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Herein, we study the impact of benzene\u2010derivative ligands with elaborately modulated binding strength and acidity on wide\u2010bandgap perovskites for high\u2010performance perovskite\/silicon TSCs. Specifically, the acidity\/alkalinity and binding strength are preliminarily tuned using different functional groups of \u2010PO\u2083H\u2082, \u2010COOH, and \u2010NH\u2082, and further finely adjusted by altering the chain lengths between the benzene ring and the functional groups. The results show that strong binding is indispensable for effectively suppressing voltage loss. However, the commonly used benzylphosphonic acid (BPPA) for firm surface binding exhibits too strong acidity that can etch the perovskite surface, resulting in halide\u2010vacancy defects and pronounced hysteresis. Increasing the side chain length of BPPA to (2\u2010phenylethyl)phosphonic acid not only enables a suitable acid dissociation constant (p\n                    <jats:italic>K<\/jats:italic>\n                    a) to avoid acid\u2010induced etching but also achieves robust anchoring to the perovskite surface with a parallel adsorption orientation, which reduces the charge transport barrier at the interface. These properties enable strong\u2010adsorption surface termination (SAST) of the perovskite surface while preventing acid\u2010induced etching. As a result, the SAST strategy achieves a remarkable efficiency of 32.13% (certified 31.72%) for hysteresis\u2010free perovskite\/silicon TSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.202500350","type":"journal-article","created":{"date-parts":[[2025,3,11]],"date-time":"2025-03-11T08:45:08Z","timestamp":1741682708000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":38,"title":["Modulating Binding Strength and Acidity of Benzene\u2010Derivative Ligands Enables Efficient and Hysteresis\u2010Free Perovskite\/Silicon Tandem Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"given":"Liu","family":"Yang","sequence":"first","affiliation":[{"name":"Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information Displays College of Materials Science and Engineering Huaqiao University  Xiamen 361021 China"},{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shibo","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ninggui","family":"Ma","sequence":"additional","affiliation":[{"name":"Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information Displays College of Materials Science and Engineering Huaqiao University  Xiamen 361021 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Shi","sequence":"additional","affiliation":[{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zheng","family":"Fang","sequence":"additional","affiliation":[{"name":"Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information Displays College of Materials Science and Engineering Huaqiao University  Xiamen 361021 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongbin","family":"Jin","sequence":"additional","affiliation":[{"name":"Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information Displays College of Materials Science and Engineering Huaqiao University  Xiamen 361021 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Enlong","family":"Hou","sequence":"additional","affiliation":[{"name":"Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information Displays College of Materials Science and Engineering Huaqiao University  Xiamen 361021 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Xu","sequence":"additional","affiliation":[{"name":"Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing Institute of Luminescent Materials and Information Displays College of Materials Science and Engineering Huaqiao University  Xiamen 361021 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fengxian","family":"Cao","sequence":"additional","affiliation":[{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenhao","family":"Li","sequence":"additional","affiliation":[{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kun","family":"Gao","sequence":"additional","affiliation":[{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yao","family":"Li","sequence":"additional","affiliation":[{"name":"College of Energy Soochow Institute for Energy and Materials InnovationS (SIEMIS) Soochow University  Suzhou 215006 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dinxin","family":"Cao","sequence":"additional","affiliation":[{"name":"Suzhou Maxwell Technologies Co. 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