Silicon(Si)has been regarded as an alternative anode material to traditional graphite owing to its higher theoretical capacity(4200 vs.372 m Ah g;).However,Si anodes suffer from the inherent volume expansion and unsta...Silicon(Si)has been regarded as an alternative anode material to traditional graphite owing to its higher theoretical capacity(4200 vs.372 m Ah g;).However,Si anodes suffer from the inherent volume expansion and unstable solid electrolyte interphase,thus experiencing fast capacity decay,which hinders their commercial application.To address this,herein,an endotenon sheathinspired water-soluble double-network binder(DNB)is presented for resolving the bottleneck of Si anodes.The as-developed binder shows excellent adhesion,high mechanical properties,and a considerable self-healing capability mainly benefited by its supramolecular hybrid network.Apart from these advantages,this binder also induces a Li;N/Li F-rich solid electrolyte interface layer,contributing to a superior cycle stability of Si electrodes.As expected,the DNB can achieve mechanically more stable Si electrodes than traditional polyacrylic acid and pectin binders.As a result,DNB delivers superior electrochemical performance ofSi/Li half cells and Li Ni;Co;Mn;O;/Si full cells,even with a high loading of Si electrode,to traditional polyacrylic acid and pectin binders.The bioinspired binder design provides a promising route to achieve long-life Si anode-assembled lithium batteries.展开更多
The electrochemical performance of a battery is considered to be primarily dependent on the electrode material. However, engineering and optimization of electrodes also play a crucial role, and the same electrode mate...The electrochemical performance of a battery is considered to be primarily dependent on the electrode material. However, engineering and optimization of electrodes also play a crucial role, and the same electrode material can be designed to offer significantly improved batteries. In this work, Si–Fe–Mn nanomaterial alloy(Si/alloy) and graphite composite electrodes were densified at different calendering conditions of 3, 5, and 8 tons, and its influence on electrode porosity, electrolyte wettability, and long-term cycling was investigated. The active material loading was maintained very high(~2 mg cm^(-2)) to implement electrode engineering close to commercial loading scales. The densification was optimized to balance between the electrode thickness and wettability to enable the best electrochemical properties of the Si/alloy anodes.In this case, engineering and optimizing the Si/alloy composite electrodes to 3 ton calendering(electrode densification from 0.39 to 0.48 g cm^(-3)) showed enhanced cycling stability with a high capacity retention of ~100% over 100 cycles.展开更多
The 100 crystal-oriented silicon micropillar array platforms were prepared by microfabrication processes for the purpose of electrolyte additive identification. The silicon micropillar array platform was used for the ...The 100 crystal-oriented silicon micropillar array platforms were prepared by microfabrication processes for the purpose of electrolyte additive identification. The silicon micropillar array platform was used for the study of fluorinated vinyl carbonate(FEC), vinyl ethylene carbonate(VEC), ethylene sulfite(ES), and vinyl carbonate(VC) electrolyte additives in the LiPF_6 dissolved in a mixture of ethylene carbonate and diethyl carbonate electrolyte system using charge/discharge cycles, electrochemical impedance spectroscopy, cyclic voltammetry, scanning electron microscopy, and x-ray photoelectron spectroscopy. The results show that the silicon pillar morphology displays cross-shaped expansion after lithiation/delithiation, the inorganic lithium salt keeps the silicon pillar morphology intact, and the organic lithium salt content promotes a rougher silicon pillar surface. The presence of poly-(VC) components on the surface of FEC and VC electrodes allows the silicon pillar to accommodate greater volume expansion while remaining intact. This work provides a standard, fast, and effective test method for the performance analysis of electrolyte additives and provides guidance for the development of new electrolyte additives.展开更多
