Osman Ali, Aruntima Das, Anupam Jana, Sinjini Mandal, Ashadul Adalder, Dr. Bholanath Maity, Dr. Asamanjoy Bhunia
{"title":"[Ir(ppy) 2 (H2dcbpy)]和分子镍配合物在光催化CO2还原金属-有机框架中的功能集成","authors":"Osman Ali, Aruntima Das, Anupam Jana, Sinjini Mandal, Ashadul Adalder, Dr. Bholanath Maity, Dr. Asamanjoy Bhunia","doi":"10.1002/cctc.202500844","DOIUrl":null,"url":null,"abstract":"<p>Developing multifunctional photocatalysts that efficiently convert CO₂ into valuable chemical products (e.g., CO, CH<sub>4</sub>, HCOOH, and CH<sub>3</sub>OH) is essential for achieving sustainable development. To address this challenge, we report a remarkable multifunctional metal-organic framework (MOF)-based photocatalyst, termed UiO-67-Ni-Ir, which has been elegantly crafted through an in situ synthesis strategy. This promising catalyst contains a highly efficient light-absorbing iridium unit, [Ir(ppy)₂(H2dcbpy)] (where ppy = 2-phenylpyridine, H<sub>2</sub>dcbpy = 2,2′-bipyridine-4,4′-dicarboxylic acid), referred to as Ir-PS, in conjunction with a catalytically active nickel center. The broad absorption of visible light of the Ir-PS unit empowers the efficient CO<sub>2</sub> reduction reactions under visible light illumination. The photocatalyst UiO-67-Ni-Ir exhibits exceptional photocatalytic performance, producing 5800 µmol g<sup>−1</sup> of formate (HCOO⁻) over a 6 h period with a remarkable selectivity of 96.5%. This high formate yield is further supported by a turnover number (TON) exceeding 51 during the same photocatalysis run, which is ten times higher than that of the corresponding homogeneous system. Moreover, this catalyst is completely heterogeneous and recyclable, making it an attractive candidate for the photocatalytic conversion of CO<sub>2</sub> to formate under visible light irradiation. Furthermore, a plausible mechanism has been proposed based on the photophysical and electrochemical study along with density functional theory (DFT), which provides a comprehensive understanding of the underlying catalytic process.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 18","pages":""},"PeriodicalIF":3.9000,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Functional Integration of [Ir(ppy)₂(H2dcbpy)] and a Molecular Nickel Complex into Metal-Organic Frameworks for Photocatalytic CO2 Reduction\",\"authors\":\"Osman Ali, Aruntima Das, Anupam Jana, Sinjini Mandal, Ashadul Adalder, Dr. Bholanath Maity, Dr. Asamanjoy Bhunia\",\"doi\":\"10.1002/cctc.202500844\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Developing multifunctional photocatalysts that efficiently convert CO₂ into valuable chemical products (e.g., CO, CH<sub>4</sub>, HCOOH, and CH<sub>3</sub>OH) is essential for achieving sustainable development. To address this challenge, we report a remarkable multifunctional metal-organic framework (MOF)-based photocatalyst, termed UiO-67-Ni-Ir, which has been elegantly crafted through an in situ synthesis strategy. This promising catalyst contains a highly efficient light-absorbing iridium unit, [Ir(ppy)₂(H2dcbpy)] (where ppy = 2-phenylpyridine, H<sub>2</sub>dcbpy = 2,2′-bipyridine-4,4′-dicarboxylic acid), referred to as Ir-PS, in conjunction with a catalytically active nickel center. The broad absorption of visible light of the Ir-PS unit empowers the efficient CO<sub>2</sub> reduction reactions under visible light illumination. The photocatalyst UiO-67-Ni-Ir exhibits exceptional photocatalytic performance, producing 5800 µmol g<sup>−1</sup> of formate (HCOO⁻) over a 6 h period with a remarkable selectivity of 96.5%. This high formate yield is further supported by a turnover number (TON) exceeding 51 during the same photocatalysis run, which is ten times higher than that of the corresponding homogeneous system. Moreover, this catalyst is completely heterogeneous and recyclable, making it an attractive candidate for the photocatalytic conversion of CO<sub>2</sub> to formate under visible light irradiation. 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Functional Integration of [Ir(ppy)₂(H2dcbpy)] and a Molecular Nickel Complex into Metal-Organic Frameworks for Photocatalytic CO2 Reduction
Developing multifunctional photocatalysts that efficiently convert CO₂ into valuable chemical products (e.g., CO, CH4, HCOOH, and CH3OH) is essential for achieving sustainable development. To address this challenge, we report a remarkable multifunctional metal-organic framework (MOF)-based photocatalyst, termed UiO-67-Ni-Ir, which has been elegantly crafted through an in situ synthesis strategy. This promising catalyst contains a highly efficient light-absorbing iridium unit, [Ir(ppy)₂(H2dcbpy)] (where ppy = 2-phenylpyridine, H2dcbpy = 2,2′-bipyridine-4,4′-dicarboxylic acid), referred to as Ir-PS, in conjunction with a catalytically active nickel center. The broad absorption of visible light of the Ir-PS unit empowers the efficient CO2 reduction reactions under visible light illumination. The photocatalyst UiO-67-Ni-Ir exhibits exceptional photocatalytic performance, producing 5800 µmol g−1 of formate (HCOO⁻) over a 6 h period with a remarkable selectivity of 96.5%. This high formate yield is further supported by a turnover number (TON) exceeding 51 during the same photocatalysis run, which is ten times higher than that of the corresponding homogeneous system. Moreover, this catalyst is completely heterogeneous and recyclable, making it an attractive candidate for the photocatalytic conversion of CO2 to formate under visible light irradiation. Furthermore, a plausible mechanism has been proposed based on the photophysical and electrochemical study along with density functional theory (DFT), which provides a comprehensive understanding of the underlying catalytic process.
期刊介绍:
With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.