Multilevel carbon architecture of subnanoscopic silicon for fast‐charging high‐energy‐density lithium‐ion batteries

Silicon(Si)is widely used as a lithium‐ion‐battery anode owing to its high capacity and abundant crustal reserves.However,large volume change upon cycling and poor conductivity of Si cause rapid capacity decay and poor fast‐charging capability limiting its commercial applications.Here,we propose a multilevel carbon architecture with vertical graphene sheets(VGSs)grown on surfaces of subnanoscopically and homogeneously dispersed Si–C composite nanospheres,which are subsequently embedded into a carbon matrix(C/VGSs@Si–C).Subnanoscopic C in the Si–C nanospheres,VGSs,and carbon matrix form a three‐dimensional conductive and robust network,which significantly improves the conductivity and suppresses the volume expansion of Si,thereby boosting charge transport and improving electrode stability.The VGSs with vast exposed edges considerably increase the contact area with the carbon matrix and supply directional transport channels through the entire material,which boosts charge transport.The carbon matrix encapsulates VGSs@Si–C to decrease the specific surface area and increase tap density,thus yielding high first Coulombic efficiency and electrode compaction density.Consequently,C/VGSs@Si–C delivers excellent Li‐ion storage performances under industrial electrode conditions.In particular,the full cells show high energy densities of 603.5 Wh kg^(−1)and 1685.5 Wh L^(−1)at 0.1 C and maintain 80.7%of the energy density at 3 C.

A review of the carbon coating of the silicon anode in highperformance lithium-ion batteries

In the development of rechargeable lithium ion batteries(LIBs),silicon anodes have attracted much attention because of their extremely high theoretical capacity,relatively low Li-insertion voltage and the availability of silicon resources.However,their large volume expansion and fragile solid electrolyte interface(SEI)film hinder their commercial application.To solve these problems,Si has been combined with various carbon materials to increase their structural stability and improve their interface properties.The use of different carbon materials,such as amorphous carbon and graphite,as three-dimensional(3D)protective anode coatings that help buffer mechanical strain and isolate the electrolyte is detailed,and novel methods for applying the coatings are outlined.However,carbon materials used as a protective layer still have some disadvantages,necessitating their modification.Recent developments have focused on modifying the protective carbon shells,and substitutes for the carbon have been suggested.

Multi-scale design of silicon/carbon composite anode materials for lithium-ion batteries:A review

Silicon/carbon composites,which integrate the high lithium storage performance of silicon with the exceptional mechanical strength and conductivity of carbon,will replace the traditional graphite electrodes for high-energy lithium-ion batteries.Various strategies have been designed to synthesize silicon/carbon composites for tackling the issues of anode pulverization and poor stability in the anodes,thereby improving the lithium storage ability.The effect of the regulation method at each scale on the final negative electrode performance remains unclear.However,it has not been fully clarified how the regulation methods at each scale influence the final anode performance.This review will categorize the materials structure into three scales:molecular scale,nanoscale,and microscale.First,the review will examine modification methods at the molecular scale,focusing on the interfacial bonding force between silicon and carbon.Next,it will summarize various nanostructures and special shapes in the nanoscale to explore the construction of silicon/carbon composites.Lastly,the review will provide an analysis of microscale control approaches,focusing on the formation of composite particle with micron size and the utilization of micro-Si.This review provides a comprehensive overview of the multi-scale design of silicon/carbon composite anode materials and their optimization strategies to enhance the performance of lithium-ion batteries.

Preparation and electrochemical lithium storage performance of porous silicon microsphere composite with metal modification and carbon coating

This work adopts a multi⁃step etching⁃heat treatment strategy to prepare porous silicon microsphere com⁃posite with Sb⁃Sn surface modification and carbon coating(pSi/Sb⁃Sn@C),using industrial grade SiAl alloy micro⁃spheres as a precursor.pSi/Sb⁃Sn@C had a 3D structure with bimetallic(Sb⁃Sn)modified porous silicon micro⁃spheres(pSi/Sb⁃Sn)as the core and carbon coating as the shell.Carbon shells can improve the electronic conductivi⁃ty and mechanical stability of porous silicon microspheres,which is beneficial for obtaining a stable solid electrolyte interface(SEI)film.The 3D porous core promotes the diffusion of lithium ions,increases the intercalation/delithia⁃tion active sites,and buffers the volume expansion during the intercalation process.The introduction of active met⁃als(Sb⁃Sn)can improve the conductivity of the composite and contribute to a certain amount of lithium storage ca⁃pacity.Due to its unique composition and microstructure,pSi/Sb⁃Sn@C showed a reversible capacity of 1247.4 mAh·g^(-1) after 300 charge/discharge cycles at a current density of 1.0 A·g^(-1),demonstrating excellent rate lithium storage performance and enhanced electrochemical cycling stability.