We previously reported the direct electrochemical detection of insulin at bare carbon electrodes. Here a novel modified acetylene carbon black paste electrode(SiC/CB-CPE), based on the outstanding characteristics of s...We previously reported the direct electrochemical detection of insulin at bare carbon electrodes. Here a novel modified acetylene carbon black paste electrode(SiC/CB-CPE), based on the outstanding characteristics of silicon carbide nanostructure,was developed for the electrooxidation of insulin in alkaline solution and it was characterized by cyclic voltammetry(CV) and electrochemical impedance spectroscopy(EIS) in 5 mmol/L Fe(CN)63-/4- solution. It is found that silicon carbide nanostructure doped into the CB-CPE greatly facilitates the redox electrochemistry of Fe(CN)63-/4- probe and the electrochemical oxidation of insulin. The electrooxidation of insulin is a one-electron and one-proton reaction and an irreversible adsorption-controlled electrode process. The anodic oxidation current increases linearly with the concentration of insulin from 1×10-7mol/L to1.2×10-6mol/L in 0.1 mol/L Na2CO3-NaHCO3 buffer solution(pH 10.0) and the detection limit was 50 nmol/L. In addition, the SiC/CB-CPE shows good sensitivity, reproducibility, renewability and capacity of resisting disturbance.展开更多
Sulphur(S)-template method based on conventional slurry-casting method has been developed to pro-duce porous silicon(Si)electrodes.The facile fabrication technology is suitable for current production line and expected...Sulphur(S)-template method based on conventional slurry-casting method has been developed to pro-duce porous silicon(Si)electrodes.The facile fabrication technology is suitable for current production line and expected to be widely applied to various electrode materials under large volume change during operation.Specifically,S particles as template agent are mixed with active material Si,carbon conductor and binder forming uniform slurry.After casting and drying,the electrodes are immersed in carbon disul-fide solution to remove S particles rapidly,generating pores in-situ at the original position of S particles.Electrochemical analysis shows that the pores inside electrodes are able to shorten lithium ion diffusion paths,reduce normal expansion rate and decrease formation of cracks in the Si electrode(2 mg_(Si)/cm^(2)),demonstrating a reversible capacity of 951 mAh/g at 0.5 A/g after 100 cycles(with a capacity retention of 99.5%)and a capacity of-826 mAh/g at 2 A/g.展开更多
Lithium-ion batteries suffer from mechano–electrochemical coupling problems that directly determine the battery life. In this paper, we investigate the electrode electrochemical performance under stress conditions, w...Lithium-ion batteries suffer from mechano–electrochemical coupling problems that directly determine the battery life. In this paper, we investigate the electrode electrochemical performance under stress conditions, where seven tensile/compressive stresses are designed and loaded on electrodes, thereby decoupling mechanics and electrochemistry through incremental stress loads. Four types of multi-group electrochemical tests under tensile/compressive stress loading and normal package loading are performed to quantitatively characterize the effects of tensile stress and compressive stress on cycle performance and the kinetic performance of a silicon composite electrode. Experiments show that a tensile stress improves the electrochemical performance of a silicon composite electrode, exhibiting increased specific capacity and capacity retention rate, reduced energy dissipation rate and impedances, enhanced reactivity, accelerated ion/electron migration and diffusion, and reduced polarization. Contrarily, a compressive stress has the opposite effect, inhibiting the electrochemical performance. The stress effect is nonlinear, and a more obvious suppression via compressive stress is observed than an enhancement via tensile stress. For example, a tensile stress of 675 k Pa increases diffusion coefficient by 32.5%, while a compressive stress reduces it by 35%. Based on the experimental results, the stress regulation mechanism is analyzed. Tensile stress loads increase the pores of the electrode material microstructure, providing more deformation spaces and ion/electron transport channels. This relieves contact compressive stress, strengthens diffusion/reaction, and reduces the degree of damage and energy dissipation. Thus, the essence of stress enhancement is that it improves and optimizes diffusion, reaction and stress in the microstructure of electrode material as well as their interactions via physical morphology.展开更多
