Stability Of Interface Research Articles

Mitigating Li-Rich Layered Cathode Capacity Loss by Using a Siloxane Electrolyte Additive.

The instability of the electrode-electrolyte interface in high-voltage cathode materials significantly hinders the development of high-energy-density lithium-ion batteries (LIBs). In this study, 1,3-diphenyl-1,1,3,3-tetramethyldisiloxane (DTS) is employed as an electrolyte additive to enhance the cycling stability and capacity retention for Li||LLO (Li-rich layered oxide) batteries operating at 4.8 V. Theoretical calculations show that DTS can preferentially oxidize on the surface of the cathode. The oxidation forms a robust cathode electrolyte interface (CEI) on the LLO surface, significantly mitigating cracking, regeneration, and irreversible phase transitions of the LLO cathode. As anticipated, the Li||LLO batteries with the DTS electrolyte exhibit a capacity retention of 85.4% after 100 cycles at 4.8 V compared to the baseline electrolyte (45.2%). Furthermore, these batteries demonstrate superior capacity retention after 100 cycles at 4.8 V, even with the presence of 1000 ppm of H2O.

Reinforced Li/Garnet Interface by Ceramic Metallization‐Assisted Room‐Temperature Ultrasound Welding

ABSTRACTSolid‐state lithium metal batteries (SSLMBs), heralded as a promising next‐generation energy storage technology, have garnered considerable attention owing to inherent high safety and potential for achieving high energy density. However, their practical deployment is hindered by the formidable interfacial challenges, primarily stemming from the poor wettability, (electro) chemical instability, and discontinuous charge/mass transport between solid‐state electrolytes and Li metal. To overcome these obstacles, taking garnet‐based electrolyte (Li6.5La3Zr1.5Ta0.5O12, LLZTO) as a pathfinder, the ceramic metallization‐assisted room‐temperature ultrasound werlding (UW) has been developed to reinforce the Li/LLZTO interface. This ultrasound welding approach constructs a compact interface that facilitates rapid Li+/e− transport, while the formation of Li−M (M = Au, Ag, and Sn) alloy homogenizes the distribution of Li+/e− at the interface. By optimization, the atomic‐level contact achieved by ultrasound welding, coupled with a nanosized Au modification layer, significantly reduces the Li/LLZTO interfacial resistance to 5.4 Ω cm2, a marked decrease compared to the resistance achieved by static pressing methods (1727 Ω cm2). The symmetric cell exhibits a high critical current density of 1 mA cm−2 and sustains long‐term stability for over 1600 h at 0.3 mA cm−2, with a Li plating/stripping overpotential of < 45 mV. By incorporating a robust anode‐side interface into solid‐state lithium metal batteries, the LiFePO4‐based full battery contributes 118.4 mAh g⁻1 after 600 cycles at 1 C (capacity: ∼100%). This study offers a facile and effective approach to bolster the interfacial stability between Li and solid‐state electrolytes, paving the way for the development of high‐performance solid‐state lithium metal batteries.

Ion Redistribution Gel Electrolyte Dissipates Interfacial Turbulence for Aqueous Zinc‐Ion Batteries

AbstractAqueous zinc‐ion batteries (AZBs) degrade under a high current density due to the existence of interfacial turbulence with severe concentration polarization. Herein, an ion redistribution gel electrolyte is introduced to stabilize the electrode‐electrolyte interface by regulating the ion density gradient. Negatively charged carboxymethyl groups in carboxymethyl starch ether polymer (PCMS) electrolytes can preferentially regulate the ion concentration at the anode interface. The quasi‐solid PCMS gel electrolytes can dissipate the charge accumulation caused by ion concentration differences, which is beneficial for achieving excellent electrochemical stability at high current densities. As a result, the symmetric Zn cells with PCMS gel electrolyte can be cycled for more than 2000 h at a high current density of 40 mA cm−2. Furthermore, the Zn//I2 cell using PCMS gel electrolyte also sustained cycling for over 8000 cycles, and the pouch cell with PCMS gel electrolyte exhibited practical deformable applications in flexible devices. This work highlights an effective gel electrolyte approach for enhancing interfacial stability, potentially advancing the development of highly reversible AZBs.

