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However, kinetic disparities between the competing reduction pathways of CO2 and NO3\u2013 lead to spatiotemporal mismatches between C- and N-intermediates, severely hindering efficient C\u2013N coupling. In this context, we demonstrated a strategic design of enzyme-inspired \u201cspatial decoupling\u2013temporal coupling\u201d on a ferroelectric SnS-Cu0.15-TiO2 heterojunction. A high urea yield rate of 2392.5 \u03bcg h\u20131 mgcat\u20131 with a Faradaic efficiency (FE) of 71.2% outperforms the state-of-the-art electrocatalysts. Atomically dispersed Cu1 sites induce an unprecedented ferroelectricity enhancement, whereby a strengthened built-in electric field generates spatially resolved charge domains for coactivation of both CO2 and NO3\u2013. Correlated in situ Raman and infrared spectroscopic studies disclose that the S-Cu1-O interfacial channels mediate remote *CO spillover and its dynamic, temporal coupling with *NH2. Moreover, a coupled electrolyzer integrating the electrocatalytic upcycling of wastewater-derived NO3\u2013 and Cl\u2013 achieves a remarkable 79.4% urea FE, while enabling simultaneous environmental remediation. This work highlights the unique advantages of ferroelectric heterojunctions-mediated dynamic catalysis in regulating complex reaction networks for urea electrosynthesis, opening sustainable electrochemical routes toward CO2 mitigation and the green transformation of coastal wastewater treatment.<\/jats:p>","DOI":"10.1021\/acs.est.6c04106","type":"journal-article","created":{"date-parts":[[2026,7,18]],"date-time":"2026-07-18T13:05:27Z","timestamp":1784379927000},"page":"20925-20938","source":"Crossref","is-referenced-by-count":0,"title":["Ferroelectric Heterojunction\nwith Spatiotemporally\nProgrammable CO Spillover Pathways Boosts Urea Electrosynthesis"],"prefix":"10.1021","volume":"60","author":[{"given":"Liying","family":"Zhang","sequence":"first","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenzhe","family":"Shang","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yao","family":"Li","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7318-2963","authenticated-orcid":true,"given":"Yantao","family":"Shi","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6665-220X","authenticated-orcid":true,"given":"Wei","family":"Liu","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7543-7766","authenticated-orcid":true,"given":"Sen","family":"Qiao","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,18]]},"reference":[{"issue":"43","key":"2026080409310006900_cit1","doi-asserted-by":"publisher","first-page":"23456","DOI":"10.1021\/acs.est.5c07104","article-title":"Fluvial Dissolved Organic Matter\nQuality Modulates Microbial Nitrate Transformation: Enhanced Denitrification\nunder Low Carbon-to-Nitrate Ratio","volume":"59","author":"Zhu","year":"2025","journal-title":"Environ.\nSci. 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