Preparation and Analysis of Carbon Fiber-Silicon Carbide Thermally Conductive Asphalt Concrete

An experimental investigation into the thermal conductivity of CF-SiC two-phase composite asphalt concrete is presented.The main objective of this study was to verify the possibility of using SiC powder instead of mineral powder as the thermal conductive filler to prepare a new type of asphalt concrete and improve the efficiency of electrothermal snow and ice melting systems accordingly.The thermal conductivity of asphalt concrete prepared with different thermally conductive fillers was tested by a transient plane source method,and the related performances were measured.Then the temperature rise rate and surface temperature were studied through field heating tests.Finally,the actual ice melting efficiency of the thermally conductive asphalt concrete was evaluated using an effective electrothermal system.As shown by the experimental results,the composite made of SiC powder and carbon fiber has a high thermal conductivity.When SiC replaces mineral powder,the thermal conductivity of the asphalt mixture increases first and then decreases with the increase of carbon fiber content.In the present study,in particular,the thermal conductivity attained a peak when the carbon fiber content was 0.2%of the aggregate mass.

Sol-gel synthesis of nanometer silicon/silicon suboxide/carbon anode material

A stacked Si/SiO_(x)/C composite anode material with carbon-coated structure was prepared by sol-gel method combined with carbothermal reduction using organic silicon.The results of X-ray diffractometry, scanning electron microscopy, and elemental analysis show that the Si/SiO_(x)/C material is a secondary particle with a porous micronanostructure, and the presence of nanometer silicon does not affect the carbothermal reduction and carbon coating.Electrochemical test results indicate that the specific capacity and first coulombic efficiency of SiO_(x)/C composite with nanometer silicon can be increased to 1 946.05 mAh/g and 76.49%,respectively.The reversible specific capacity of Si/SiO_(x)/C material blended with graphite is 749.69 mAh/g after 100 cycles at a current density of 0.1 C,and the capacity retention rate is up to 89.03%.Therefore, the composite has excellent electrochemical cycle stability.

Porous silicon/carbon composites as anodes for high-performance lithium-ion batteries

Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.

Facilitating prelithiation of silicon carbon anode by localized high-concentration electrolyte for high-rate and long-cycle lithium storage

The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Herein,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the ICE.The thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical performance.The SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic products.Thus,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G anodes.LHCE also leads to uniform decomposition and high stability of the SEI with abundant organic components.As a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 C.NCM 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.

Research Progress of Carbon-Silicone Composite Materials

Silicone is a kind of polymer material with high cross-linked structure,which is com-posed by Si-O-Si main chain.Due to the special molecular chain structure,silicone mate-rials are characterized by oxidation resistance,aging resistance,high and low temperature resistance and chemical corrosion resistance.Moreover,silicone materials have process-able properties,simple forming process,good mechanical property,non-toxic and pollution-free.Therefore,silicone has been widely concerned by researchers at home and abroad.In this paper,the main research progress and application directions of carbon-silicone composite at home and abroad in recent years are reviewed.

Influence of Carbon Content on Element Diffusion in Silicon Carbide-Based TRISO Composite Fuel

The coating layers of Tri-structural Isotropic Particles(TRISO)serve to protect the kernel and act as barriers to fission products.Sintering aids in the silicon carbide matrix variably react with TRISO coating layers,leading to the destruction of the coating layers.Investigating how carbon content affects element diffusion in silicon carbide-based TRISO composite fuel is of great significance for predicting reactor safety.In this study,silicon carbide-based TRISO composite fuels with different carbon contents were prepared by adding varying amounts of phenolic resin to the silicon carbide matrix.X-ray Diffraction(XRD)and Scanning Electron Microscopy(SEM)were employed to characterize the phase composition,morphology,and microstructure of the composite fuels.The elemental content in each coating layer of TRISO was quantified using Energy-Dispersive X-ray Spectroscopy(EDS).The results demonstrated that the addition of phenolic resin promoted the uniform distribution of sintering aids in the silicon carbide matrix.The atomic percentage(at.%)of aluminum(Al)in the pyrolytic carbon layer of the TRISO particles reached its lowest value of 0.55%when the phenolic resin addition was 1%.This is because the addition of phenolic resin caused the Al and silicon(Si)in the matrix to preferentially react with the carbon in the phenolic resin to form a metastable liquid phase,rather than preferentially consuming the pyrolytic carbon in the outer coating layer of the TRISO particles.The findings suggest that carbon addition through phenolic resin incorporation can effectively mitigate the deleterious reactions between the TRISO coating layers and sintering aids,thereby enhancing the durability and safety of silicon carbide-based TRISO composite fuels.

