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Molecular catalysts, such as cobalt phthalocyanine (CoPc), are known to be effective in converting carbon dioxide (CO\n                    <jats:sub>2<\/jats:sub>\n                    ) to CO. However, increasing the rate and selectivity of this reaction remains challenging and sometimes complicated. In this work, we report a simple molecule\u2010coadsorption strategy to improve the efficiency of CoPc\u2010catalyzed electrocatalytic conversion of CO\n                    <jats:sub>2<\/jats:sub>\n                    to CO on graphitic carbon nitride (g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    ). By coadsorbing nitropyrene (NPy) molecules, together with CoPc, on the surface of graphitic g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    <jats:italic>via \u03c0\u2013\u03c0<\/jats:italic>\n                    conjugation, the catalytic activity of CoPc increased by 84%, and the Faradaic efficiency (FE) of CO increased up to 98.2% \u00b1 1.6% in a H\u2010type cell. This FE could further improve up to \u223c100% in a flow cell. The improved catalysis performance could be attributed to the NPy\u2010modulated change in electronic structure of the cobalt center in CoPc and the modulated reaction thermodynamics. Overall, this work paves a new way for fine modulation of the electronic structure of molecular catalysts for improvements in both activity and selectivity.\n                  <\/jats:p>","DOI":"10.1002\/smll.75194","type":"journal-article","created":{"date-parts":[[2026,8,11]],"date-time":"2026-08-11T07:50:11Z","timestamp":1786434611000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Electronic Modulation of the Cobalt Phthalocyanine on G\u2010C\n                    <sub>3<\/sub>\n                    N\n                    <sub>4<\/sub>\n                    via Coadsorbing Nitropyrene for Improved Electroreduction of Carbon Dioxide to Carbon Monoxide"],"prefix":"10.1002","volume":"22","author":[{"given":"Kun","family":"Gao","sequence":"first","affiliation":[{"name":"School of Flexible Electronics (Future Technologies) State Key Laboratory of Flexible Electronics and Institute of Advanced Materials Nanjing Tech University  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Miao","family":"Ji","sequence":"additional","affiliation":[{"name":"School of Flexible Electronics (Future Technologies) State Key Laboratory of Flexible Electronics and Institute of Advanced Materials Nanjing Tech University  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinya","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Flexible Electronics (Future Technologies) State Key Laboratory of Flexible Electronics and Institute of Advanced Materials Nanjing Tech University  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qinghua","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Flexible Electronics (Future Technologies) State Key Laboratory of Flexible Electronics and Institute of Advanced Materials Nanjing Tech University  Nanjing P. R. 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