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The central challenge is developing an efficient photoelectrocatalyst that simultaneously reduces overpotential and maximizes NH\n                    <jats:sub>3<\/jats:sub>\n                    selectivity. Herein, an amorphous\/crystalline heterojunction Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    \/Cu\n                    <jats:sub>2<\/jats:sub>\n                    O bonded by Cu\u2010O\n                    <jats:sub>v<\/jats:sub>\n                    \u2010Ni, is constructed via photoelectrocatalytic interface regulation for synergistic photoelectrocatalysis (SPEC) NH\n                    <jats:sub>3<\/jats:sub>\n                    synthesis. Results demonstrate \u223c100% light absorption efficiency and \u223c90% high charge separation efficiency, enabling almost completely rapid 98.80% NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    conversion with stable NH\n                    <jats:sub>3<\/jats:sub>\n                    FE (&gt; 99%) and high selectivity (&gt; 97%). A superior NH\n                    <jats:sub>3<\/jats:sub>\n                    yield of 1316.1\u00a0\u00b5mol h\n                    <jats:sup>\u22121<\/jats:sup>\n                    cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    is attained, alongside an excellent positive onset potential of 0.322\u00a0V versus RHE. In situ experiments further reveal that crystalline Cu\n                    <jats:sub>2<\/jats:sub>\n                    O activates carriers to accelerate the rate\u2010determining step (N\n                    <jats:sup>+5<\/jats:sup>\n                    \u2192 N\n                    <jats:sup>+3<\/jats:sup>\n                    ), while amorphous Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    significantly enhances electron extraction and *H accumulation for protonation (N\n                    <jats:sup>+3<\/jats:sup>\n                    \u2192 N\n                    <jats:sup>\u22123<\/jats:sup>\n                    ). Increasing potential shifts the system from electro\u2010assisted photocatalysis (activating Cu\u2010O\u00b7\u00b7\u00b7*NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    sites) to photo\u2010assisted electrocatalysis (Cu\n                    <jats:sub>2<\/jats:sub>\n                    O \u2192 Ni(OH)\n                    <jats:sub>2<\/jats:sub>\n                    electron transfer), then to SPEC (efficient *H coupling) process. Further application to actual fertilizer plant wastewater achieves \u223c90% NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    removal efficiency and &gt; 85% NH\n                    <jats:sub>3<\/jats:sub>\n                    selectivity, demonstrating promising scalability for efficient photoelectrocatalysis NO\n                    <jats:sub>3<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    \u2010to\u2010NH\n                    <jats:sub>3<\/jats:sub>\n                    with great environmental remediation potential.\n                  <\/jats:p>","DOI":"10.1002\/anie.3509008","type":"journal-article","created":{"date-parts":[[2026,4,6]],"date-time":"2026-04-06T05:07:18Z","timestamp":1775452038000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Amorphous\/Crystalline Heterojunction Ni(OH)\n                    <sub>2<\/sub>\n                    \/Cu\n                    <sub>2<\/sub>\n                    O(111) for Photoelectrocatalysis NO\n                    <sub>3<\/sub>\n                    <sup>\u2212<\/sup>\n                    \u2010to\u2010NH\n                    <sub>3<\/sub>\n                    : Positive Onset Potential, High Selectivity, and Complete Conversion"],"prefix":"10.1002","volume":"65","author":[{"given":"Lan","family":"Wang","sequence":"first","affiliation":[{"name":"School of Chemical Science and Engineering Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration Ministry of Education Tongji Hospital Tongji University  Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qihao","family":"Xie","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration Ministry of Education Tongji Hospital Tongji University  Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziwen","family":"An","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration Ministry of Education Tongji Hospital Tongji University  Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4909-9796","authenticated-orcid":false,"given":"Lina","family":"Li","sequence":"additional","affiliation":[{"name":"Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute  Shanghai P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8693-1193","authenticated-orcid":false,"given":"Guohua","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration Ministry of Education Tongji Hospital Tongji University  Shanghai P. R. 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