{"title":"Durable modulation of Zn(002) plane deposition via reproducible zincophilic carbon quantum dots towards low N/P ratio zinc-ion batteries†","authors":"Zhu Xu, Heng Li, Yupeng Liu, Kexuan Wang, Huibo Wang, Mingzheng Ge, Junpeng Xie, Jielei Li, Zhaorui Wen, Hui Pan, Songnan Qu, Jilei Liu, Yanyan Zhang, Yuxin Tang and Shi Chen","doi":"10.1039/D3MH00261F","DOIUrl":null,"url":null,"abstract":"<p >Aqueous zinc-ion batteries (ZIBs) are promising candidates for next-generation energy storage systems due to their intrinsic safety, environmental friendliness, and low cost. However, the uncontrollable Zn dendrite growth during cycling is still a critical challenge for the long-term operation of ZIBs, especially under harsh lean-Zn conditions. Herein, we report nitrogen and sulfur-codoped carbon quantum dots (N,S-CDs) as zincophilic electrolyte additives to regulate the Zn deposition behaviors. The N,S-CDs with abundant electronegative groups can attract Zn<small><sup>2+</sup></small> ions and co-deposit with Zn<small><sup>2+</sup></small> ions on the anode surface, inducing a parallel orientation of the (002) crystal plane. The deposition of Zn preferentially along the (002) crystal direction fundamentally avoids the formation of Zn dendrites. Moreover, the co-depositing/stripping feature of N,S-CDs under an electric field force ensures the reproducible and long-lasting modulation of the Zn anode stability. Benefiting from these two unique modulation mechanisms, stable cyclability of the thin Zn anodes (10 and 20 μm) at a high depth of discharge (DOD) of 67% and high Zn||Na<small><sub>2</sub></small>V<small><sub>6</sub></small>O<small><sub>16</sub></small>·3H<small><sub>2</sub></small>O (NVO, 11.52 mg cm<small><sup>−2</sup></small>) full-cell energy density (144.98 W h Kg<small><sup>−1</sup></small>) at a record-low negative/positive (N/P) capacity ratio of 1.05 are achieved using the N,S-CDs as an additive in ZnSO<small><sub>4</sub></small> electrolyte. Our findings not only offer a feasible solution for developing actual high-energy density ZIBs but also provide in-depth insights into the working mechanism of CDs in regulating Zn deposition behaviors.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":null,"pages":null},"PeriodicalIF":12.2000,"publicationDate":"2023-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"1","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Horizons","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2023/mh/d3mh00261f","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 1
Abstract
Aqueous zinc-ion batteries (ZIBs) are promising candidates for next-generation energy storage systems due to their intrinsic safety, environmental friendliness, and low cost. However, the uncontrollable Zn dendrite growth during cycling is still a critical challenge for the long-term operation of ZIBs, especially under harsh lean-Zn conditions. Herein, we report nitrogen and sulfur-codoped carbon quantum dots (N,S-CDs) as zincophilic electrolyte additives to regulate the Zn deposition behaviors. The N,S-CDs with abundant electronegative groups can attract Zn2+ ions and co-deposit with Zn2+ ions on the anode surface, inducing a parallel orientation of the (002) crystal plane. The deposition of Zn preferentially along the (002) crystal direction fundamentally avoids the formation of Zn dendrites. Moreover, the co-depositing/stripping feature of N,S-CDs under an electric field force ensures the reproducible and long-lasting modulation of the Zn anode stability. Benefiting from these two unique modulation mechanisms, stable cyclability of the thin Zn anodes (10 and 20 μm) at a high depth of discharge (DOD) of 67% and high Zn||Na2V6O16·3H2O (NVO, 11.52 mg cm−2) full-cell energy density (144.98 W h Kg−1) at a record-low negative/positive (N/P) capacity ratio of 1.05 are achieved using the N,S-CDs as an additive in ZnSO4 electrolyte. Our findings not only offer a feasible solution for developing actual high-energy density ZIBs but also provide in-depth insights into the working mechanism of CDs in regulating Zn deposition behaviors.