Lightweight and drift-free magnetically actuated millirobots via asymmetric laser-induced graphene.

Millirobots must have low cost, efficient locomotion, and the ability to track target trajectories precisely if they are to be widely deployed. With current materials and fabrication methods, achieving all of these features in one millirobot remains difficult. We develop a series of graphene-based helical millirobots by introducing asymmetric light pattern distortion to a laser-induced polymer-to-graphene conversion process; this distortion resulted in the spontaneous twisting and peeling off of graphene sheets from the polymer substrate. The lightweight nature of graphene in combine with the laser-induced porous microstructure provides a millirobot scaffold with a low density and high surface hydrophobicity. Magnetically driven nickel-coated graphene-based helical millirobots with rapid locomotion, excellent trajectory tracking, and precise drug delivery ability were fabricated from the scaffold. Importantly, such high-performance millirobots are fabricated at a speed of 77 scaffolds per second, demonstrating their potential in high-throughput and large-scale production. By using drug delivery for gastric cancer treatment as an example, we demonstrate the advantages of the graphene-based helical millirobots in terms of their long-distance locomotion and drug transport in a physiological environment. This study demonstrates the potential of the graphene-based helical millirobots to meet performance, versatility, scalability, and cost-effectiveness requirements simultaneously.

Wood-inspired anisotropic hydrogel electrolyte with large modulus and low tortuosity realizing durable dendrite-free zinc-ion batteries.

While aqueous zinc-ion batteries exhibit great potential, their performance is impeded by zinc dendrites. Existing literature has proposed the use of hydrogel electrolytes to ameliorate this issue. Nevertheless, the mechanical attributes of hydrogel electrolytes, particularly their modulus, are suboptimal, primarily ascribed to the substantial water content. This drawback would severely restrict the dendrite-inhibiting efficacy, especially under large mass loadings of active materials. Inspired by the structural characteristics of wood, this study endeavors to fabricate the anisotropic carboxymethyl cellulose hydrogel electrolyte through directional freezing, salting-out effect, and compression reinforcement, aiming to maximize the modulus along the direction perpendicular to the electrode surface. The heightened modulus concurrently serves to suppress the vertical deposition of the intermediate product at the cathode. Meanwhile, the oriented channels with low tortuosity enabled by the anisotropic structure are beneficial to the ionic transport between the anode and cathode. Comparative analysis with an isotropic hydrogel sample reveals a marked enhancement in both modulus and ionic conductivity in the anisotropic hydrogel. This enhancement contributes to significantly improved zinc stripping/plating reversibility and mitigated electrochemical polarization. Additionally, a durable quasi-solid-state Zn//MnO2 battery with noteworthy volumetric energy density is realized. This study offers unique perspectives for designing hydrogel electrolytes and augmenting battery performance.

Biomimetic Electronic Skin Based on a Stretchable Ionogel Mechanoreceptor Composed of Crumpled Conductive Rubber Electrodes for Synchronous Strain, Pressure, and Temperature Detection.

Electronic skin (e-skin) is showing a huge potential in human-computer interaction, intelligent robots, human health, motion monitoring, etc. However, it is still challenging for e-skin to realize distinguishable detection of stretching strain, vertical pressure, and temperature through a simple noncoupling structure design. Here, a stretchable multimodal biomimetic e-skin was fabricated by integrating layer-by-layer self-assembled crumpled reduced graphene oxide/multiwalled carbon nanotubes film on natural rubber (RGO/MWCNTs@NR) as stretchable conductive electrodes and polyacrylamide/NaCl ionogel as a dielectric layer into an ionotropic capacitive mechanoreceptor. Unlike natural skin receptors, the sandwich-like stretchable ionogel mechanoreceptor possessed a distinct ionotropic capacitive behavior for strain and pressure detection. The results showed that the biomimetic e-skin displayed a negative capacitance change with superior stretchability (0-300%) and a high gauge factor of 0.27 in 180-300% strain, while exhibiting a normal positive piezo-capacitance behavior in vertical pressure range of 0-15 kPa with a maximal sensitivity of 1.759 kPa-1. Based on this feature, the biomimetic e-skin showed an excellent synchronous detection capability of planar strain and vertical pressure in practical wearable applications such as gesture recognition and grasping movement detection without a complicated mathematical or signal decoupling process. In addition, the biomimetic e-skin exhibited a quantifiable linear responsiveness to temperature from 20-90 °C with a temperature coefficient of 0.55%/°C. These intriguing properties gave the biomimetic e-skin the ability to perform a complete function similar to natural skin but beyond its performance for future wearable devices and artificial intelligence devices.

