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Herein, atomically dispersed Fe and Mo sites are designed and achieved in the form of well\u2010defined FeN\n                    <jats:sub>4<\/jats:sub>\n                    and MoN\n                    <jats:sub>4<\/jats:sub>\n                    coordination in polyphthalocyanine (PPc) organic framework to investigate the influence of the spin state of FeN\n                    <jats:sub>4<\/jats:sub>\n                    on NRR behavior. The neighboring MoN\n                    <jats:sub>4<\/jats:sub>\n                    can regulate the spin state of Fe center in FeN\n                    <jats:sub>4<\/jats:sub>\n                    from high\u2010spin (\n                    <jats:italic>d<\/jats:italic>\n                    <jats:italic>\n                      <jats:sub>xy<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>2<\/jats:sup>\n                    <jats:italic>\n                      d\n                      <jats:sub>yz<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>1<\/jats:sup>\n                    <jats:italic>\n                      d\n                      <jats:sub>xz<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>1<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    ) to medium\u2010spin (\n                    <jats:italic>\n                      d\n                      <jats:sub>xy<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>2<\/jats:sup>\n                    <jats:italic>\n                      d\n                      <jats:sub>yz<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>2<\/jats:sup>\n                    <jats:italic>\n                      d\n                      <jats:sub>xz<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sup>1<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    ), where the empty d orbitals and separate d electron favor the overlap of Fe 3d with the N 2p orbitals, more effectively activating N\u2261N triple bond. Theoretical modeling suggests that the NRR preferably takes place on FeN\n                    <jats:sub>4<\/jats:sub>\n                    instead of MoN\n                    <jats:sub>4<\/jats:sub>\n                    , and the transition of Fe spin state significantly lowers the energy barrier of the potential determining step, which is conducive to the first hydrogenation of N\n                    <jats:sub>2<\/jats:sub>\n                    . As a result, FeMoPPc with medium\u2010spin FeN\n                    <jats:sub>4<\/jats:sub>\n                    exhibits 2.0 and 9.0 times higher Faradaic efficiency and 2.0 and 17.2 times higher NH\n                    <jats:sub>3<\/jats:sub>\n                    yields for NRR than FePPc with high\u2010spin FeN\n                    <jats:sub>4<\/jats:sub>\n                    and MoPPc with MoN\n                    <jats:sub>4<\/jats:sub>\n                    , respectively. These new insights may open up opportunities for exploiting efficient NRR electrocatalysts by atomically regulating the spin state of metal centers.\n                  <\/jats:p>","DOI":"10.1002\/advs.202102915","type":"journal-article","created":{"date-parts":[[2021,9,2]],"date-time":"2021-09-02T09:33:55Z","timestamp":1630575235000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":117,"title":["Boosting Nitrogen Reduction to Ammonia on FeN\n                    <sub>4<\/sub>\n                    Sites by Atomic Spin Regulation"],"prefix":"10.1002","volume":"8","author":[{"given":"Yajin","family":"Wang","sequence":"first","affiliation":[{"name":"College of Materials Science and Engineering Zhengzhou University  Zhengzhou 450001 P. R. 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