Interfacial instability in a viscoelastic microfluidic coflow system

Understanding interfacial instability in a coflow system has relevance in the effective manipulation of small objects in microfluidic applications. We experimentally elucidate interfacial instability in stratified coflow systems of Newtonian and viscoelastic fluid streams in microfluidic confinements. By performing a linear stability analysis, we derive equations that describe the complex wave speed and the dispersion relationship between wavenumber and angular frequency, thus categorizing the behaviour of the systems into two main regimes: stable (with a flat interface) and unstable (with either a wavy interface or droplet formation). We characterize the regimes in terms of the capillary numbers of the phases in a comprehensive regime plot. We decipher the dependence of interfacial instability on fluidic parameters by decoupling the physics into viscous and elastic components. Remarkably, our findings reveal that elastic stratification can both stabilize and destabilize the flow, depending on the fluid and flow parameters. We also examine droplet formation, which is important for microfluidic applications. Our findings suggest that adjusting the viscous and elastic properties of the fluids can control the transition between wavy and droplet-forming unstable regimes. Our investigation uncovers the physics behind the instability involved in interfacial flows of Newtonian and viscoelastic fluids in general, and the unexplored behaviour of interfacial waves in stratified liquid systems. The present study can lead to a better understanding of the manipulation of small objects and production of droplets in microfluidic coflow systems.

Self‐Assembled Monolayer in Hybrid Quasi‐Solid Electrolyte Enables Boosted Interface Stability and Ion Conduction

AbstractComplex interactions between the inorganic solid electrolyte (ISE) and the liquid electrolyte (LE) give rise to challenges of achieving durable interface stability in hybrid quasi‐solid electrolytes (HQSE), and the influence on the involved ISE surface ionic conductivity also needs to be investigated. Here, 4‐chlorobenzenesulfonic acid (CBSA) is utilized to establish a self‐assembled monolayer (SAM) on the surface of Li6.4La3Zr1.4Ta0.6O12 (LLZTO), which is then incorporated into PEGDA‐based in situ polymerized HQSE. The results show that the introduction of CBSA significantly improves the LLZTO/LE interface stability with the optimized solvation structure, resulting in a favorable ionic conductivity (1.19 mS⋅cm−1) and an increasing Li+ transference number (0.647). Mechanisms for the promotion of ionic conduction and interfacial stability of SAM‐HQSE are unveiled through the density functional theory (DFT) combined with Raman spectra and 7Li solid‐state nuclear‐magnetic‐resonance. There are no short‐circuits in the Li|SAM‐HQSE|Li cells after 1000 h. The LFP|SAM‐HQSE|Li cells or LFP|SAM‐HQSE|Graphite pouch cells respectively achieve the capacity retention of 91.2 % and 87.0 % with the 0.5.C‐rate for 500 and 300 cycles. This facile and effective strategy proposed in this work make it accessible for constructing the stable surface micro‐environments of LLZTO where boost and homogenize the Li+ conduction in a hybrid quasi‐solid electrolyte system.

Metal‐Organic Coordination Enhanced Metallopolymer Electrolytes for Wide‐Temperature Solid‐State Lithium Metal Batteries

The practical application of polymer electrolytes is seriously hindered by the inferior Li+ ionic conductivity, low Li+ transference number (tLi+), and poor interfacial stability. Herein, a structurally novel metallopolymer is designed and synthesized by exploiting a molybdenum (Mo) paddle‐wheel complex as a tetratopic linker to bridge organic and inorganic moieties at molecular level. The prepared metallopolymer possesses combined merits of outstanding mechanical and thermal stability, as well as a low glass transition temperature (Tg < –50 °C). Based on this metallopolymer, an advanced metal‐organic coordination enhanced metallopolymer electrolyte (MPE) is developed for constructing high‐performance solid‐state lithium metal batteries (LMBs). Due to the unsaturated coordination of Mo atoms, the uniformly distributed Mo‐polyoxometalates (Mo‐POMs) in metallopolymer skeleton can effectively bis(fluorosulfonyl)imide anions (FSI‐) and promote the dissociation of Li salts. Moreover, dynamic metal‐organic coordination bonds endow the MPE with re‐processability and self‐healing, enabling it to accommodate electrode volume changes and maintain good interfacial contact. Consequently, the MPE achieves a competitive ionic conductivity of 0.712 mS cm‐1 (25 °C), a high tLi+ (0.625), and a wide electrochemical stability window (> 5.0 V). This study presents a unique MPE design based on metal‐organic coordination enhanced strategy, providing a promising solution for developing wide‐temperature solid‐state LMBs.

Metal-Organic Coordination Enhanced Metallopolymer Electrolytes for Wide-Temperature Solid-State Lithium Metal Batteries.

