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The liquid\u2013solid Li\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>4<\/jats:sub>\n                    \u2010to\u2010Li\n                    <jats:sub>2<\/jats:sub>\n                    S conversion governs the reaction rate, underscoring the importance of electrocatalysts in accelerating polysulfide conversion. Here, we report a defective ZIF\u201067 catalyst, designed through controlled ligand removal, to simultaneously regulate the electronic structure and induce confinement\u2010driven active site densification. The partial removal of ligands exposed unsaturated Co sites, forming \u201cenzyme\u2010like catalytic pockets\u201d to immobilize polysulfides. The remaining ligands surrounding the metal centers tuned the local electronic environment, optimizing intermediate stabilization and catalytic activity. This synergistic regulation enhanced polysulfide adsorption, reduced steric hindrance, and accelerated the critical Li\n                    <jats:sub>2<\/jats:sub>\n                    S deposition\/dissolution processes. Consequently, the sulfur cathode incorporating defective ZIF\u201067 exhibited improved cycling stability, delivering a capacity fade rate of 0.11 % per cycle over 200 cycles at 5 C, and maintaining a fade rate of 0.075 % per cycle over 150 cycles at 1 C with a sulfur loading of 4\u00a0mg cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . Our findings highlight the pivotal role of defect engineering in tailoring both site density and electronic structure within MOFs, offering a rational strategy for boosting polysulfide catalysis and advancing the practical application of lithium\u2013sulfur batteries.\n                  <\/jats:p>","DOI":"10.1002\/smtd.202502136","type":"journal-article","created":{"date-parts":[[2026,1,21]],"date-time":"2026-01-21T06:26:56Z","timestamp":1768976816000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Regulating Electronic Structure and Confinement\u2010Induced Site Densification in Defective MOF for Boosted Polysulfide Catalysis in Lithium\u2013Sulfur Batteries"],"prefix":"10.1002","volume":"10","author":[{"given":"Liyuan","family":"Qian","sequence":"first","affiliation":[{"name":"Shenzhen Key Laboratory of Solid State Batteries &amp; Guangdong Provincial Key Laboratory of Energy Materials For Electric Power &amp; Guangdong\u2010Hong Kong\u2010Macao Joint Laboratory For Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices &amp; Institute of Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiqian","family":"Lin","sequence":"additional","affiliation":[{"name":"Shenzhen Key Laboratory of Solid State Batteries &amp; Guangdong Provincial Key Laboratory of Energy Materials For Electric Power &amp; Guangdong\u2010Hong Kong\u2010Macao Joint Laboratory For Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices &amp; Institute of Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen 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Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"You","sequence":"additional","affiliation":[{"name":"Shenzhen Key Laboratory of Solid State Batteries &amp; Guangdong Provincial Key Laboratory of Energy Materials For Electric Power &amp; Guangdong\u2010Hong Kong\u2010Macao Joint Laboratory For Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices &amp; Institute of Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0088-9447","authenticated-orcid":false,"given":"Haibin","family":"Lin","sequence":"additional","affiliation":[{"name":"Shenzhen Key Laboratory of Solid State Batteries &amp; Guangdong Provincial Key Laboratory of Energy Materials For Electric Power &amp; Guangdong\u2010Hong Kong\u2010Macao Joint Laboratory For Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices &amp; Institute of Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruo","family":"Zhao","sequence":"additional","affiliation":[{"name":"Institute For Advanced Study Shenzhen University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaofei","family":"Wang","sequence":"additional","affiliation":[{"name":"Shenzhen Key Laboratory of Solid State Batteries &amp; Guangdong Provincial Key Laboratory of Energy Materials For Electric Power &amp; Guangdong\u2010Hong Kong\u2010Macao Joint Laboratory For Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices &amp; Institute of Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinlong","family":"Zhu","sequence":"additional","affiliation":[{"name":"Shenzhen Key Laboratory of Solid State Batteries &amp; Guangdong Provincial Key Laboratory of Energy Materials For Electric Power &amp; Guangdong\u2010Hong Kong\u2010Macao Joint Laboratory For Photonic\u2010Thermal\u2010Electrical Energy Materials and Devices &amp; Institute of Major Scientific Facilities for New Materials &amp; Academy for Advanced Interdisciplinary Studies Southern University of Science and Technology  Shenzhen China"},{"name":"Department of Physics &amp; State Key Laboratory of Quantum Functional Materials &amp; Guangdong Basic Research Center of Excellence for Quantum Science Southern University of Science and Technology  Shenzhen 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