Quasi-Hyperbolic Framework Graphite Foam-Based Composites with High Thermal Conductivity and Electromagnetic Shielding Properties Fabricated by an Electrochemical Expansion Method.

Nowadays, the rapid development of electronic devices requires composites with high thermal conductivity and good electromagnetic shielding properties. The key challenge lies in the construction of high-performance conductive networks. Herein, an electrochemical expansion graphite foam (EEG) with a quasi-hyperbolic framework was prepared by an electrochemical expansion method, and then the epoxy resin (EP) was filled to fabricate the composites. The graphite plate was first electrochemically intercalated and then foamed, in which plasticization was caused by weak oxidation in intercalation and the quasi-hyperbolic framework was induced by foaming during expansion. These processes were characterized by Fourier transform infrared (FTIR), micro-Raman, X-ray photoelectron spectroscopy (XPS), and so on. Based on the highly efficient quasi-hyperbolic framework and high-quality graphite structure, the thermal conductivity of the composite reached 43.523 W/(m·K), and total electromagnetic interference (EMI) shielding (SET) reached 105 dB. The heat transfer behavior was simulated by finite element analysis (FEA) in detail. This method of preparing high thermal conductivity and electromagnetic shielding materials has a good application prospect.

Suppressing Rampant and Vertical Deposition of Cathode Intermediate Product via PH Regulation Toward Large-Capacity and High-Durability Zn//MnO2 Batteries.

Despite great prospects, Zn//MnO2 batteries suffer from rampant and vertical deposition of zinc sulfate hydroxide (ZSH) at the cathode surface, which leads to a significant impact on their electrochemical performance. This phenomenon is primarily due to the drastic increase in the electrolyte pH value upon discharging, which is closely associated with the electrodissolution of Mn-based active materials. Herein, the pH value change is effectively inhibited by employing an electrolyte additive with excellent pH buffering capability. As such, the formation of ZSH at the cathode is postponed, resulting in the deposition of ZSH in a horizontal arrangement. This strategy can significantly enhance the utilization efficiency of cathode active material, while also enabling a solid electrolyte interphase layer at the Zn anode to address low Zn stripping/plating reversibility. With the optimal electrolyte, the Zn//MnO2 battery realizes a 25.6% increase in the specific capacity at 0.2 A g-1 compared to that with the baseline electrolyte, great rate capability (161.6 mAh g-1 at 5 A g-1 ), and superior capacity retention (90.2% over 5,000 cycles). In addition, the pH buffering strategy is highly applicable in hydrogel electrolytes. This work underscores the importance of pH regulation for Zn//MnO2 batteries and provides enlightening insights.

A General Strategy for Ordered Carrier Transport of Quasi-2D and 3D Perovskite Films for Giant Self-Powered Photoresponse and Ultrahigh Stability.

Organic-inorganic hybrid perovskite materials have been focusing more attention in the field of self-powered photodetectors due to their superb photoelectric properties. However, a universal growth approach is required and challenging to realize vertically oriented growth and grain boundary fusion of 2D and 3D perovskite grains to promote ordered carrier transport, which determines superior photoresponse and high stability. Herein, a general thermal-pressed (TP) strategy is designed to solve the above issues, achieving uniaxial orientation and single-grain penetration along the film thickness direction. It constructs the efficient channel for ordered carrier transport between two electrodes. Combining of the improved crystal quality and lower trap-state density, the quasi-2D and 3D perovskite-based self-powered photodetector devices (with/without hole transport layer) all exhibit giant and stable photoresponse in a wide spectrum range and specific wavelength laser. For the MAPbI3-based self-powered photodetectors, the largest Rλ value is as high as 0.57 A W-1 at 760 nm, which is larger than most reported results. Meanwhile, under laser illumination (532 nm), the FPEA2MA4Pb5I16-based device exhibits a high responsivity (0.4 A W-1) value, which is one of the best results in 2DRP self-powered photodetectors. In addition, fast response, ultralow detection limit, and markedly improved humidity, optical and heat stabilities are clearly demonstrated for these TP-based devices.

