Chemical fixation of CO2 for the synthesis of valuable chemicals is very demanding in the context of green and sustainable chemistry. Herein, we report highly efficient silver-loaded porous organic polymer catalysts for the exclusive N-formylation and N-methylation of amines under ambient reaction conditions using CO2 as a green C1 source. By adjusting the solvent and temperature of the reaction, the successful production of formamides and methylamines could be accomplished with high levels of selectivity and efficiency. POP-based materials Ag@TTP-1 and Ag@PAN-T are utilized as low-cost catalysts for both the N-methylation and N-formylation of primary and secondary amines and the product yields up to 98 % could be achieved. Ag@TTP-1 demonstrated superior catalytic efficiency compared to Ag@PAN-T in the N-methylation and N-formylation reactions. This result suggests that the grafting of Ag nanoparticles onto POP surface with a high surface area plays a crucial role in these CO2 fixation reactions. The above-mentioned catalysts (Ag@TTP-1 and Ag@PAN-T) are characterized through powder XRD, FT IR spectroscopy, FE-SEM, TEM, thermogravimetric techniques, N-2 sorption and XPS analysis. Ag-nanocatalysts demonstrated heterogeneous nature and high recycling efficiency for several cycles in this CO2 fixation reaction.
机构:
Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Univ Chinese Acad Sci, Beijing 100049, Peoples R ChinaChinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Huang, Zijun
Jiang, Xiaolin
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Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Shenyang Pharmaceut Univ, Key Lab Struct Based Drug Design & Discovery, Minist Educ, Shenyang 110016, Liaoning, Peoples R ChinaChinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Jiang, Xiaolin
Zhou, Shaofang
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Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R ChinaChinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Zhou, Shaofang
Yang, Peiju
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Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R ChinaChinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Yang, Peiju
Du, Chen-Xia
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机构:
Zhengzhou Univ, Coll Chem & Mol Engn, Zhengzhou 450001, Henan, Peoples R ChinaChinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
Du, Chen-Xia
Li, Yuehui
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Chinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R ChinaChinese Acad Sci, State Key Lab Oxo Synth & Select Oxidat, Suzhou Res Inst, LICP, Lanzhou 730000, Gansu, Peoples R China
机构:
Univ Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R ChinaUniv Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
Wei, Xiu-Zhi
Lu, Qiqi
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Chinese Acad Sci, Guangzhou Inst Energy Convers, CAS Key Lab Renewable Energy, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R ChinaUniv Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
Lu, Qiqi
Liu, Jianguo
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Southeast Univ Nanjing, Sch Energy & Environm, Minist Educ, Key Lab Energy Thermal Convers & Control, Nanjing 210096, Peoples R ChinaUniv Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
Liu, Jianguo
Ma, Longlong
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Univ Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
Southeast Univ Nanjing, Sch Energy & Environm, Minist Educ, Key Lab Energy Thermal Convers & Control, Nanjing 210096, Peoples R ChinaUniv Sci & Technol China, Dept Engn Sci, Hefei 230026, Peoples R China
机构:
China Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China
Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R ChinaChina Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China
Zhang, Suqi
Mei, Qingqing
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Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R ChinaChina Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China
Mei, Qingqing
Liu, Hangyu
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Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R ChinaChina Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China
Liu, Hangyu
Liu, Huizhen
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Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R ChinaChina Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China
Liu, Huizhen
Zhang, Zepeng
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China Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R ChinaChina Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China
Zhang, Zepeng
Han, Buxing
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Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R ChinaChina Univ Geosci, Sch Mat Sci & Technol, Beijing 100083, Peoples R China