Interfacial design of silicon/carbon anodes for rechargeable batteries:A review

Silicon(Si)has been studied as a promising alloying type anode for lithium-ion batteries due to its high specific capacity,low operating potential and abundant resources.Nevertheless,huge volume expansion during alloying/dealloying processes and low electronic conductivity of Si anodes restrict their electrochemical performance.Thus,carbon(C)materials with special physical and chemical properties are applied in Si anodes to effectively solve these problems.This review focuses on current status in the exploration of Si/C anodes,including the lithiation mechanism and solid electrolyte interface formation,various carbon sources in Si/C anodes,such as traditional carbon sources(graphite,pitch,biomass),and novel carbon sources(MXene,graphene,MOFs-derived carbon,graphdiyne,etc.),as well as interfacial bonding modes of Si and C in the Si/C anodes.Finally,we summarize and prospect the selection of carbonaceous materials,structural design and interface control of Si/C anodes,and application of Si/C anodes in all-solid-state lithium-ion batteries and sodium-ion batteries et al.This review will help researchers in the design of novel Si/C anodes for rechargeable batteries.

Influence of carbon sources on the performance of carbon-coated nano-silicon

Silicon-based material is an important anode material for next-generation lithium-ion batteries.In order to overcome its shortcomings,carbon coating is often employed to improve the electrochemical performance.However,the carbon source,carbon content,and different contact and mixing schemes between carbon sources and silicon are all complex factors and need to be clarified.In this study,nano-silicon is coated by the chemical vapor deposition method using different carbon sources,such as acetylene,methane,propane,and propylene.Carbon content after coating is designed to stay at the same level to reduce the experimental error.Results show the sample with higher conductivity provides higher cycle performance.Propylene is the best choice of the four carbon sources studied in this work.These results indicate that the selection of the carbon source is an important factor that plays a significant role in electrochemical performance.

In Situ Formation of LiF-Rich Carbon Interphase on Silicon Particles for Cycle-Stable Battery Anodes

Silicon(Si)is a potential high-capacity anode material for the next-generation lithium-ion battery with high energy density.However,Si anodes suff er from severe interfacial chemistry issues,such as side reactions at the electrode/electrolyte interface,leading to poor electrochemical cycling stability.Herein,we demonstrate the fabrication of a conformal fl uorine-containing carbon(FC)layer on Si particles(Si-FC)and its in situ electrochemical conversion into a LiF-rich carbon layer above 1.5 V(vs.Li^(+)/Li).The as-formed LiF-rich carbon layer not only isolates the active Si and electrolytes,leading to the suppression of side reactions,but also induces the formation of a robust solid-electrolyte interface(SEI),leading to the stable interfacial chemistry of as-designed Si-FC particles.The Si-FC electrode has a high initial Coulombic effi ciency(CE)of 84.8%and a high reversible capacity of 1450 mAh/g at 0.4 C(1000 mA/g)for 300 cycles.In addition,a hybrid electrode consisting of 85 wt%graphite and 15 wt%Si-FC,and mass 2.3 mg/cm^(2) loading delivers a high areal capacity of 2.0 mAh/cm^(2) and a high-capacity retention of 93.2%after 100 cycles,showing the prospects for practical use.

基于In Silicon模拟消化的北极虾DPP-Ⅳ抑制肽活性分析

北极虾具有很高的营养价值,在食品领域已引起越来越多的关注。对北极虾蛋白进行In Silicon模拟消化获得寡肽,通过PeptideRanker活性评分及理化性质分析,从中筛选出具有潜在生物活性的寡肽。使用ToxinPred分析和BIOPEP-UWM生物活性预测,发现部分寡肽具有二肽基肽酶-Ⅳ(dipeptidyl peptidase-Ⅳ,DPP-Ⅳ)抑制活性,最终确定WFP(一种三肽,Trp-Phe-Pro)具有最优的DPP-Ⅳ抑制活性肽。分子对接表明,WFP和DPP-Ⅳ能够形成稳定的复合物,其结合能为-6.93 kcal/mol,进一步研究表明,WFP通过与DPP-Ⅳ S1、S2、S3三个活性口袋中的9个氨基酸残基发生相互作用而抑制其活性。本研究为阐释北极虾营养价值及生物活性肽的开发提供了理论依据。

Innovative Solutions for High-Performance Silicon Anodes in Lithium-Ion Batteries:Overcoming Challenges and Real-World Applications

