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Herein, a CuCl annealing strategy is developed to leverage Cu interstitial intercalation for the precise modulation of electronic band structures and phonon dispersions in SnSe2. By synergizing with the Cu-induced formation of SnSe heterojunctions, this approach effectively decouples electron and phonon transport. Consequently, the SnSe2-2 mol% CuCl sample achieves a maximum power factor (PF) of 0.74 mW m\u20131 K\u20132 and surpasses pristine SnSe2 by 8-fold. Furthermore, the \u03baL is reduced to 0.53 W m\u20131 K\u20131 at 723 K, marking a 31% decrease relative to pristine SnSe2. This translates to a dimensionless figure of merit (zT) of 0.88 at 723 K parallel to the spark plasma sintering direction. Notably, we fabricate the first SnSe2-based single-leg thermoelectric generator (TEG), which delivers an energy conversion efficiency of about 2% under a \u0394T of 340.8 K. By effectively decoupling electronic and thermal transport, this work unlocks the full potential of eco-friendly SnSe2, providing a sustainable and high-performance paradigm for green energy harvesting without relying on toxic elements.<\/jats:p>","DOI":"10.1021\/acsami.6c14760","type":"journal-article","created":{"date-parts":[[2026,10,3]],"date-time":"2026-10-03T09:01:49Z","timestamp":1791018109000},"page":"55632-55644","source":"Crossref","is-referenced-by-count":0,"title":["Interstitial Cu-Induced Band Structure and Phonon Transport Regulation for Eco-friendly n-Type SnSe2 Thermoelectric Power Generation"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-3633-2288","authenticated-orcid":true,"given":"Wenxin","family":"Lai","sequence":"first","affiliation":[{"name":"Nanjing University of Science and Technology , , ,","place":["Nanjing, China, 210094"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pengfei","family":"Xu","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Molly Meng-Jung","family":"Li","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University , , ,","place":["Hong Kong, China, 999077"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Biao","family":"Xu","sequence":"additional","affiliation":[{"name":"Nanjing University of Posts & Telecommunications , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,3]]},"reference":[{"issue":"27","key":"2026101409073054700_cit1","doi-asserted-by":"publisher","first-page":"12642","DOI":"10.1007\/s10853-020-04949-0","article-title":"Review of current high-ZT thermoelectric materials","volume":"55","author":"Wei","year":"2020","journal-title":"J. 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