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Here, a series of 1D COFs based nano\u2010structures (i.e. yolk\u2013shell spheres (YS\u2010COF), hollow spheres (HS\u2010COF) and solid spheres (SS\u2010COF)) is prepared via a solvent\u2010induced strategy that can be applied as binder modulators for Li\u2010S batteries. Specifically, they can impart enhanced mechanical properties, more adaptability to volume change, and better ability in adsorbing\/catalyzing lithium polysulfide intermediates (LiPSs) to traditional PVDF binder. Remarkably, the thus\u2010assembled YS\u2010COF\u2010based cell displays an initial specific capacity of up to 1011 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 0.5 C, which is much higher than that of HS\u2010COF, SS\u2010COF, and PVDF\u2010based Li\u2010S batteries. Even at 4 C, it still maintains a discharge specific capacity of 962 mAh g\n                    <jats:sup>\u22121<\/jats:sup>\n                    and can cycle for &gt;600 cycles. DFT calculations and finite element simulation reveal the important roles of nanomorphology and functional groups of YS\u2010COF in promoting electrochemical redox kinetics to boost battery performances. This strategy might provide in\u2010depth insights in the morphology engineering and performance optimization of 1D COFs for Li\u2010S batteries.\n                  <\/jats:p>","DOI":"10.1002\/adma.202505206","type":"journal-article","created":{"date-parts":[[2025,5,16]],"date-time":"2025-05-16T05:41:59Z","timestamp":1747374119000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":23,"title":["Steering Yolk\u2013Shell Nanostructures of 1D Unit\u2010Based Covalent Organic Frameworks as Binder Modulators"],"prefix":"10.1002","volume":"37","author":[{"given":"Yiwen","family":"Yang","sequence":"first","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization School of Chemistry South China Normal University  Guangzhou 510006 P. R. 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