The practical application of polymer electrolytes is seriously hindered by the inferior Li+ ionic conductivity, low Li+ transference number (tLi+), and poor interfacial stability. Herein, a structurally novel metallopolymer is designed and synthesized by exploiting a molybdenum (Mo) paddle-wheel complex as a tetratopic linker to bridge organic and inorganic moieties at molecular level. The prepared metallopolymer possesses combined merits of outstanding mechanical and thermal stability, as well as a low glass transition temperature (Tg < -50 °C). Based on this metallopolymer, an advanced metal-organic coordination enhanced metallopolymer electrolyte (MPE) is developed for constructing high-performance solid-state lithium metal batteries (LMBs). Due to the unsaturated coordination of Mo atoms, the uniformly distributed Mo-polyoxometalates (Mo-POMs) in metallopolymer skeleton can effectively bis(fluorosulfonyl)imide anions (FSI-) and promote the dissociation of Li salts. Moreover, dynamic metal-organic coordination bonds endow the MPE with re-processability and self-healing, enabling it to accommodate electrode volume changes and maintain good interfacial contact. Consequently, the MPE achieves a competitive ionic conductivity of 0.712 mS cm-1 (25 °C), a high tLi+ (0.625), and a wide electrochemical stability window (> 5.0 V). This study presents a unique MPE design based on metal-organic coordination enhanced strategy, providing a promising solution for developing wide-temperature solid-state LMBs.

Stabilization Strategies of Buried Interface for Efficient SAM‐Based Inverted Perovskite Solar Cells

AbstractIn recent years, self‐assembled monolayers (SAMs) anchored on metal oxides (MO) have greatly boosted the performance of inverted (p‐i‐n) perovskite solar cells (PVSCs) by serving as hole‐selective contacts due to their distinct advantages in transparency, hole‐selectivity, passivation, cost‐effectiveness, and processing efficiency. While the intrinsic monolayer nature of SAMs provides unique advantages, it also makes them highly sensitive to external pressure, posing a significant challenge for long‐term device stability. At present, the stability issue of SAM‐based PVSCs is gradually attracting attention. In this minireview, we discuss the fundamental stability issues arising from the structural characteristics, operating mechanisms, and roles of SAMs, and highlight representative works on improving their stability. We identify the buried interface stability concerns in three key aspects: 1) SAM/MO interface, 2) SAM inner layer, and 3) SAM/perovskite interface, corresponding to the anchoring group, linker group, and terminal group in the SAMs, respectively. Finally, we have proposed potential strategies for achieving excellent stability in SAM‐based buried interfaces, particularly for large‐scale and flexible applications. We believe this review will deepen understanding of the relationship between SAM structure and their device performance, thereby facilitating the design of novel SAMs and advancing their eventual commercialization in high‐efficiency and stable inverted PVSCs.

Constructing a Li2O/LiZn Mixed Ionic Electron Conductive Layer by Ultrasonic Spraying to Enhance Li/Garnet Solid Electrolyte Interface Stability for Solid-State Batteries.

Garnet-type Li6.25Ga0.25La3Zr2O12(LGLZO) is believed to be a promising solid electrolyte for solid-state batteries due to its high ionic conductivity, safety, and good stability toward Li. However, one of the most challenges in practical application of LGLZO is the poor contact between Li and LGLZO. Herein, a ZnO layer is prepared on the surface of LGLZO pellet by ultrasonic spraying. Then, a Li2O/LiZn mixed ionic and electron conductive (MIEC) layer is formed at the Li/LGLZO interface via the conversion reaction between ZnO and molten Li. Experiments and theoretical calculations reveal that this MIEC layer can simultaneously improve interface contact, optimize interfacial kinetics, and guide homogeneous Li deposition. As a result, the interface impedance decreases significantly to 36 Ω cm2, the critical current density (CCD) can reach as high as 2.15 mA cm-2, and the Li/ZnO@LGLZO/LiFePO4 all-solid-state cells stably cycle 100 times at 0.5 C. This simple and effective approach may provide a viable strategy for improving the cycle performance of solid lithium metal batteries.

A Solid Electrolyte Based on Sodium-Doped Li4-xNaxTi5O12 with PVDF for Solid State Lithium Metal Battery.