Regulating the Electrical and Mechanical Properties of TaS2 Films via van der Waals and Electrostatic Interaction for High Performance Electromagnetic Interference Shielding.

Low-dimensional transition metal dichalcogenides (TMDs) have unique electronic structure, vibration modes, and physicochemical properties, making them suitable for fundamental studies and cutting-edge applications such as silicon electronics, optoelectronics, and bioelectronics. However, the brittleness, low toughness, and poor mechanical and electrical stabilities of TMD-based films limit their application. Herein, a TaS2 freestanding film with ultralow void ratio of 6.01% is restacked under the effect of bond-free van der Waals (vdW) interactions within the staggered 2H-TaS2 nanosheets. The restacked films demonstrated an exceptionally high electrical conductivity of 2,666 S cm-1, electromagnetic interference shielding effectiveness (EMI SE) of 41.8 dB, and absolute EMI SE (SSE/t) of 27,859 dB cm2 g-1, which is the highest value reported for TMD-based materials. The bond-free vdW interactions between the adjacent 2H-TaS2 nanosheets provide a natural interfacial strain relaxation, achieving excellent flexibility without rupture after 1,000 bends. In addition, the TaS2 nanosheets are further combined with the polymer fibers of bacterial cellulose and aramid nanofibers via electrostatic interactions to significantly enhance the tensile strength and flexibility of the films while maintaining their high electrical conductivity and EMI SE.This work provides promising alternatives for conventional materials used in EMI shielding and nanodevices.

Laser-Induced Transient Self-Organization of TiNx Nano-Filament Percolated Networks for High Performance Surface-Mountable Filter Capacitors.

Filter capacitors (FCs) are substantial for digital circuits and microelectronic devices, and thus more compact FCs are eternally demanded for system miniaturization. Even though microsupercapacitors are broadly regarded as an excellent candidate for future FCs, yet due to the limitation of available electrode materials, the capacitive performance of reported MSCs drops sharply under high-frequency alternating current. Herein, we present a unique laser-induced transient self-organization strategy, which synergizes pulsed laser energy and multi-physical field controlled coalescence processes, leading to the rapid and controllable preparation of titanium nitride ultrafine nano-filaments (diameter ≈3-5 nm) networks. Their chaotic fractal nanoporous structure, superior specific surface area, and excellent conductivity render these nanostructures promising candidates for FCs. Surface-mounted filter capacitors based on this electrode material exhibit ultra-long cycle-life (2 000 000 cycles) with record ultrahigh volumetric energy density of 9.17 mWh cm-3 at 120 Hz in aqueous electrolyte, displaying advantages in function, size, and integrability compared with the state-of-the-art aluminum electrolytic capacitors. The method here provides a versatile toolbox for designing novel nanostructures with intriguing characteristics and insights for developing advanced and miniaturized filter and power devices.

Melamine-graphene epoxy nanocomposite based die attach films for advanced 3D semiconductor packaging applications.

With the ultra-fast development of personal portable electronic devices, it is important to explore new die attach film (DAF) materials in the limited mounting area and height in order to meet the requirements of a high packaging density and a high operating speed. Graphene-based epoxy nanocomposites are becoming one of the most promising candidates for the next generation of DAFs combining the ultra-high thermal conductivity of graphene, and ultra-strong adhesion of epoxy polymers. However, poor dispersion and weak interfacial connections, due to the overly smooth surface of graphene nanosheets, are still pressing issues that limit their industrial applications. Additionally, pristine graphene nanosheets have only a small effect on improving the glass transition temperature (Tg) of epoxy composites to meet the requirements of DAFs. In this work, melamine-functionalized graphene is synthesized by using a nondestructive ball milling process, which results in greater dispersion and enhancement of the interfacial connections between graphene and epoxy resins demonstrated by both experimental and simulation results. In particular, the aromatic triazine rings of melamine increase Tg in the cured resin, thus improving the thermal stability of DAFs. The melamine-graphene (M-G) epoxy nanocomposites synthesized have a high Tg of 172 °C and an out-of-plane thermal conductivity of 1.08 W m-1 K-1 at 10 wt% loading. This is 6.4 multiples higher than that of neat epoxy. Moreover, M-G epoxy nanocomposites exhibit superb thermal stability, an effective low coefficient of thermal expansion (CTE), low moisture adsorption, and a useful high electrical resistivity. In the DAF performance test, involving experimentation and modeling, the samples present a better cooling capability and heat dissipation. This supports the idea that our findings have potential to be applied in the next generation of DAFs for high-power and high-density 3D packaging.