Since hydrogen-terminated Si surface has hydrophobicity, it is expected that adsorbed monomolecular film of surfactant will be formed on the Si surface in aqueous solution containing the surfactant. Such an adsorbed m...Since hydrogen-terminated Si surface has hydrophobicity, it is expected that adsorbed monomolecular film of surfactant will be formed on the Si surface in aqueous solution containing the surfactant. Such an adsorbed monolayer film is very effective for the development of a functional electrode. In this study, we have investigated the state of adsorption about an aerosol OT as the monolayer on the electrode surface and its orientation with hydrogen-terminated Si(111) surface by in situ ATR-FTIR spectroscopy. At this time, in situ observation performed while imposing bias to the electrode. The results suggested that the aerosol OT were desorbed by the oxidation of back-bonds in the Si atoms on the electrode surface under the imposing noble potential, although no change was observed especially when imposing less-noble potential.展开更多
Peroxodiphosphate anion (a powerful oxidant) can be formed in a special water-based cleaning agent through an electrochemical reaction on boron-doped diamond electrodes. This electrochemical reaction was applied dur...Peroxodiphosphate anion (a powerful oxidant) can be formed in a special water-based cleaning agent through an electrochemical reaction on boron-doped diamond electrodes. This electrochemical reaction was applied during the oxidation,decomposition, and removal of organic contaminations on a silicon wafer surface, and it was used as the first step in the diamond electrochemical cleaning technique (DECT). The cleaning effects of DECT were compared with the RCA cleaning technique, including the silicon surface chemical composition that was observed with X-ray photoelectron spectroscopy and the morphology observed with atomic force microscopy. The measurement results show that the silicon surface cleaned by DECT has slightly less organic residue and lower micro-roughness,so the new technique is more effective than the RCA cleaning technique.展开更多
Lithium-ion batteries with composite anodes of graphite and silicon are increasingly being used. However, their degradation pathways are complicated due to the blended nature of the electrodes, with graphite and silic...Lithium-ion batteries with composite anodes of graphite and silicon are increasingly being used. However, their degradation pathways are complicated due to the blended nature of the electrodes, with graphite and silicon degrading at different rates. Here, we develop a deep learning health diagnostic framework to rapidly quantify and separate the different degradation rates of graphite and silicon in composite anodes using partial charging data. The convolutional neural network (CNN), trained with synthetic data, uses experimental partial charging data to diagnose electrode-level health of tested batteries, with errors of less than 3.1% (corresponding to the loss of active material reaching ∼75%). Sensitivity analysis of the capacity-voltage curve under different degradation modes is performed to provide a physically informed voltage window for diagnostics with partial charging data. By using the gradient-weighted class activation mapping approach, we provide explainable insights into how these CNNs work;highlighting regions of the voltage-curve to which they are most sensitive. Robustness is validated by introducing noise to the data, with no significant negative impact on the diagnostic accuracy for noise levels below 10 mV, thus highlighting the potential for deep learning approaches in the diagnostics of lithium-ion battery performance under real-world conditions. The framework presented here can be generalised to other cell formats and chemistries, providing robust and explainable battery diagnostics for both conventional single material electrodes, but also the more challenging composite electrodes.展开更多
Crystalline silicon(c-Si)heterojunction(HJT)solar cells are one of the promising technologies for next-generation industrial high-efficiency silicon solar cells,and many efforts in transferring this technology to high...Crystalline silicon(c-Si)heterojunction(HJT)solar cells are one of the promising technologies for next-generation industrial high-efficiency silicon solar cells,and many efforts in transferring this technology to high-volume manufacturing in the photovoltaic(PV)industry are currently ongoing.Metallization is of vital importance to the PV performance and long-term reliability of HJT solar cells.In this review,we summarize the development status of metallization approaches for highefficiency HJT solar cells.For conventional screen printing technology,to avoid the degradation of the passivation properties of the amorphous silicon layer,a low-temperature-cured(<250℃)paste and process are needed.This process,in turn,leads to high line/contact resistances and high paste costs.To improve the conductivity of electrodes and reduce the metallization cost,multi-busbar,fine-line printing,and low-temperature-cured silver-coated copper pastes have been developed.In addition,several potential metallization technologies for HJT solar cells,such as the Smart Wire Contacting Technology,pattern transfer printing,inkjet/FlexTrailprinting,and copper electroplating,are discussed in detail.B ased on the summary,the potential and challenges of these metallization technologies for HJT solar cells are analyzed.展开更多
