{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,5]],"date-time":"2026-10-05T22:27:05Z","timestamp":1791239225664,"version":"4.1.0"},"reference-count":35,"publisher":"MDPI AG","issue":"9","license":[{"start":{"date-parts":[[2022,4,19]],"date-time":"2022-04-19T00:00:00Z","timestamp":1650326400000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Nanomaterials"],"abstract":"<jats:p>Silicon-based anodes are promising to replace graphite-based anodes for high-capacity lithium-ion batteries (LIB). However, the charge\u2013discharge cycling suffers from internal stresses created by large volume changes of silicon, which form silicon-lithium compounds, and excessive consumption of lithium by irreversible formation of lithium-containing compounds. Consumption of lithium by the initial conditioning of the anode, as indicated by low initial coulombic efficiency (ICE), and subsequently continuous formation of solid-electrolyte-phase (SEI) on the freshly exposed silicon surface, are among the main issues. A high-performance, silicon-based, high-capacity anode exhibiting 88.8% ICE and the retention of 2 mAh\/cm2 areal capacity after 200 discharge\u2013charge cycles at the rate of 1 A\/g is reported. The anode is made on a copper foil using a mixture of 70%:10%:20% by weight ratio of silicon flakes of 100 \u00d7 800 \u00d7 800 nm in size, Super P conductivity enhancement additive, and an equal-weight mixture of CMC and SBR binders. Pyrolysis of fabricated anodes at 700 \u00b0C in argon environment for 1 h was applied to convert the binders into a porous graphitic carbon structure that encapsulates individual silicon flakes. The porous anode has a mechanically strong and electrically conductive graphitic carbon structure formed by the pyrolyzed binders, which protect individual silicon flakes from excessive reactions with the electrolyte and help keep small pieces of broken silicon flakes together within the carbon structure. The selection and amount of conductivity enhancement additives are shown to be critical to the achievement of both high-ICE and high-capacity retention after long cycling. The Super P conductivity enhancement additive exhibits a smaller effective surface area where SEI forms compared to KB, and thus leads to the best combination of both high-ICE and high-capacity retention. A silicon-based anode exhibiting high capacity, high ICE, and a long cycling life has been achieved by the facile and promising one-step fabrication process.<\/jats:p>","DOI":"10.3390\/nano12091387","type":"journal-article","created":{"date-parts":[[2022,4,19]],"date-time":"2022-04-19T02:39:31Z","timestamp":1650335971000},"page":"1387","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":22,"title":["High-ICE and High-Capacity Retention Silicon-Based Anode for Lithium-Ion Battery"],"prefix":"10.3390","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4763-1144","authenticated-orcid":false,"given":"Yonhua","family":"Tzeng","sequence":"first","affiliation":[{"name":"Institute of Microelectronics, Department of Electrical Engineering, National Cheng Kung University, Tainan City 70101, Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng-Ying","family":"Jhan","sequence":"additional","affiliation":[{"name":"Institute of Microelectronics, Department of Electrical Engineering, National Cheng Kung University, Tainan City 70101, Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi-Chen","family":"Wu","sequence":"additional","affiliation":[{"name":"Institute of Microelectronics, Department of Electrical Engineering, National Cheng Kung University, Tainan City 70101, Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guan-Yu","family":"Chen","sequence":"additional","affiliation":[{"name":"Institute of Microelectronics, Department of Electrical Engineering, National Cheng Kung University, Tainan City 70101, Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kuo-Ming","family":"Chiu","sequence":"additional","affiliation":[{"name":"Institute of Microelectronics, Department of Electrical Engineering, National Cheng Kung University, Tainan City 70101, Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-7528-7968","authenticated-orcid":false,"given":"Stephen Yang-En","family":"Guu","sequence":"additional","affiliation":[{"name":"Institute of Microelectronics, Department of Electrical Engineering, National Cheng Kung University, Tainan City 70101, Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2022,4,19]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"1003","DOI":"10.1016\/j.jpowsour.2006.09.084","article-title":"Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cells","volume":"163","author":"Kasavajjula","year":"2007","journal-title":"J. Power Sources"},{"key":"ref_2","first-page":"2137","article-title":"25th anniversary article: Understanding the lithiation of silicon and other alloying anodes for lithium-ion batteries","volume":"26","author":"McDowell","year":"2013","journal-title":"Adv. Mater."},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"125380","DOI":"10.1016\/j.cej.2020.125380","article-title":"Recent progress of structural designs of silicon for performance-enhanced lithium-ion batteries","volume":"397","author":"Qi","year":"2020","journal-title":"Chem. Eng. J."