Journal
ACS CATALYSIS
Volume 10, Issue 15, Pages 8557-8566Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c01678
Keywords
CO2 hydrogenation; formic acid; heterogeneous catalysis; polymers; ruthenium
Categories
Funding
- National Key Research and Development Program of China [2018YFB0605801, 2017YFA0403003]
- National Natural Science Foundation of China [21871277, 21603235, 21403248]
- Beijing Municipal Science & Technology Commission [Z181100004218004]
- Recruitment Program of Global Youth Experts of China
- Chinese Academy of Sciences [QYZDY-SSW-SLH013]
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Development of high-performance catalysts for carbon dioxide (CO2) hydrogenation is crucial for CO2 utilization. Herein, a heterogeneous catalyst for CO2 hydrogenation to formate was developed by coordinating the mononuclear Ru3+ center (Ru hereafter) with a N,P-containing polymer, which was synthesized from phosphonitrilic chloride trimer and 2,6-diaminopyridine. Multiple nitrogen functionalities in the polymer (N content: 25.9 wt %) containing pyridine nitrogen and phosphazene nitrogen not only provided an electron-rich coordination environment for stabilizing mononuclear Ru center but also facilitated CO2 conversion by interacting with CO2 molecules. The polymer-coordinated mononuclear Ru catalysts (Ru/p-dop-POMs) could promote the hydrogenation of CO2 to formate with a turnover number (TON) up to 25.4 x 10(3) in aqueous solutions, and the concentration of formate in the solution could reach 3.4 mol/L. DFT calculations revealed that the electron-rich mononuclear Ru site could promote H-2 dissociation, which is the rate-determining step in the reaction, thereby enhancing the catalytic activity. Systemic studies demonstrated that the synergistic effect between individually electron-rich Ru centers and nitrogen-rich polymer enhanced catalytic efficiency.
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