基金This work was financially supported by the Science Foundation for the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010600)the National Natural Science Foundation of China(21933006)+4 种基金the Key Scientific and Technological Innovation Project of Shandong(2020CXGC010401)the Key research and development plan of Shandong Province(2019GHZ009)Fundamental Research Funds for the Central Universities(20CX02205A)and financial support from the Taishan Scholar Project(ts201511063)Open access funding provided by Shanghai Jiao Tong University
文摘Silicon(Si)has been regarded as an alternative anode material to traditional graphite owing to its higher theoretical capacity(4200 vs.372 m Ah g;).However,Si anodes suffer from the inherent volume expansion and unstable solid electrolyte interphase,thus experiencing fast capacity decay,which hinders their commercial application.To address this,herein,an endotenon sheathinspired water-soluble double-network binder(DNB)is presented for resolving the bottleneck of Si anodes.The as-developed binder shows excellent adhesion,high mechanical properties,and a considerable self-healing capability mainly benefited by its supramolecular hybrid network.Apart from these advantages,this binder also induces a Li;N/Li F-rich solid electrolyte interface layer,contributing to a superior cycle stability of Si electrodes.As expected,the DNB can achieve mechanically more stable Si electrodes than traditional polyacrylic acid and pectin binders.As a result,DNB delivers superior electrochemical performance ofSi/Li half cells and Li Ni;Co;Mn;O;/Si full cells,even with a high loading of Si electrode,to traditional polyacrylic acid and pectin binders.The bioinspired binder design provides a promising route to achieve long-life Si anode-assembled lithium batteries.
基金financial support from Joint School of Nanoscience and Nanoengineering,USA
文摘The electrochemical performance of a battery is considered to be primarily dependent on the electrode material. However, engineering and optimization of electrodes also play a crucial role, and the same electrode material can be designed to offer significantly improved batteries. In this work, Si–Fe–Mn nanomaterial alloy(Si/alloy) and graphite composite electrodes were densified at different calendering conditions of 3, 5, and 8 tons, and its influence on electrode porosity, electrolyte wettability, and long-term cycling was investigated. The active material loading was maintained very high(~2 mg cm^(-2)) to implement electrode engineering close to commercial loading scales. The densification was optimized to balance between the electrode thickness and wettability to enable the best electrochemical properties of the Si/alloy anodes.In this case, engineering and optimizing the Si/alloy composite electrodes to 3 ton calendering(electrode densification from 0.39 to 0.48 g cm^(-3)) showed enhanced cycling stability with a high capacity retention of ~100% over 100 cycles.
基金supported by the National Key R&D Program of China (Grant Nos. 2016YFB0100500 and 2016YFB0100100)the National Natural Science Foundation of China (Grant Nos. 11674387, 11574385, 22005332, 115674368, and 62065005)。
文摘The 100 crystal-oriented silicon micropillar array platforms were prepared by microfabrication processes for the purpose of electrolyte additive identification. The silicon micropillar array platform was used for the study of fluorinated vinyl carbonate(FEC), vinyl ethylene carbonate(VEC), ethylene sulfite(ES), and vinyl carbonate(VC) electrolyte additives in the LiPF_6 dissolved in a mixture of ethylene carbonate and diethyl carbonate electrolyte system using charge/discharge cycles, electrochemical impedance spectroscopy, cyclic voltammetry, scanning electron microscopy, and x-ray photoelectron spectroscopy. The results show that the silicon pillar morphology displays cross-shaped expansion after lithiation/delithiation, the inorganic lithium salt keeps the silicon pillar morphology intact, and the organic lithium salt content promotes a rougher silicon pillar surface. The presence of poly-(VC) components on the surface of FEC and VC electrodes allows the silicon pillar to accommodate greater volume expansion while remaining intact. This work provides a standard, fast, and effective test method for the performance analysis of electrolyte additives and provides guidance for the development of new electrolyte additives.