Electron-Injection and Atomic-Interface Engineering toward Stabilized Defected 1T-Rich MoS2 as High Rate Anode for Sodium Storage.

1T-phase MoS2 is a promising electrode material for electrochemical energy storage due to its metallic conductivity, abundant active sites, and high theoretical capacity. However, because of the habitual conversion of metastable 1T to stable 2H phase via restacking, the poor rate capacity and cycling stability at high current densities hamper their applications. Herein, a synergetic effect of electron-injection engineering and atomic-interface engineering is employed for the formation and stabilization of defected 1T-rich MoS2 nanoflowers. The 1T-rich MoS2 and carbon monolayers are alternately intercalated with each other in the nanohybrids. The metallic 1T-phase MoS2 and conductive carbon monolayers are favorable for charge transport. The expanded interlayer spacing ensures fast electrolyte diffusion and the decrease of the ion diffusion barrier. The obtained defected 1T-rich MoS2/m-C nanoflowers exhibit high Na-storage capacity (557 mAh g-1 after 80 cycles at 0.1 A g-1), excellent rate capacity (411 mAh g-1 at 10 A g-1), and long-term cycling performance (364 mAh g-1 after 1000 cycles at 2 A g-1). Furthermore, a Na-ion full cell composed of the 1T-rich MoS2/m-C anode and Na3V2(PO4)3/C cathode maintains excellent cycling stability at 0.5 A g-1 during 400 cycles. Theoretical calculations are also performed to evaluate the phase stability, electronic conductivity, and Na+ diffusion behavior of 1T-rich MoS2/m-C. The energy storage performance demonstrates its excellent application prospects.

Laser Processing of Flexible In-Plane Micro-supercapacitors: Progresses in Advanced Manufacturing of Nanostructured Electrodes.

Flexible in-plane architecture micro-supercapacitors (MSCs) are competitive candidates for on-chip miniature energy storage applications owing to their light weight, small size, high flexibility, as well as the advantages of short charging time, high power density, and long cycle life. However, tedious and time-consuming processes are required for the manufacturing of high-resolution interdigital electrodes using conventional approaches. In contrast, the laser processing technique enables high-efficiency high-precision patterning and advanced manufacturing of nanostructured electrodes. In this review, the recent advances in laser manufacturing and patterning of nanostructured electrodes for applications in flexible in-plane MSCs are comprehensively summarized. Various laser processing techniques for the synthesis, modification, and processing of interdigital electrode materials, including laser pyrolysis, reduction, oxidation, growth, activation, sintering, doping, and ablation, are discussed. In particular, some special features and merits of laser processing techniques are highlighted, including the impacts of laser types and parameters on manufacturing electrodes with desired morphologies/structures and their applications on the formation of high-quality nanoshaped graphene, the selective deposition of nanostructured materials, the controllable nanopore etching and heteroatom doping, and the efficient sintering of nanometal products. Finally, the current challenges and prospects associated with the laser processing of in-plane MSCs are also discussed. This review will provide a useful guidance for the advanced manufacturing of nanostructured electrodes in flexible in-plane energy storage devices and beyond.

Anisotropic Charge Transport Enabling High-Throughput and High-Aspect-Ratio Wet Etching of Silicon Carbide.

Wet etching of silicon carbide typically exhibits poor etching efficiency and low aspect ratio. In this study, an etching structure that exploits anisotropic charge carrier flow to enable high-throughput, external-bias-free wet etching of high-aspect-ratio SiC micro/nano-structures is demonstrated. Specifically, by applying a catalytic metal coating at the bottom surface of a SiC wafer while introducing patterned ultraviolet light illumination from its top surface, spatial charge separation across the wafer is achieved, i.e., photogenerated electrons are channeled to the bottom to participate in the reduction reaction of an oxidant in the etchant solution, while holes flow to the top to trigger oxidation of SiC and subsequent etching. Such design largely suppresses recombination-induced charge losses, and when used in combination with a top metal catalyst mask, the structure yields a remarkable vertical etching rate of 0.737 µm min-1 and an aspect ratio of 3.2, setting new records for wet-etching methods for SiC.