Solid-state batteries (SSBs) present a potential pathway for advancing next-generation lithium batteries, characterized by exceptional energy density and enhanced safety performance. Solid-state electrolytes have been extensively researched, yet an affordable option with outstanding electrochemical performance is still lacking. In this work, Li4-xNaxTi5O12 (LNTO)-based composite solid electrolytes (CSEs) were developed to enhance the interface stability and electronic insulation. The CSE is composed of Li3.88Na0.12Ti5O12 (LNTO3) and poly (vinylidene fluoride) (PVDF) with a proportion of 20 wt % exhibited high ionic conductivity (4.49×10-4 S cm-1 at a temperature value equal to 35 °C), high ionic transfer number (equal to 0.72), low activation energy (equal to 0.192 eV), and favorable compatibility with the Li metal anode. The Li|LNTO3|LiFePO4 cell, tested at a 0.5 C current density, demonstrated 154.5 mAh g-1 of outstanding cycling stability for 200 cycles, capacity retention of 97.6 % along with a Coulombic efficiency of over 99 %, as well as a significant average specific capacity of 127.8 mAh g-1 over 400 cycles at 5 C. The Li|LNTO3|LiNi0.8Co0.1Mn0.1O2 (NCM811) cell could also operate over 100 cycles at 1 C. This study offers an effective method for preparing commercial CSEs for SSBs.

Buried hole-selective interface engineering for high-efficiency tin-lead perovskite solar cells with enhanced interfacial chemical stability

Mixed Sn-Pb perovskites are attracting significant attention due to their narrow bandgap and consequent potential for all-perovskite tandem solar cells. However, the conventional hole transport materials can lead to band misalignment or induce degradation at the buried interface of perovskite. Here we designed a self-assembled material 4-(9H-carbozol-9-yl)phenylboronic acid (4PBA) for the surface modification of the substrate as the hole-selective contact. It incorporates an electron-rich carbazole group and conjugated phenyl group, which contribute to a substantial interfacial dipole moment and tune the substrate’s energy levels for better alignment with the Sn-Pb perovskite energy levels, thereby promoting hole extraction. Meanwhile, enhanced perovskite crystallization and improved contact at bottom of the perovskite minimized defects within perovskite bulk and at the buried interface, suppressing non-radiative recombination. Consequently, Sn-Pb perovskite solar cells using 4PBA achieved efficiencies of up to 23.45%. Remarkably, 4PBA layer provided superior interfacial chemical stability, and effectively mitigated device degradation. Unencapsulated devices retained 93.5% of their initial efficiency after 2000 h of shelf storage.

Anode interface-stabilizing dry process employing a binary binder system for ultra-thick and durable battery electrode fabrication

Polytetrafluoroethylene (PTFE)-based dry process has gained attention in the battery industry owing to their sustainability, cost-effectiveness, and ability to fabricate high loading electrodes. However, the electrochemical instability of PTFE in anodic environments causes significant capacity loss, hindering the development of high-performance dry-processed anodes. In this study, a binary binder system of PTFE and polyvinylpyrrolidone (PVP) is proposed to prevent direct contact between graphite and PTFE, mitigating unwanted interphase evolution. This strategy improves the mechanical integrity of the electrode. It maintains the binding force between the active materials and PTFE binders. PVP also forms a robust inorganic-rich SEI, enhancing Li-ion kinetics and interfacial stability. Consequently, dry-processed graphite with PVP achieved ultra-high loading anodes (∼10 mAh cm−2) with excellent cycle stability over 200 cycles in full cells coupled with LiNi0.8Co0.1Mn0.1O2 cathodes. This paper presents a cost-effective, high-loading electrode fabrication process and an eco-friendly approach for large-scale electrification.

In-situ construction of VN-based heterostructure with high interfacial stability and porous channel effect for efficient zinc ion storage

In-situ construction of VN-based heterostructure with high interfacial stability and porous channel effect for efficient zinc ion storage

Enhanced strength and ductility of boron nitride nanosheet reinforced cu composites through constructing an interfacial three-dimensional structure

To address the poor wettability and weak interface bonding between boron nitride nanosheet (BNNS) and Cu, BNNS/CuTi composites were prepared through matrix microalloying by adding 1 wt% Ti. Solid-state interfacial reactions resulted in the formation of TiN transition layers and TiB whiskers (TiBw), collectively constructed a BNNS-(TiN&TiB)-Cu interfacial three-dimensional structure (I-3DS). The coherent I-3DS significantly reduced the interfacial energy, improved the interfacial stability, and achieved a favorable combination of strength and ductility in BNNS/CuTi composites. The 0.1 wt% BNNS/CuTi composite achieved an ultimate tensile strength (UTS) of 485 MPa, representing increases of 114 % and 62 % over pure Cu and 0.1 wt% BNNS/Cu composite, respectively. The interlocking structure formed by I-3DS and Cu doubled the theoretical interface shear strength limit and improved load transfer efficiency. This study offered new insights into the innovative design of high-performance Cu matrix composites (CMCs) by constructing I-3DS.

