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However, achieving the efficient redox coupling reaction is still challenging due to the lack of suitable electrocatalysts. Herein, we designed two bifunctional polyimides-linked covalent organic frameworks (PI-COFs) through assembling phthalocyanine (Pc) and porphyrin (Por) by non-toxic hydrothermal methods in pure water to realize the above catalytic reactions. Due to the high conductivity and well-defined active sites with different chemical environments, NiPc-NiPor COF performs efficient ECR coupled with methanol oxidation reaction (MOR) (Faradaic efficiency of CO (FECO) = 98.12%, partial current densities of CO (jCO) = 6.14\u00a0mA cm\u22122 for ECR, FEHCOOH\u00a0=\u00a093.75%, jHCOOH\u00a0=\u00a05.81\u00a0mA cm\u22122 for MOR at low cell voltage (2.1\u00a0V) and remarkable long-term stability). Furthermore, experimental evidences and density functional theory (DFT) calculations demonstrate that the ECR process mainly conducts on NiPc unit with the assistance of NiPor, meanwhile, the MOR prefers NiPor conjugating with NiPc. The two units of NiPc-NiPor COF collaboratively promote the coupled oxidation-reduction reaction. For the first time, this work achieves the rational design of bifunctional COFs for coupled heterogeneous catalysis, which opens a new area for crystalline material catalysts.<\/jats:p>","DOI":"10.1093\/nsr\/nwad226","type":"journal-article","created":{"date-parts":[[2023,9,3]],"date-time":"2023-09-03T08:27:54Z","timestamp":1693729674000},"source":"Crossref","is-referenced-by-count":70,"title":["Green synthesis of bifunctional phthalocyanine-porphyrin COFs in water for efficient electrocatalytic CO2 reduction coupled with methanol oxidation"],"prefix":"10.1093","volume":"10","author":[{"given":"Mi","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia-Peng","family":"Liao","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Run-Han","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sheng-Nan","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Meng","family":"Lu","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Long-Zhang","family":"Dong","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pei","family":"Huang","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shun-Li","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue-Peng","family":"Cai","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ya-Qian","family":"Lan","sequence":"additional","affiliation":[{"name":"School of Chemistry, South China Normal University , Guangzhou \u00a0 510006 , China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"286","published-online":{"date-parts":[[2023,9,2]]},"reference":[{"key":"2024011507520794200_bib1","doi-asserted-by":"publisher","first-page":"7610","DOI":"10.1021\/acs.chemrev.8b00705","article-title":"Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte","volume":"119","author":"Nitopi","year":"2019","journal-title":"Chem Rev"},{"key":"2024011507520794200_bib2","doi-asserted-by":"publisher","first-page":"6640","DOI":"10.1021\/jacs.2c02245","article-title":"Utilization of low-concentration CO2 with molecular catalysts assisted by CO2-capturing ability of catalysts, additives, or reaction media","volume":"144","author":"Yamazaki","year":"2022","journal-title":"J Am Chem Soc"},{"key":"2024011507520794200_bib3","doi-asserted-by":"publisher","first-page":"53","DOI":"10.1093\/nsr\/nwz096","article-title":"Multielectron transportation of polyoxometalate-grafted metalloporphyrin 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