{
  "abstract": "Electrocatalytic nitrate reduction reaction (e-NO₃RR) offers a promising route to valorize nitrate-contaminated wastewater while enabling sustainable ammonia production; however, how local coordination asymmetry regulates Cu-site evolution and reaction pathways across different pH environments remains insufficiently understood. Herein, three- and four-nitrogen-coordinated Cu single-atom motifs, denoted as Cu─N₃ and Cu─N₄, are constructed as well-defined pre-catalyst models to elucidate how the initial Cu coordination environment directs pH-dependent active-site reconstruction. Operando X-ray absorption spectroscopy and wavelet-transform EXAFS reveal that Cu─N₄ readily undergoes rapid reconstruction under acidic, neutral, and alkaline conditions, generating low-coordinated, electron-enriched Cu species while concomitantly inducing Cu─Cu aggregation and excessive Cu─site reduction. In contrast, Cu─N₃ displays more regulated site evolution, with limited activation under acidic conditions but progressive formation of low-coordinated Cu─Nx active structures under neutral and alkaline conditions. In situ ATR-FTIR further verifies that the dynamically evolved Cu─N₃ sites enhance nitrate adsorption, facilitate N─O bond activation, and promote the formation of hydrogenated nitrogen intermediates. These findings establish coordination-governed site evolution as a design principle for balancing productive Cu─site activation and metal-centered over-reduction, providing molecular-level guidance for the design of pH-adaptive NO₃RR catalysts.",
  "abstract_shown": true,
  "affiliations": [
    "Scientific Research Division, National Synchrotron Radiation Research Center, Hsinchu, Taiwan.",
    "Department of Chemistry, National Taiwan University, Taipei, Taiwan.",
    "Department of Materials Science and Engineering, National Yang Ming Chiao Tung University, Hsinchu, Taiwan.",
    "Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu, Taiwan.",
    "Experimental Facility Division, National Synchrotron Radiation Research Center, Hsinchu, Taiwan."
  ],
  "article_type": "research article",
  "arxiv": null,
  "author_total": 12,
  "authors": [
    {
      "affs": [
        0
      ],
      "name": "Shih-Ching Huang",
      "orcid": "0000-0002-6499-6973"
    },
    {
      "affs": [
        0
      ],
      "name": "Yu-Ru Lin"
    },
    {
      "affs": [
        1
      ],
      "name": "Hsiang-Chun Yu"
    },
    {
      "affs": [
        2
      ],
      "name": "Yi-Dong Lin"
    },
    {
      "affs": [
        3
      ],
      "name": "Yu-Chiao Chang"
    },
    {
      "affs": [
        0
      ],
      "name": "Chun-Kuo Peng"
    },
    {
      "affs": [
        4
      ],
      "name": "Yu-Chang Lin",
      "orcid": "0000-0001-7531-9591"
    },
    {
      "affs": [
        2
      ],
      "name": "Wen-Wei Wu",
      "orcid": "0000-0002-8388-8417"
    },
    {
      "affs": [
        1
      ],
      "name": "Hao Ming Chen",
      "orcid": "0000-0002-7480-9940"
    },
    {
      "affs": [
        4
      ],
      "name": "Chi-Liang Chen",
      "orcid": "0000-0001-8509-0655"
    },
    {
      "affs": [
        3
      ],
      "name": "Han-Yi Chen",
      "orcid": "0000-0001-8146-7101"
    },
    {
      "affs": [
        0,
        2
      ],
      "name": "Yan-Gu Lin",
      "orcid": "0000-0002-4210-7709"
    }
  ],
  "bibtex": "https://research.draconitic.com/paper/9xbe6es00h247.bib",
  "cited_by": 0,
  "doi": "10.1002/advs.78164",
  "fulltext_url": "https://europepmc.org/articles/PMC13669220",
  "id": "9xbe6es00h247",
  "issns": [
    "2198-3844"
  ],
  "landing_url": "https://europepmc.org/article/MED/42875820",
  "language": "eng",
  "licence": "CC-BY",
  "licence_label": "CC BY",
  "licence_source": "article",
  "licence_url": "https://creativecommons.org/licenses/by/4.0/",
  "metadata_licence": null,
  "native_subjects": [
    [
      "openalex",
      "1503|Ammonia Synthesis and Nitrogen Reduction"
    ]
  ],
  "openalex": "W7221754822",
  "pdf_url": "https://europepmc.org/articles/PMC13669220?pdf=render",
  "pmcid": "PMC13669220",
  "pmid": "42875820",
  "published": "2026-10-14",
  "publisher": null,
  "ris": "https://research.draconitic.com/paper/9xbe6es00h247.ris",
  "sources": [
    {
      "first_seen": "2026-10-30T12:18:46Z",
      "native_id": "MED:42875820",
      "source": "europepmc",
      "url": "https://europepmc.org/article/MED/42875820"
    }
  ],
  "subjects": [
    {
      "field": "chemistry",
      "origin": "openalex:1503|Ammonia Synthesis and Nitrogen Reduction",
      "subfield": "catalysis"
    }
  ],
  "title": "Coordination-Asymmetry-Regulated Reconstruction of Electron-Rich Cu Sites for pH-Dependent Nitrate-to-Ammonia Electrocatalysis.",
  "title_text": "Coordination-Asymmetry-Regulated Reconstruction of Electron-Rich Cu Sites for pH-Dependent Nitrate-to-Ammonia Electrocatalysis.",
  "type": "peer-reviewed",
  "updated_at": "2026-10-30T12:18:46Z",
  "url": "https://research.draconitic.com/paper/9xbe6es00h247",
  "venue": "Advanced science (Weinheim, Baden-Wurttemberg, Germany)",
  "versions": []
}