Dynamic analysis of the air–water interface instability in a wind-wave flume: Initial conditions for wave generation

This paper aims to investigate the dynamic mechanism for a previously calm water surface under a background wind field, which would lose stability due to minor perturbations. When spatial distribution and growth rate of the shear wind field satisfy a certain relationship, an Orr–Sommerfeld equation can be derived from linearized Navier–Stokes equations, for the amplitude of perturbation waves at the air–water interface. After transforming its coordinates to a finite interval, this fourth-order linear ordinary differential equation with variable coefficients can turn into a linear singular differential equation. It is solved under the background flow fields of air and water using the corrected Fourier method that we previously developed, to yield two sets of four analytical solutions with physical significance. The perturbation flow at the air–water interface must satisfy the kinematic and dynamic matching conditions (continuity of velocity and smooth transition of shear stress), which results in a fourth-order homogeneous linear algebraic equation for four undetermined constants. Setting various parameters in accordance with measured data with a wind-wave flume, the corresponding perturbation waves solution is identified. Our calculation densely distributes the most unstable and readily growing waves among perturbation waves with small phase speeds, consistent with the experimental results. Our perturbation solutions over a flat air–water interface are only applicable to the short period after instability onset, which provides an initial condition for wave generation. The consequent interaction between small-amplitude waves and wind field is beyond the scope of our linear theory, which has indeed been sufficiently addressed in the literature.

Bubble dynamics in liquid metals under external horizontal magnetic field

In this study, computational fluid dynamics simulation was used to derive full understanding of a bubble rising in liquid metals with the presence of an external horizontal magnetic field. The major aim of the study was to develop new correlations for bubble velocity and stability in liquid metals. In-house code PSI-BOIL (Parallel SImulator of BOILing phenomena, developed by Paul Scherrer Institute, Switzerland) has been used for the simulations. Single bubble rising in quiescent liquid is simulated for three different sets of materials (nitrogen+mercury, argon+GalnSn, and argon+steel). The influence of external horizontal magnetic field on bubble dynamics is analyzed, and vertical magnetic field is not considered in this study. Overall, results show that horizontal magnetic field reduces bubble rising velocity, straightens the bubble trajectory, and enhances bubble interface stability.

Scientometric Insights into Rechargeable Solid-State Battery Developments

Solid-state batteries (SSBs) offer significant improvements in safety, energy density, and cycle life over conventional lithium-ion batteries, with promising applications in electric vehicles and grid storage due to their non-flammable electrolytes and high-capacity lithium metal anodes. However, challenges such as interfacial resistance, low ionic conductivity, and manufacturing scalability hinder their commercial viability. This study conducts a comprehensive scientometric analysis, examining 131 peer-reviewed SSB research articles from IEEE Xplore and Web of Science databases to identify key thematic areas and bibliometric patterns driving SSB advancements. Through a detailed analysis of thematic keywords and publication trends, this study uniquely identifies innovations in high-ionic-conductivity solid electrolytes and advanced cathode materials, providing actionable insights into the persistent challenges of interfacial engineering and scalable production, which are critical to SSB commercialization. The findings offer a roadmap for targeted research and strategic investments by researchers and industry stakeholders, addressing gaps in long-term stability, scalable production, and high-performance interface optimization that are currently hindering widespread SSB adoption. The study reveals key advances in electrolyte interface stability and ion transport mechanisms, identifying how solid-state electrolyte modifications and cathode coating methods improve charge cycling and reduce dendrite formation, particularly for high-energy-density applications. By mapping publication growth and clustering research themes, this study highlights high-impact areas such as cycling stability and ionic conductivity. The insights from this analysis guide researchers toward impactful areas, such as electrolyte optimization and scalable production, and provide industry leaders with strategies for accelerating SSB commercialization to extend electric vehicle range, enhance grid storage, and improve overall energy efficiency.

