To address the issues of large volume change and low conductivity of silicon(Si)materials,carbon coatings have been widely employed as surface protection agent and conductive medium to encapsulate the Si materials,whi...To address the issues of large volume change and low conductivity of silicon(Si)materials,carbon coatings have been widely employed as surface protection agent and conductive medium to encapsulate the Si materials,which can improve the electrochemical performance of Si-based electrodes.There has been a strong demand to gain a deeper understanding of the impact of efficient carbon coating over the lithiation and delithiation process of Si materials.Here,we report the first observation of the extended two-phase transformation of carbon-coated Si nanoparticles(Si/C)during electrochemical processes.The Si/C nanoparticles were prepared by sintering Si nanoparticles with polyvinylidene chloride precursor.The Si/C electrode underwent a two-phase transition during the first 20 cycles at 0.2 C,but started to engage in solid solution reaction when the ordered compact carbon coating began to crack.Under higher current density conditions,the electrode was also found to be involved in solid solution reaction,which,however,was due to the overwhelming demand of kinetic property rather than the breaking of the carbon coating.In comparison,the Si/C composites prepared with sucrose possessed more disordered and porous carbon structures,and presented solid solution reaction throughout the entire cycling process.展开更多
Humic substances(HS),which are defined as a series of highly acidic,relatively high-molecular-weight,and yellow to black colored substances formed during the decay and transformation of plant and microbial remains,ubi...Humic substances(HS),which are defined as a series of highly acidic,relatively high-molecular-weight,and yellow to black colored substances formed during the decay and transformation of plant and microbial remains,ubiquitously occur in nature.Humic substances represent the largest stable organic carbon pool in terrestrial environments and are the central characteristic of the soil.However,the validity of the HS concept and the justification of their extraction procedure have been recently debated.Here,we argue that the traditional humic paradigm is still relevant.Humic substances are distinctive and complex because the extracted HS formed during the humification are chemically distinct from their precursors and are heterogeneous among soils.By reviewing the concept,formation pathways,and stabilization of HS,we propose that the key question facing soil scientists is whether HS are soil microbial residues or unique synthesized compounds.Without revealing the distinctiveness of HS,it is impossible to address this question,as the structure,composition,and reactivity of HS are still poorly known owing to the heterogeneity and geographical variability of HS and the limits of the currently available analytical techniques.In our view,the distinctiveness of HS is fundamental to the soil,and thus further studies should be focused on revealing the distinctiveness of HS and explaining why HS hold this distinctiveness.展开更多
基金This study is funded by the Assistant Secretary for Energy Efficiency,Vehicle Technologies Office of the U.S.Department of Energy,under the Si Consortium Program.Electron microscopy experiments are conducted at the National Centre for Electron Microscopy and the Molecular Foundry located at Lawrence Berkeley National Laboratory is supported by the Director,Office of Science,Office of Basic Energy Sciences,the U.S.Department of Energy under Contract No.DE-AC02-05CH11231.
文摘To address the issues of large volume change and low conductivity of silicon(Si)materials,carbon coatings have been widely employed as surface protection agent and conductive medium to encapsulate the Si materials,which can improve the electrochemical performance of Si-based electrodes.There has been a strong demand to gain a deeper understanding of the impact of efficient carbon coating over the lithiation and delithiation process of Si materials.Here,we report the first observation of the extended two-phase transformation of carbon-coated Si nanoparticles(Si/C)during electrochemical processes.The Si/C nanoparticles were prepared by sintering Si nanoparticles with polyvinylidene chloride precursor.The Si/C electrode underwent a two-phase transition during the first 20 cycles at 0.2 C,but started to engage in solid solution reaction when the ordered compact carbon coating began to crack.Under higher current density conditions,the electrode was also found to be involved in solid solution reaction,which,however,was due to the overwhelming demand of kinetic property rather than the breaking of the carbon coating.In comparison,the Si/C composites prepared with sucrose possessed more disordered and porous carbon structures,and presented solid solution reaction throughout the entire cycling process.
基金supported by the National Natural Science Foundation of China(Nos.41571231 and 41201221)the National Key Research and Development Program of China(No.2016YFD0200304)+3 种基金the Scientific Instrument and Equipment Development Project of Chinese Academy Sciences(CAS)(No.YJKYYQ20170058)the Natural Science Foundation of Jiangsu Province,China(No.BK2012496)the Youth Innovation Promotion Association,CAS(No.2017362)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.19KJB180010)。
文摘Humic substances(HS),which are defined as a series of highly acidic,relatively high-molecular-weight,and yellow to black colored substances formed during the decay and transformation of plant and microbial remains,ubiquitously occur in nature.Humic substances represent the largest stable organic carbon pool in terrestrial environments and are the central characteristic of the soil.However,the validity of the HS concept and the justification of their extraction procedure have been recently debated.Here,we argue that the traditional humic paradigm is still relevant.Humic substances are distinctive and complex because the extracted HS formed during the humification are chemically distinct from their precursors and are heterogeneous among soils.By reviewing the concept,formation pathways,and stabilization of HS,we propose that the key question facing soil scientists is whether HS are soil microbial residues or unique synthesized compounds.Without revealing the distinctiveness of HS,it is impossible to address this question,as the structure,composition,and reactivity of HS are still poorly known owing to the heterogeneity and geographical variability of HS and the limits of the currently available analytical techniques.In our view,the distinctiveness of HS is fundamental to the soil,and thus further studies should be focused on revealing the distinctiveness of HS and explaining why HS hold this distinctiveness.