},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"722","DOI":"10.1002\/aenm.201200024","article-title":"In Situ TEM experiments of electrochemical lithiation and delithiation of individual nanostructures","volume":"2","author":"Liu","year":"2012","journal-title":"Adv. Energy Mater."},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"414","DOI":"10.1016\/j.nantod.2012.08.004","article-title":"Designing nanostructured Si anodes for high energy lithium ion batteries","volume":"7","author":"Wu","year":"2012","journal-title":"Nano Today"},{"key":"ref_6","doi-asserted-by":"crossref","unstructured":"Tzeng, Y., Jhan, C.-Y., and Wu, Y.-H. (2022). Effects of Pyrolysis on High-Capacity Si-Based Anode of Lithium Ion Battery with High Coulombic Efficiency and Long Cycling Life. Nanomaterials, 12.","DOI":"10.3390\/nano12030469"},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"946","DOI":"10.1038\/s41598-018-36797-z","article-title":"Influence of Conductive additives on the stability of red phosphorus-carbon anodes for sodium-ion batteries","volume":"9","author":"Wang","year":"2019","journal-title":"Sci. Rep."},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"11NM01","DOI":"10.7567\/JJAP.52.11NM01","article-title":"Microstructural Effect of Carbon Blacks for the Application in Lithium Ion Batteries","volume":"52","author":"Yun","year":"2013","journal-title":"Jpn. J. Appl. Phys."},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"924","DOI":"10.1016\/S0378-7753(03)00230-1","article-title":"Charge\u2013discharge properties of a cathode prepared with ketjen black as the electro-conductive additive in lithium ion batteries","volume":"119\u2013121","author":"Kuroda","year":"2003","journal-title":"J. Power Sources"},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"A2509","DOI":"10.1149\/2.0131514jes","article-title":"Review-Nano-Silicon\/Carbon Composite Anode Materials Towards Practical Application for Next Generation Li-Ion Batteries","volume":"162","author":"Luo","year":"2015","journal-title":"J. Electrochem. Soc."},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"74","DOI":"10.1039\/C5NR05116A","article-title":"Silicon as a potential anode material for Li-ion batteries: Where size, geometry and structure matter","volume":"8","author":"Maziar","year":"2016","journal-title":"Nanoscale"},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"133","DOI":"10.1016\/j.nanoen.2015.09.016","article-title":"Yolk-shell silicon-mesoporous carbon anode with compact solid electrolyte interphase film for superior lithium-ion batteries","volume":"18","author":"Yang","year":"2015","journal-title":"Nano Energy"},{"key":"ref_13","doi-asserted-by":"crossref","first-page":"5124","DOI":"10.1021\/acs.nanolett.9b01492","article-title":"Silicon carbide as a protective layer to stabilize Si-based anodes by inhibiting chemical reactions","volume":"19","author":"Yu","year":"2019","journal-title":"Nano Lett."},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"8634","DOI":"10.1038\/s41598-018-26769-8","article-title":"Substoichiometric silicon nitride\u2013an anode material for Li-ion batteries promising high stability and high capacity","volume":"8","author":"Ulvestad","year":"2018","journal-title":"Sci. Rep."},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"285","DOI":"10.1039\/C8CS00441B","article-title":"Silicon oxides: A promising family of anode materials for lithium-ion batteries","volume":"48","author":"Liu","year":"2019","journal-title":"Chem. Soc. Rev."},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"16411","DOI":"10.1021\/acsami.0c00676","article-title":"Covalently bonded silicon\/carbon nanocomposites as cycle-stable anodes for Li-ion batteries","volume":"12","author":"Fan","year":"2020","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"2591","DOI":"10.1021\/acs.chemmater.5b00339","article-title":"Improved Performance of the Silicon Anode for Li-Ion Batteries: Understanding the Surface Modification Mechanism of Fluoroethylene Carbonate as an Effective Electrolyte Additive","volume":"27","author":"Xu","year":"2015","journal-title":"Chem. Mater."},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"285","DOI":"10.1016\/j.jpowsour.2016.09.062","article-title":"Electrochemical Impedance Spectroscopy study in micro-grain structured amorphous silicon anodes for lithium-ion batteries","volume":"331","author":"Paloukis","year":"2016","journal-title":"J. Power Sources"},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"1086","DOI":"10.1016\/j.ceramint.2020.08.224","article-title":"Lithium ion batteries with enhanced electrochemical performance by using carbon-coated SiOx\/Ag composites as anode material","volume":"47","author":"Ouyang","year":"2021","journal-title":"Ceram. Int."