbonaceous electrode, glassy carbon electrode (GCE), was employed as the supporting electrode and was pre-treated through electrochemical polarization to achieve the stable binding of a vertically ordered mesoporous silica film with amino groups (NH2-VMSF) without the use of any adhesive layer. To fabricate the immunorecognition interface, antibodies were covalently immobilized after the amino groups on the outer surface of NH2-VMSF was derivatized to aldehyde groups. The presence of amino sites within the high-density nanochannels of NH2-VMSF can facilitate the migration of negatively charged redox probes (Fe(CN)63-/4-) to the supporting electrode through electrostatic adsorption, leading to the generation of electrochemical signals. In the presence of CEA, the formation of immunocomplexes on the recognitive interface can reduce the electrochemical signal of Fe(CN)63-/4- on the supporting electrode. Based on this principle, the sensitive electrochemical detection of CEA was achieved. CEA can be determined to range from 0.01 ng mL-1 to 100 ng mL-1 with a limit of detection of 6.3 pg mL-1. The fabricated immunosensor exhibited high selectivity, and the detection of CEA in fetal bovine serum was achieved.

Electrochemical alcohol oxidation using a TEMPO nitroxide polymer as a homogeneous and surface‐confined catalyst

AbstractPolymers containing TEMPO moieties are effective catalysts for the electrochemical oxidation of alcohols. Such polymers, almost exclusively, are non‐commercial and are prepared using multi‐step synthetic procedures. Here we show that a commercially available TEMPO bearing polymer, Polyamine Immobilised Piperidinyl Oxyl (PIPO), is an effective homogeneous and surface‐confined polymeric catalyst for electrochemical alcohol oxidation at carbonaceous electrodes. We probe electrolytic conditions for effective and stable electrocatalytic alcohol oxidation showing that dichloromethane (DCM), containing tetrabutylammonium perchlorate (TBAP) and N‐methyl imidazole (NMI), is a suitable medium for homogeneous catalysis whilst carbonate buffer (pH 9.5) is better suited when PIPO is adsorbed at the electrode surface. These findings demonstrate the viability of PIPO as an effective and accessible catalyst for electrochemical alcohol oxidations.

Development of Heteroatomic Constant Potential Method with Application to MXene-Based Supercapacitors.

We describe a method for modeling constant-potential charges in heteroatomic electrodes, keeping pace with the increasing complexity of electrode composition and nanostructure in electrochemical research. The proposed "heteroatomic constant potential method" (HCPM) uses minimal added parameters to handle differing electronegativities and chemical hardnesses of different elements, which we fit to density functional theory (DFT) partial charge predictions in this paper by using derivative-free optimization. To demonstrate the model, we performed molecular dynamics simulations using both HCPM and conventional constant potential method (CPM) for MXene electrodes with Li-TFSI/AN (lithium bis(trifluoromethane sulfonyl)imide/acetonitrile)-based solvent-in-salt electrolytes. Although the two methods show similar accumulated charge storage on the electrodes, the results indicated that HCPM provides a more reliable depiction of electrode atom charge distribution and charge response compared with CPM, accompanied by increased cationic attraction to the MXene surface. These results highlight the influence of elemental composition on electrode performance, and the flexibility of our HCPM opens up new avenues for studying the performance of diverse heteroatomic electrodes including other types of MXenes, two-dimensional materials, metal-organic frameworks (MOFs), and doped carbonaceous electrodes.

Weakly Solvating Few-Layer-Carbon Interface toward High Initial Coulombic Efficiency and Cyclability Hard Carbon Anodes.

The carbonaceous anodes in sodium ion batteries suffer from low initial Coulombic efficiency (ICE) and poor cyclability due to rampant solid electrolyte interface (SEI) growth. The concept of the weakly solvating electrolyte (WSE) has been popularized for SEI regulation on the anode by adjusting the cation solvation structure. Nevertheless, the effects on the solvation sheath from the electrode/electrolyte interface are ignored in most WSE applications. In this work, we extend the WSE from the bulk electrolyte to the electrolyte/carbon interface. By recycling asphalt wastes into sp2 C enriched few-layer carbon on hard carbon, a weakly solvating interface is fabricated with lower adsorption energy to electrolyte solvent molecules than a pristine anode (-0.89 vs -1.08 eV for Na/diglyme). Accordingly, more anionic groups are attracted into the solvent-weakened solvation sheath during sodiation (2.30 vs 1.96 coordination number for PF6-). The anion-mediated contact ion pairs facilitate a thin, inorganic-rich SEI layer with a homogeneous distribution, which confers a high ICE of 97.9% and a high capacity of 335.6 mA h g-1 at 1 C (89.5% retention, 1000 cycles). The full battery also manifests an energy density of 209 W h kg-1. This interfacial design is applicable in both ether- and ester-based electrolytes, which is promising in cost-effective modification for carbonaceous electrodes.