Difluorobenzylamine Treatment of Organolead Halide Perovskite Boosts the High Efficiency and Stability of Photovoltaic Cells.

As one of the most competitive light-harvesting materials, organometal halide perovskites have attracted great attention due to their low-cost and top-down solution fabricability. However, the instability of perovskites in a moist environment reduces the potential for their commercialization. In this study, novel 2,4-fluorobenzylamine (FBA) was employed as the passivation material, which could successfully suppress the defects and improve the moisture resistance of perovskites, resulting in an ultrahigh power conversion efficiency of 17.6% for the carbon-based perovskite solar cells with good stability. Meanwhile, the whole process of interactions between the H2O molecule and the perovskite lattice was first elucidated by density functional theory calculations, which demonstrated the underlying mechanism of the improvement of moisture stability with the FBA treatment. This work opens up a new route toward addressing the main obstacles in the practical application of perovskite devices under ambient conditions.

One-Step Ultraviolet Laser-Induced Fluorine-Doped Graphene Achieving Superhydrophobic Properties and Its Application in Deicing.

Joule heaters based on flexible thin films have attracted a significant amount of attention in both academia and the industry. However, it has been highly challenging to fabricate such heaters. In this study, a one-step laser induction method was proposed to prepare fluorine-doped laser-induced graphene (F-LIG) with stable and superhydrophobic properties by confining a 355 nm ultraviolet laser at the interface between the fluorinated ethylene propylene (FEP) film and polyimide (PI) film. The superhydrophobic properties of the F-LIG composite films could be attributed to the doping of fluorine elements and the laser-processed microstructures, which could be tuned by laser processing parameters. Based on the processed F-LIG films, Joule deicing heaters were developed and their deicing efficiencies are 7 times higher than that of the undoped LIG-based deicing heater. The method will provide new means and ideas to develop LIG-based flexible devices.

Metallized Skeleton of Polymer Foam Based on Metal-Organic Decomposition for High-Performance EMI Shielding.

Highly conductive polymer foam with light weight, flexibility, and high-performance electromagnetic interference (EMI) shielding is highly desired in the fields of aerospace, communication, and high-power electronic equipment, especially in the board-level packaging. However, traditional technology for preparing conductive polymer foam such as electroless plating and electroplating involves serious pollution, a complex fabrication process, and high cost. It is urgent to develop a facile method for the fabrication of highly conductive polymer foam. Herein, we demonstrated a lightweight and flexible silver-wrapped melamine foam (Ag@ME) via in situ sintering of metal-organic decomposition (MOD) at a low temperature (200 °C) on the ME skeleton modified with poly(ethylene imine). The Ag@ME with a continuous 3D conductive network exhibits good compressibility, an excellent conductivity of 158.4 S/m, and a remarkable EMI shielding effectiveness of 63 dB in the broad frequency of 8.2-40 GHz covering X-, Ku-, K-, and Ka-bands, while the volume content is only 2.03 vol %. The attenuation mechanism of Ag@ME for EM waves is systematically investigated by both EM simulation and experimental analysis. Moreover, the practical EMI shielding application of Ag@ME in board-level packaging is demonstrated and it shows outstanding near-field shielding performance. This novel strategy for fabrication of highly conductive polymer foam with low cost and non-pollution could potentially promote the practical applications of Ag@ME in the field of EMI shielding.

Integration of efficient microwave absorption and shielding in a multistage composite foam with progressive conductivity modular design.

Ultra-efficient electromagnetic interference (EMI) shielding composites with excellent microwave absorbing properties are the most desirable solution for eliminating microwave pollution. However, integrating absorbing and electromagnetic shielding materials is a difficult challenge because they have different design strategies. In this work, the compatibility of high absorption and shielding capability based on progressive conductivity modular design was realized. Reduced graphene oxide@ferroferric oxide/carbon nanotube/tetraneedle-like ZnO whisker@silver/waterborne polyurethane (rGO@Fe3O4/CNT/T-ZnO@Ag/WPU) multistage composite foams with aligned porous structures were fabricated, which exhibited an excellent average EMI SE > 92.3 dB and remarkable microwave absorption performance with reflection loss < -10 dB in the frequency range of 8.2-18.0 GHz. The average shielding effectiveness of reflection (SER) and reflectivity (R) are as low as 0.065 dB and 0.015, respectively. Besides, the correlations between the morphology and structure of the composite foam and the electromagnetic wave attenuation mechanism were established via electromagnetic simulation. Significantly, the integration of efficient absorbing and shielding materials was realized for the first time. Such composite foams with electromagnetic wave absorption and shielding characteristics are light weight and structurally designable with an adjustable shielding mechanism, and exhibit low filler consumption and high performance. They display promising applications in demanding electromagnetic environments. Our work provides a new strategy to design ultra-efficient EMI shielding materials with reliable absorption-dominated features.