},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"3981","DOI":"10.1016\/j.electacta.2011.02.014","article-title":"Cyclability study of silicon\u2013carbon composite anodes for lithium-ion batteries using electrochemical impedance spectroscopy","volume":"56","author":"Guo","year":"2011","journal-title":"Electrochim. Acta"},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"14066","DOI":"10.1021\/acsami.8b22221","article-title":"Identification of the Solid Electrolyte Interface on the Si\/C Composite Anode with FEC as the Additive","volume":"11","author":"Li","year":"2019","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"295","DOI":"10.1002\/aenm.201200857","article-title":"Microsized Si-C Composite with Interconnected Nanoscale Building Blocks as High-Performance Anodes for Practical Application in Lithium-Ion Batteries","volume":"3","author":"Yi","year":"2013","journal-title":"Adv. Energy Mater."},{"key":"ref_23","doi-asserted-by":"crossref","first-page":"1571","DOI":"10.1002\/adma.201203981","article-title":"Mussel-inspired adhesive binders for high-performance silicon nanoparticle anodes inlithium-ion batteries","volume":"25","author":"Ryou","year":"2013","journal-title":"Adv. Mater."},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"4679","DOI":"10.1002\/adma.201102421","article-title":"Polymers with tailored electronic structure for high capacity lithium battery electrodes","volume":"23","author":"Liu","year":"2011","journal-title":"Adv. Mater."},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"8234","DOI":"10.1039\/c3ta10883j","article-title":"A high capacity silicon\u2212graphite composite as anode for lithium-ion batteries using low content amorphous silicon and compatible binders","volume":"1","author":"Yim","year":"2013","journal-title":"J. Mater. Chem. A"},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"19","DOI":"10.1016\/j.jallcom.2019.03.310","article-title":"Facile synthesizing silicon waste\/carbon composites via rapid thermal process for lithium-ion battery anode","volume":"791","author":"Chen","year":"2019","journal-title":"J. Alloys Compd."},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"105654","DOI":"10.1016\/j.nanoen.2020.105654","article-title":"A mechanically robust self-healing binder for silicon anode in lithium ion batteries","volume":"81","author":"Chen","year":"2021","journal-title":"Nano Energy"},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"137580","DOI":"10.1016\/j.electacta.2020.137580","article-title":"Epoxy and amide crosslinked polarity enhanced polysaccharides binder for silicon anode in lithium-ion batteries","volume":"368","author":"Wang","year":"2021","journal-title":"Electrochim. Acta"},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"229530","DOI":"10.1016\/j.jpowsour.2021.229530","article-title":"A carboxymethyl vegetable gum as a robust water soluble binder for silicon anodes in lithium-ion batteries","volume":"489","author":"Wang","year":"2021","journal-title":"J. Power Sources"},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"129468","DOI":"10.1016\/j.cej.2021.129468","article-title":"Silicon nanoparticles encapsulated in multifunctional crosslinked nano-silica\/carbon hybrid matrix as a high-performance anode for Li-ion batteries","volume":"418","author":"Dai","year":"2020","journal-title":"Chem. Eng. J."},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"228021","DOI":"10.1016\/j.jpowsour.2020.228021","article-title":"Controlled swelling behavior and stable cycling of silicon\/graphite granular composite for high energy density in lithium ion batteries","volume":"457","author":"Lee","year":"2020","journal-title":"J. Power Sources"},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"1474","DOI":"10.1038\/s41467-020-15217-9","article-title":"Hierarchical porous silicon structures with extraordinary mechanical strength as high-performance lithium-ion battery anodes","volume":"11","author":"Jia","year":"2020","journal-title":"Nat. Commun."},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"103824","DOI":"10.1016\/j.nanoen.2019.06.020","article-title":"A facile and versatile strategy towards high-performance Si anodes for Li-ion capacitors: Concomitant conductive network construction and dual-interfacial engineering","volume":"63","author":"Shao","year":"2019","journal-title":"Nano Energy"},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"134975","DOI":"10.1016\/j.electacta.2019.134975","article-title":"Bilayer-graphene-coated Si nanoparticles as advanced anodes for high-rate lithium-ion batteries","volume":"329","author":"Ding","year":"2020","journal-title":"Electrochim. Acta"},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"104444","DOI":"10.1016\/j.nanoen.2019.104444","article-title":"In situ synthesis of MOF-derived carbon shells for silicon anode with improved lithium-ion storage","volume":"70","author":"Gao","year":"2020","journal-title":"Nano Energy"}],"container-title":["Nanomaterials"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2079-4991\/12\/9\/1387\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,10,10]],"date-time":"2025-10-10T22:56:21Z","timestamp":1760136981000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2079-4991\/12\/9\/1387"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2022,4,19]]},"references-count":35,"journal-issue":{"issue":"9","published-online":{"date-parts":[[2022,5]]}},"alternative-id":["nano12091387"],"URL":"https:\/\/doi.org\/10.3390\/nano12091387","relation":{},"ISSN":["2079-4991"],"issn-type":[{"value":"2079-4991","type":"electronic"}],"subject":[],"published":{"date-parts":[[2022,4,19]]}}}