Silicon(Si)has emerged as a potent anode material for lithium-ion batteries(LIBs),but faces challenges like low electrical conductivity and significant volume changes during lithiation/delithiation,leading to material pulverization and capacity degradation.Recent research on nanostructured Si aims to mitigate volume expansion and enhance electrochemical performance,yet still grapples with issues like pulverization,unstable solid electrolyte interface(SEI)growth,and interparticle resistance.This review delves into innovative strategies for optimizing Si anodes’electrochemical performance via structural engineering,focusing on the synthesis of Si/C composites,engineering multidimensional nanostructures,and applying non-carbonaceous coatings.Forming a stable SEI is vital to prevent electrolyte decomposition and enhance Li^(+)transport,thereby stabilizing the Si anode interface and boosting cycling Coulombic efficiency.We also examine groundbreaking advancements such as self-healing polymers and advanced prelithiation methods to improve initial Coulombic efficiency and combat capacity loss.Our review uniquely provides a detailed examination of these strategies in real-world applications,moving beyond theoretical discussions.It offers a critical analysis of these approaches in terms of performance enhancement,scalability,and commercial feasibility.In conclusion,this review presents a comprehensive view and a forward-looking perspective on designing robust,high-performance Si-based anodes the next generation of LIBs.

Enhancing the Interaction of Carbon Nanotubes by Metal-Organic Decomposition with Improved Mechanical Strength and Ultra-Broadband EMI Shielding Performance

The remarkable properties of carbon nanotubes(CNTs)have led to promising applications in the field of electromagnetic inter-ference(EMI)shielding.However,for macroscopic CNT assemblies,such as CNT film,achieving high electrical and mechanical properties remains challenging,which heavily depends on the tube-tube interac-tions of CNTs.Herein,we develop a novel strategy based on metal-organic decomposition(MOD)to fabricate a flexible silver-carbon nanotube(Ag-CNT)film.The Ag particles are introduced in situ into the CNT film through annealing of MOD,leading to enhanced tube-tube interactions.As a result,the electrical conductivity of Ag-CNT film is up to 6.82×10^(5) S m^(-1),and the EMI shielding effectiveness of Ag-CNT film with a thickness of~7.8μm exceeds 66 dB in the ultra-broad frequency range(3-40 GHz).The tensile strength and Young’s modulus of Ag-CNT film increase from 30.09±3.14 to 76.06±6.20 MPa(~253%)and from 1.12±0.33 to 8.90±0.97 GPa(~795%),respectively.Moreover,the Ag-CNT film exhibits excellent near-field shield-ing performance,which can effectively block wireless transmission.This innovative approach provides an effective route to further apply macroscopic CNT assemblies to future portable and wearable electronic devices.

Carbon Emission Effects Driven by Evolution of Chinese Dietary Structure from 1987 to 2020

Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important task.This study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary structure.The results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption pattern.The dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality one.During the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing trend.The per capita food carbon emissions of residents in urban and rural showed an overall upward trend.The total food carbon emissions in urban increased significantly,while that in rural increased first and then decreased.The influence of beef and mutton on carbon emissions is the highest in dietary structure.Compared with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.

Aboveground carbon sequestration of Cunninghamia lanceolata forests:Magnitude and drivers

Understanding the spatial variation,temporal changes,and their underlying driving forces of carbon sequestration in various forests is of great importance for understanding the carbon cycle and carbon management options.How carbon density and sequestration in various Cunninghamia lanceolata forests,extensively cultivated for timber production in subtropical China,vary with biodiversity,forest structure,environment,and cultural factors remain poorly explored,presenting a critical knowledge gap for realizing carbon sequestration supply potential through management.Based on a large-scale database of 449 permanent forest inventory plots,we quantified the spatial-temporal heterogeneity of aboveground carbon densities and carbon accumulation rates in Cunninghamia lanceolate forests in Hunan Province,China,and attributed the contributions of stand structure,environmental,and management factors to the heterogeneity using quantile age-sequence analysis,partial least squares path modeling(PLS-PM),and hot-spot analysis.The results showed lower values of carbon density and sequestration on average,in comparison with other forests in the same climate zone(i.e.,subtropics),with pronounced spatial and temporal variability.Specifically,quantile regression analysis using carbon accumulation rates along an age sequence showed large differences in carbon sequestration rates among underperformed and outperformed forests(0.50 and 1.80 Mg·ha^(-1)·yr^(-1)).PLS-PM demonstrated that maximum DBH and stand density were the main crucial drivers of aboveground carbon density from young to mature forests.Furthermore,species diversity and geotopographic factors were the significant factors causing the large discrepancy in aboveground carbon density change between low-and high-carbon-bearing forests.Hotspot analysis revealed the importance of culture attributes in shaping the geospatial patterns of carbon sequestration.Our work highlighted that retaining largesized DBH trees and increasing shade-tolerant tree species were important to enhance carbon sequestration in C.lanceolate forests.

Carbon nanocages bridged with graphene enable fast kinetics for dual-carbon lithium-ion capacitors

Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.

Construction and Application of a Regional Kilometer-Scale Carbon Source and Sink Assimilation Inversion System(CCMVS-R)

CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.