Pressure-Enhanced Vertical Orientation and Compositional Control of Ruddlesden-Popper Perovskites for Efficient and Stable Solar Cells and Self-Powered Photodetectors.

It is well-known that two-dimensional Ruddlesden-Popper (2DRP) perovskite has higher stability than three-dimensional counterparts. However, fundamental issues still exist in the vertical orientation and phase composition as well as phase distribution. Here, obvious control of the film quality of 2DRP PEA2MA4Pb5I16 (n = 5) perovskite is demonstrated via a thermal-pressed (TP) effect. The crystallinity, morphology, phase composition, and optoelectronic features unequivocally illustrate that the TP effect achieves a larger gain size, a smoother surface, an effectively vertical orientation, a relatively pure phase with a large n value, a gradient distribution of quantum wells, and enhanced interlayer interaction. These film and interface features lead to markedly enhanced charge transport/extraction and lower trap density. Accordingly, the TP-based perovskite film device delivers a power conversion efficiency of 15.14%, far higher than that of the control film device (11.10%) because of significant improvements in open-circuit voltage and short-circuit current. More importantly, it also presents excellent hydrophobicity, illumination stability, and environmental stability. In addition, the 2D perovskite self-powered photodetector also exhibits high responsivity (0.25 A W-1) and specific detectivity (1.4 × 1012 Jones) at zero bias.

Interfacial Laser-Induced Graphene Enabling High-Performance Liquid-Solid Triboelectric Nanogenerator.

Laser-induced graphene (LIG) has emerged as a promising and versatile method for high-throughput graphene patterning; however, its full potential in creating complex structures and devices for practical applications is yet to be explored. In this study, an in-situ growing LIG process that enables to pattern superhydrophobic fluorine-doped graphene on fluorinated ethylene propylene (FEP)-coated polyimide (PI) is demonstrated. This method leverages on distinct spectral responses of FEP and PI during laser excitation to generate the environment preferentially for LIG formation, eliminating the need for multistep processes and specific atmospheres. The structured and water-repellant structures rendered by the spectral-tuned interfacial LIG process are suitable as the electrode for the construction of a flexible droplet-based electricity generator (DEG), which exhibits high power conversion efficiency, generating a peak power density of 47.5 W m-2 from the impact of a water droplet 105 µL from a height of 25 cm. Importantly, the device exhibits superior cyclability and operational stability under high humidity and various pH conditions. The facile process developed can be extended to realize various functional devices.

The in vivo dissolution of tricalcium silicate bone cement.

This study aimed to investigate the in vivo dissolution of tricalcium silicate (Ca3 SiO5 , C3 S) bone cement in the rabbit femoral defect. Results indicated that C3 S paste directly integrated with the bone tissue without the protection of the bone-like apatite. Calcium silicate hydrate gel (C-S-H gel) and Ca(OH)2 were the main components of C3 S paste. The dissolution model of C3 S paste was a mass loss rather than a decrease in volume. The initial dissolution of C3 S paste (0 ~ 6 weeks) was greatly attributed to the release of Ca(OH)2 , and the later dissolution (>6 weeks) was attributed to the decalcification of C-S-H gel. Although the mass of C3 S paste could decrease by more than 19 wt % after 6 weeks of implantation, the created pores (<1 µm) were not large enough for the bone tissue to migrate into C3 S paste. The loss of Ca ions also resulted in the transformation of SiO4 tetrahedrons from Q1 and Q2 to Q0 , Q3 , and Q4 in C-S-H gel. Because only isolated SiO4 tetrahedrons (Q0 ) and Ca ions could be absorbed by the bone tissue, C3 S paste gradually transformed into a silica-rich gel. The fundamental reason for no decrease in volume of C3 S paste was that the SiO4 tetrahedron network still maintained the frame structure of C3 S paste during the implantation.