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Herein, a new type of ENRR catalyst is designed consisting of carbon\u2010bifunctionalized Mo\n                    <jats:sub>2<\/jats:sub>\n                    N nanoparticles (NPs) embedded in a hierarchical porous carbon matrix with atomic Pb sites (PbNC) through a one\u2010step carbonitridation strategy. The carbon\u2010bifunctionalization effect not only creates nitrogen vacancies through interstitial carbon doping to form molybdenum carbonitride (Mo\n                    <jats:sub>2<\/jats:sub>\n                    CN) phase that enhances N\n                    <jats:sub>2<\/jats:sub>\n                    adsorption and activation, but also stabilizes active sites via nanoconfinement of the in situ formed carbon layer on Mo\n                    <jats:sub>2<\/jats:sub>\n                    CN NPs. Concurrently,\u00a0the atomically dispersed Pb\u00a0within the PbNC matrix suppresses HER due to its weak H\n                    <jats:sup>*<\/jats:sup>\n                    affinity. The optimized catalyst demonstrates 38.7 \u00b5g h\n                    <jats:sup>\u22121<\/jats:sup>\n                    mg\n                    <jats:sup>\u22121<\/jats:sup>\n                    NH\n                    <jats:sub>3<\/jats:sub>\n                    yield at a low potential of \u22120.1 V with 50 h operational stability. Density functional theory calculations reveal that carbon\u2010induced nitrogen vacancies modulate the Mo d\u2010band center, which facilitates electron back\u2010donation to N\n                    <jats:sub>2<\/jats:sub>\n                    and thus shifts the potential\u2010determining step from initial protonation to the NH\n                    <jats:sub>3<\/jats:sub>\n                    desorption step\u00a0via\u00a0the Mars\u2010van Krevelen mechanism with a lower energy barrier for ENRR. This study proposes an integrated approach involving vacancy engineering, atomic\u2010level HER suppression, and nanoconfinement toward efficient ENRR catalysis.\n                  <\/jats:p>","DOI":"10.1002\/smll.202511794","type":"journal-article","created":{"date-parts":[[2026,1,12]],"date-time":"2026-01-12T15:15:11Z","timestamp":1768230911000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Carbon\u2010Bifunctionalized Mo\n                    <sub>2<\/sub>\n                    N Coupled Atomic Pb Sites for Efficient Nitrogen Reduction"],"prefix":"10.1002","volume":"22","author":[{"given":"Qingqing","family":"Ye","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical Technology  Beijing 100029 P. R. 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