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Alloying Ru transforms metastable hexagonal close-packed (hcp) Ni into NO3RR-active face-centered cubic (fcc) Ni1\u2013xRux (x = 0\u20130.3) alloys by modulating the nucleation and growth kinetics of Ni. Concurrently, the high density of twin boundaries and edge dislocations in hcp Ni approaches a defect-saturation limit, driving a structural transition that stabilizes a semicrystalline Ru-alloyed fcc phase with a phase fraction of 96%. Operando Raman and attenuated total reflection Fourier transform infrared (ATR-FTIR) spectral analyses along with theoretical calculations show potential-dependent NH3 formation through stepwise *NO3 to *NO reduction at charge-modulated Ni\u03b4+-Ru\u03b4- sites, and subsequent *N hydrogenation to *NH3 on Ru\u03b4- sites, assisted by interfacial H2O-derived *H. Preadsorbed *H on fcc Ni74Ru26 surface facilitates *NO3 adsorption and lowers the rate-determining energy barrier. Ni74Ru26 delivers nearly 100% NH3 Faradaic efficiency from 0 to \u22120.4 VRHE, with a maximum of 99.6 \u00b1 0.3% at \u22120.1 VRHE. NH3 yield reaches 30077 \u00b1 4316 \u03bcg h\u20131 cm\u20132 (48201 \u03bcg h\u20131 mgRu\u20131) at \u22120.9 VRHE and energy efficiency of 37% at +0.1 VRHE. Ni74Ru26 retains \u223c100% NH3 Faradaic efficiency over 10 cycles and 50 h at \u22120.1 VRHE, and \u2212100 mA cm\u20132, respectively. When Ni74Ru26 is used as the cathode in a galvanic Zn-NO3\u2013 battery, it achieves a power density of 5.6 mW cm\u20132.<\/jats:p>","DOI":"10.1021\/acsnano.6c06447","type":"journal-article","created":{"date-parts":[[2026,8,13]],"date-time":"2026-08-13T03:02:30Z","timestamp":1786590150000},"page":"23314-23329","source":"Crossref","is-referenced-by-count":2,"title":["Ruthenium-Induced\nStrain- and Phase-Polarized Multifaceted\nNickel for Nitrate-to-Ammonia Electrocatalysis"],"prefix":"10.1021","volume":"20","author":[{"given":"Mamoni","family":"Maji","sequence":"first","affiliation":[{"name":"Indian Institute of Science Education and Research (IISER) Kolkata , , ,","place":["Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0009-1205-6777","authenticated-orcid":true,"given":"Ritika","family":"Saroha","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Roorkee , , , ,","place":["Roorkee, Uttarakhand, India, 247667"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-8152-9397","authenticated-orcid":true,"given":"Immanuel","family":"Jabez","sequence":"additional","affiliation":[{"name":"Jawaharlal Nehru Centre for Advanced Scientific Research , , ,","place":["Bangalore, India, 560064"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kamal","family":"Manna","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research (IISER) Kolkata , , ,","place":["Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ahitagni","family":"Roy","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research (IISER) Kolkata , , ,","place":["Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Saswati","family":"Sasmal","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research (IISER) Kolkata , , ,","place":["Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sebastian C.","family":"Peter","sequence":"additional","affiliation":[{"name":"Jawaharlal Nehru Centre for Advanced Scientific Research , , ,","place":["Bangalore, India, 560064"]},{"name":"Jawaharlal Nehru Centre for Advanced Scientific Research , , ,","place":["Bangalore, India, 560064"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8202-4628","authenticated-orcid":true,"given":"Swastika","family":"Banerjee","sequence":"additional","affiliation":[{"name":"Indian Institute of Technology Roorkee , , , ,","place":["Roorkee, Uttarakhand, India, 247667"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8074-965X","authenticated-orcid":true,"given":"Sayan","family":"Bhattacharyya","sequence":"additional","affiliation":[{"name":"Indian Institute of Science Education and Research (IISER) Kolkata , , ,","place":["Mohanpur, India, 741246"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,12]]},"reference":[{"key":"2026083119010167800_cit1","doi-asserted-by":"publisher","first-page":"290","DOI":"10.1016\/j.joule.2020.12.025","article-title":"Electrocatalytic\nNitrate Reduction for Sustainable Ammonia Production","volume":"5","author":"van Langevelde","year":"2021","journal-title":"Joule"},{"key":"2026083119010167800_cit2","doi-asserted-by":"publisher","first-page":"377","DOI":"10.1038\/s41929-019-0280-0","article-title":"Electrochemical\nSynthesis of Ammonia as a Potential Alternative to the Haber\u2013Bosch\nProcess","volume":"2","author":"Soloveichik","year":"2019","journal-title":"Nat. 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