基金Funded by the Innovative Talent Training Project of Chongqing University(CDJXS11220004)the Fundamental Research Funds for the Central Universities of Chongqing University+1 种基金the Natural Science Foundation Project of CQ CSTC(No.2011BB5134)the National Natural Science Foundation of China(No.NSFC81101417)
文摘We previously reported the direct electrochemical detection of insulin at bare carbon electrodes. Here a novel modified acetylene carbon black paste electrode(SiC/CB-CPE), based on the outstanding characteristics of silicon carbide nanostructure,was developed for the electrooxidation of insulin in alkaline solution and it was characterized by cyclic voltammetry(CV) and electrochemical impedance spectroscopy(EIS) in 5 mmol/L Fe(CN)63-/4- solution. It is found that silicon carbide nanostructure doped into the CB-CPE greatly facilitates the redox electrochemistry of Fe(CN)63-/4- probe and the electrochemical oxidation of insulin. The electrooxidation of insulin is a one-electron and one-proton reaction and an irreversible adsorption-controlled electrode process. The anodic oxidation current increases linearly with the concentration of insulin from 1×10-7mol/L to1.2×10-6mol/L in 0.1 mol/L Na2CO3-NaHCO3 buffer solution(pH 10.0) and the detection limit was 50 nmol/L. In addition, the SiC/CB-CPE shows good sensitivity, reproducibility, renewability and capacity of resisting disturbance.
基金the National Natural Science Foundation of China(Nos.51904344,52172264)the Natural Science Foundation of Hunan Province of China(Nos.2021JJ10060,2022GK2033).
文摘Sulphur(S)-template method based on conventional slurry-casting method has been developed to pro-duce porous silicon(Si)electrodes.The facile fabrication technology is suitable for current production line and expected to be widely applied to various electrode materials under large volume change during operation.Specifically,S particles as template agent are mixed with active material Si,carbon conductor and binder forming uniform slurry.After casting and drying,the electrodes are immersed in carbon disul-fide solution to remove S particles rapidly,generating pores in-situ at the original position of S particles.Electrochemical analysis shows that the pores inside electrodes are able to shorten lithium ion diffusion paths,reduce normal expansion rate and decrease formation of cracks in the Si electrode(2 mg_(Si)/cm^(2)),demonstrating a reversible capacity of 951 mAh/g at 0.5 A/g after 100 cycles(with a capacity retention of 99.5%)and a capacity of-826 mAh/g at 2 A/g.
基金Project supported by the Major Program of the National Natural Science Foundation of China(Grant No.11890680)the National Natural Science Foundation of China(Grant No.12022205)。
文摘Lithium-ion batteries suffer from mechano–electrochemical coupling problems that directly determine the battery life. In this paper, we investigate the electrode electrochemical performance under stress conditions, where seven tensile/compressive stresses are designed and loaded on electrodes, thereby decoupling mechanics and electrochemistry through incremental stress loads. Four types of multi-group electrochemical tests under tensile/compressive stress loading and normal package loading are performed to quantitatively characterize the effects of tensile stress and compressive stress on cycle performance and the kinetic performance of a silicon composite electrode. Experiments show that a tensile stress improves the electrochemical performance of a silicon composite electrode, exhibiting increased specific capacity and capacity retention rate, reduced energy dissipation rate and impedances, enhanced reactivity, accelerated ion/electron migration and diffusion, and reduced polarization. Contrarily, a compressive stress has the opposite effect, inhibiting the electrochemical performance. The stress effect is nonlinear, and a more obvious suppression via compressive stress is observed than an enhancement via tensile stress. For example, a tensile stress of 675 k Pa increases diffusion coefficient by 32.5%, while a compressive stress reduces it by 35%. Based on the experimental results, the stress regulation mechanism is analyzed. Tensile stress loads increase the pores of the electrode material microstructure, providing more deformation spaces and ion/electron transport channels. This relieves contact compressive stress, strengthens diffusion/reaction, and reduces the degree of damage and energy dissipation. Thus, the essence of stress enhancement is that it improves and optimizes diffusion, reaction and stress in the microstructure of electrode material as well as their interactions via physical morphology.