Impact of Self-Assembled Monolayer Structural Design on Perovskite Phase Regulation, Hole-Selective Contact, and Energy Loss in Inverted Perovskite Solar Cells

Recent studies have shown that self-assembled molecule (SAM)-based hole-selective contacts (HSCs) offer a promising solution to the challenges faced by perovskite solar cells (PVSCs), including minimal material consumption, scalable production, high interface stability, and the use of environmentally friendly solvents. In this study, the efficacy of two designs of SAMs (Cz and PA) as HSCs in inverted PVSCs was investigated by comparing them with the conventional MeO-2PACz (MeO) SAM. Surface analyses showed that the surface of PA is smoother than that of Cz, which helps to reduce interfacial defects. Subsequent perovskite deposition exhibited a reduced formation of the PbI2 phase, incidiating that its phase modulation ability is superior to that of MeO. Further analyses demonstrate the superior charge extraction ability of PA as a result of reduced interfacial defects and non-radiative recombination at the HSC/perovskite interface. By further coupling with phenethylammonium iodide (PEAI) surface passivation, both interfaces of the perovskite film were optimized and the inverted ((FAPbI3)0.85(MAPbBr3)0.15)0.95(CsPbI3)0.05 (bandgap = 1.62eV) PVSC achieves a high power conversion efficiency (PCE) of 23.3% and a very high open-circuit voltage of 1.227V due to the largely reduced energy loss. In addition, the PA PVSC exhibits enhanced long-term thermal stability at 85°C in a nitrogen atmosphere.

Soft interface instability and gas flow channeling in low-permeability deformable media

Understanding gas percolation through a clay layer or a shale formation is of great importance for the development of a geologic repository for nuclear waste disposal, a subsurface system for gas storage, and an engineering approach for hydrocarbon extraction from unconventional reservoirs. Gas injection experiments have revealed complex dynamic behaviours of gas percolation through water saturated compacted bentonite, characterized by a high breakthrough pressure, rapid breakthrough, a pressure/stress decay after the breakthrough, a relatively high migration rate, high-frequency periodic/nonperiodic variations in flow rate, stepwise rate reductions during relaxation, and low gas saturation over the whole process, all indicating channelling nature of the processes. Using linear stability analyses, we show that this channelling can autonomously emerge from the instability of the deformable interface between the injected gas and the compacted bentonite matrix driven by local stress concentration, pore dilation, and hydrologic gradient. Channel patterns formed would possess a fractal geometry. We further show that, once a percolating channel is established, the gas injected would percolate through the channel in a chain of gas bubbles, also due to the interface instability, resulting in periodic/chaotic variations in gas flow rate. Our work provides a unified explanation for key features observed for gas percolation in low-permeability deformable media. The work also suggests a possibility of designing an engineered barrier system for a nuclear waste repository that can have controllable gas release while limit water transport.

Study on improving the performance of engineered cement-based composites by modifying binder system and polyethylene fiber/matrix interface

In this study, cement, rice husk ash (RHA), silica fume, mineral powder and fly ash were used as multi-component cementing materials, and the polyethylene (PE) fiber was modified by cellulose nanocrystal (CNC) to develop an Engineered Cementitious Composites (ECC) with high ductility and strength. The hydration heat and X-ray diffractometer (XRD) results indicate that RHA delays the early hydration of cement, its pozzolanic effect refines the internal porosity of hydration matrix and improves the compactness of ECC samples. Moreover, RHA increases the interfacial properties between fiber and cement matrix, reduces the first cracking strength and significantly improves the tensile strain rate of ECC. With the increasing content of RHA, its reinforcement effect becomes more obviously. The strain rate of ECC samples that uses RHA to replace 40 % of cement can reach 6.81 %. However, once the content of RHA is too high, the quality of cement involved in hydration will be significantly weakened, which reduces the amount of hydration products and has a negative impact on the compressive strength. By CNC coating, the active groups can be coated to the fiber surface to improve the fiber’s wettability. Which has promoted the growth of hydration products on the fiber surface, enhancing the fiber/matrix interface properties, and improved the ductility of ECC. CNC coating can also make up for the loss of compressive strength caused by RHA. The molecular dynamics simulation results show that unmodified PE fiber hardly to form a stable bond with C-S-H. However, CNC can adsorb with C-S-H through hydrogen and Ca-O bonding, and can also interaction with PE fiber by hydrogen bonding. Herein, CNC acts as an intermediate to connect PE and C-S-H, increase the interface stability of fiber/cement matrix, improve the interface bonding, and thus enhance the ductility of ECC. Developing multi-binder system and reinforced fiber/interface can significantly reduce the amount of cement used in ECC, and understanding the enhancement mechanism is beneficial to guide the optimal design of ECC.