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High-efficiency catalyst and method for catalyzing formic acid dehydrogenation and reduction reaction

A catalyst, formic acid technology, applied in catalytic reactions, chemical instruments and methods, catalysts for physical/chemical processes, etc., can solve the problem of low atomic economy, and achieve the effects of excellent water solubility, high efficiency, and low catalyst dosage

Pending Publication Date: 2020-06-19
北京青木子科技发展有限公司
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

In their work, using 5 equivalents of sodium formate as a hydrogen donor, aldehydes can be efficiently reduced (TOF can reach 50,000), but sodium formate needs to be specially removed after the reaction, and the atom economy is not high

Method used

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  • High-efficiency catalyst and method for catalyzing formic acid dehydrogenation and reduction reaction
  • High-efficiency catalyst and method for catalyzing formic acid dehydrogenation and reduction reaction
  • High-efficiency catalyst and method for catalyzing formic acid dehydrogenation and reduction reaction

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0050] Catalyst cat-1 (structure see figure 1 ) preparation:

[0051] To a 100 mL round bottom flask was added the ligand 2-(4,5-dihydro-1-imidazole)pyridine (440 mg, 3 mmol), [Cp*IrCl 2 ] 2 (1.2g, 1.5mmol) and 30mL of dichloromethane, stirred until all the solids were dissolved, stirred at room temperature for 12h, then added silver tetrafluoroborate (585mg, 3mmol) to the flask, stirred for 30 minutes and then added sodium fluoride ( 126mg, 3mmol) continued to stir for 3h, then removed the solvent on a rotary evaporator, and the obtained solid was washed 3 times with ethyl acetate to obtain a tan solid, which was the catalyst cat-1 (1.2g, 2.3mmol), the yield 77%.

[0052] The catalyst cat-1 (5.6 mg, 10 μmol) was weighed and dissolved in 1 mL of deionized water, mixed to form a homogeneous solution, and then 0.1 mL of the mixed solution was taken and diluted to 10 mL with deionized water and placed in a 50 mL round bottom flask. Put the round-bottomed flask containing the ...

Embodiment 2

[0056] Others are the same as embodiment 1, but the catalyst used is changed into cat-2 (structure sees figure 1 , the preparation method is the same as cat-1, except that the ligand is changed to 2-(1-methyl-4,5-dihydro-1-imidazole)pyridine), and the results are shown in Table 1.

Embodiment 3

[0058] Others are the same as embodiment 1, but the catalyst used is changed into cat-3 (structure sees figure 1 , the preparation method is the same as cat-1, except that the ligand is changed to 4,4',5,5'-tetramethyl-1H, 1'H-2,2'-diimidazole), and the results are shown in Table 1.

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Abstract

The invention belongs to the technical field of catalysts, and relates to a high-efficiency catalyst and a method for catalyzing formic acid dehydrogenation and reduction reaction by the high-efficiency catalyst. The structure of the catalyst is shown as a formula (I), M is a metal atom and is selected from one of iridium, rhodium, ruthenium, iron, cobalt, silver, palladium, nickel and gold, Y isselected from one of NO3 <->, ClO4 <->, BF4 <->, SO4 < 2->, SbF6 <->, PF6 <->, Cl <-> and acetyl, X is selected from one of Cl, Br, I, F and OH, can also be a neutral ligand, and is selected from oneof water, methanol, ethanol and tetrahydrofuran, Z is selected from one of hydrogen, methyl and ethyl, n is 1 or 2, R is an electron-donating group from the 3-position to the 6-position on a pyridinering and is selected from MeO, R'O, Me2N or R'2N, and R' is selected from one of alkyl, naphthenic base and aryl, or R is an optional electron withdrawing group. By utilizing the efficient catalyst and the method for catalyzing the formic acid dehydrogenation and reduction reaction, the formic acid dehydrogenation and reduction reaction can be efficiently catalyzed.

Description

technical field [0001] The invention belongs to the technical field of catalysts, and relates to a high-efficiency catalyst and a method for catalyzing formic acid dehydrogenation and reduction reactions. Background technique [0002] Hydrogen has always been considered as an efficient and clean energy, but storage and transportation have become the key technical bottlenecks restricting hydrogen as a new energy, and chemical storage can effectively solve this problem. [0003] Formic acid as a hydrogen carrier has received extensive attention in recent years. The content of hydrogen in formic acid is 4.3wt% (53g L -1 ), and formic acid is a stable and non-toxic liquid at room temperature, which is more convenient to store and transport than hydrogen, so decomposing formic acid to produce hydrogen has become one of the hot research topics at home and abroad. [0004] The applicant has previously developed an iridium metal catalyst with a nitrogen-containing heterocycle as a...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/22C07F17/02C01B3/22C01B32/50C07C29/14C07C29/143C07C37/00C07C41/26C07C45/64C07C51/367C07C67/29C07C201/12C07C253/30C07D213/30C07D213/69C07D307/42C07D307/44C07C43/23C07C43/295C07C39/24C07C49/825C07C205/19C07C65/01C07C31/125C07C33/46C07C69/16C07C255/36C07B41/02
CPCB01J31/2295C07F17/02C01B3/22C01B32/50C07C41/26C07C37/002C07C45/64C07C201/12C07C51/367C07D213/69C07D307/44C07C29/14C07C29/143C07C67/29C07C253/30C07D213/30C07D307/42C07B41/02C01B2203/0277B01J2531/827B01J2531/0238B01J2231/763B01J2231/643C07C2601/18C07C43/23C07C43/295C07C39/245C07C49/825C07C205/19C07C65/01C07C31/125C07C33/46C07C69/16C07C255/36
Inventor 刘继田郑俊荣
Owner 北京青木子科技发展有限公司
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