文摘Since hydrogen-terminated Si surface has hydrophobicity, it is expected that adsorbed monomolecular film of surfactant will be formed on the Si surface in aqueous solution containing the surfactant. Such an adsorbed monolayer film is very effective for the development of a functional electrode. In this study, we have investigated the state of adsorption about an aerosol OT as the monolayer on the electrode surface and its orientation with hydrogen-terminated Si(111) surface by in situ ATR-FTIR spectroscopy. At this time, in situ observation performed while imposing bias to the electrode. The results suggested that the aerosol OT were desorbed by the oxidation of back-bonds in the Si atoms on the electrode surface under the imposing noble potential, although no change was observed especially when imposing less-noble potential.
文摘Peroxodiphosphate anion (a powerful oxidant) can be formed in a special water-based cleaning agent through an electrochemical reaction on boron-doped diamond electrodes. This electrochemical reaction was applied during the oxidation,decomposition, and removal of organic contaminations on a silicon wafer surface, and it was used as the first step in the diamond electrochemical cleaning technique (DECT). The cleaning effects of DECT were compared with the RCA cleaning technique, including the silicon surface chemical composition that was observed with X-ray photoelectron spectroscopy and the morphology observed with atomic force microscopy. The measurement results show that the silicon surface cleaned by DECT has slightly less organic residue and lower micro-roughness,so the new technique is more effective than the RCA cleaning technique.
基金supported by the EPSRC Impact Acceleration Award(EP/X52556X/1)the Faraday Institution's Industrial Fellowship(FIIF-013)+2 种基金the EPSRC Faraday Institution's Multi-Scale Modelling Project(EP/S003053/1,grant number FIRG003)the EPSRC Joint UK-India Clean Energy Center(JUICE)(EP/P003605/1)the EPSRC Integrated Development of Low-Carbon Energy Systems(IDLES)project(EP/R045518/1).
文摘Lithium-ion batteries with composite anodes of graphite and silicon are increasingly being used. However, their degradation pathways are complicated due to the blended nature of the electrodes, with graphite and silicon degrading at different rates. Here, we develop a deep learning health diagnostic framework to rapidly quantify and separate the different degradation rates of graphite and silicon in composite anodes using partial charging data. The convolutional neural network (CNN), trained with synthetic data, uses experimental partial charging data to diagnose electrode-level health of tested batteries, with errors of less than 3.1% (corresponding to the loss of active material reaching ∼75%). Sensitivity analysis of the capacity-voltage curve under different degradation modes is performed to provide a physically informed voltage window for diagnostics with partial charging data. By using the gradient-weighted class activation mapping approach, we provide explainable insights into how these CNNs work;highlighting regions of the voltage-curve to which they are most sensitive. Robustness is validated by introducing noise to the data, with no significant negative impact on the diagnostic accuracy for noise levels below 10 mV, thus highlighting the potential for deep learning approaches in the diagnostics of lithium-ion battery performance under real-world conditions. The framework presented here can be generalised to other cell formats and chemistries, providing robust and explainable battery diagnostics for both conventional single material electrodes, but also the more challenging composite electrodes.
基金supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘Crystalline silicon(c-Si)heterojunction(HJT)solar cells are one of the promising technologies for next-generation industrial high-efficiency silicon solar cells,and many efforts in transferring this technology to high-volume manufacturing in the photovoltaic(PV)industry are currently ongoing.Metallization is of vital importance to the PV performance and long-term reliability of HJT solar cells.In this review,we summarize the development status of metallization approaches for highefficiency HJT solar cells.For conventional screen printing technology,to avoid the degradation of the passivation properties of the amorphous silicon layer,a low-temperature-cured(<250℃)paste and process are needed.This process,in turn,leads to high line/contact resistances and high paste costs.To improve the conductivity of electrodes and reduce the metallization cost,multi-busbar,fine-line printing,and low-temperature-cured silver-coated copper pastes have been developed.In addition,several potential metallization technologies for HJT solar cells,such as the Smart Wire Contacting Technology,pattern transfer printing,inkjet/FlexTrailprinting,and copper electroplating,are discussed in detail.B ased on the summary,the potential and challenges of these metallization technologies for HJT solar cells are analyzed.