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Formic acid dehydrogenation catalysts in aqueous system, and application thereof

A catalyst, formic acid technology, applied in the direction of organic compound/hydride/coordination complex catalyst, physical/chemical process catalyst, hydrogen, etc., to achieve the effect of easy mass synthesis, high formic acid dehydrogenation activity, and cheap raw materials

Inactive Publication Date: 2016-07-20
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

This type of catalyst is easy to synthesize, has good stability, and is easy to adjust its structure, so it is suitable for mass production. This type of catalyst can be generated in situ or prepared before the reaction. Its application in formic acid dehydrogenation has not been reported at home or abroad.

Method used

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  • Formic acid dehydrogenation catalysts in aqueous system, and application thereof
  • Formic acid dehydrogenation catalysts in aqueous system, and application thereof
  • Formic acid dehydrogenation catalysts in aqueous system, and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0030] Weigh [Cp*IrCl 2 ] 2 (4.0mg, 5.0μmol) and L1 (6.8mg, 50μmol) were placed in a reagent bottle, and 10mL of degassed pure water was added to prepare an aqueous solution of the in-situ catalyst. Add a stirring magnet, water (8.62mL) and 1.0mL (0.5μmol) of the above prepared catalyst solution to a Schlenk reaction bottle (50mL), seal it with a rubber stopper, put it in a water bath at 60°C and stir for 10min Finally, unscrew the branch pipe to communicate with the atmosphere, then close it, connect the rubber tube to the inverted 500mL graduated cylinder filled with water in the water basin, inject formic acid (10mmol, 0.38mL) into the reaction bottle through the rubber stopper with a syringe, and start timing. Open the branch pipe piston and collect the gas by draining. Calculate the amount of gas collected per unit time, calculate TON and TOF, V(CO 2 )=Volume / 2 of drained water, the amount of formic acid decomposed M(CO 2 ) = V(CO 2 ) / 24, see Table 1 for specific dat...

Embodiment 2

[0032] Same as Example 1, except that ligand L2 was used instead of L1 for the reaction, and the results are shown in Table 1.

Embodiment 3

[0034] Same as Example 1, except that ligand L3 was used instead of L1 for the reaction, and the results are shown in Table 1.

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Abstract

Formic acid dehydrogenation catalysts used in an aqueous system comprise a metal and a ligand, the metal is iridium, rhodium, ruthenium, iron, copper, cobalt, palladium, platinum, osmium, or nickel, and the ligand is a heterocyclic compound with the structure containing C=N. The catalysts are used in the formic acid dehydrogenation reaction of the aqueous system for the first time, and the highest TOF at 90DEG C under alkali-free conditions can reach 37.5*10<4>h<-1>, and the highest TON at 80DEG C can reach 240*10<4>, and is the highest reported value.

Description

technical field [0001] The present invention relates to a kind of catalyst that is used for the dehydrogenation of formic acid in the aqueous phase system, is specifically made of a kind of bidentate or multidentate ligand containing C=N double bond structure and iridium, rhodium, ruthenium, iron, copper Catalysts generated from various metal precursors. Background technique [0002] Hydrogen is an efficient and clean energy, but hydrogen has very low volume energy density and mass energy density. Safe and efficient storage and transportation of hydrogen has become a major challenge for hydrogen energy utilization. In order to solve this problem, people have developed a variety of hydrogen storage materials. Formic acid, as one of the liquid hydrogen storage materials, has attracted people's attention because of its non-toxic, high mass energy density, and safe storage and transportation. The catalysts used to decompose formic acid to produce hydrogen in a homogeneous syste...

Claims

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Application Information

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IPC IPC(8): B01J31/22C01B3/22C01B3/32C01B31/20C01B32/50
Inventor 李灿卢胜梅王志君李军
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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