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Image: (a) Current production and application
of NH3.
Almost all synthetic nitrogenous organic compounds are synthesized from NH3
.
(b) Synthesis of nitrogenous organic compounds
directly from N2 molecules and carbon sources.
(c) Our overall strategy to achieve the above objectives: to use heterogeneous processes to produce active intermediate nitrogenous species, and then to produce valuable organic compounds
using homogeneous synthesis methods.
(d) This work serves as a proof of
concept.
N2 gas is first fixed with carbon and LiH to form active Li2CN2, and then converted into nitrogen-containing organic compounds
by homogeneous synthesis.
Elemental nitrogen is necessary for
life and human society.
However, almost all of the N atoms in the currently synthetic nitrogenous compounds come from NHH3 It was mass-produced
by the Haber-Bosch process developed in the early 20th century.
Although the Haber-Bosch process is one of the greatest inventions in human history, it puts enormous pressure on
our environment and energy.
"If we can bypass ammonia and directly synthesize complex organic compounds from nitrogen and carbon, it will reduce the number of operational steps, thereby saving a lot of energy and creating great economic value
for society.
"
In this study, the researchers proposed a homogeneous-heterogeneous synergistic strategy to solve this problem
.
N2 gas is first converted into sufficiently active nitrogenous substances (N*)
by a heterogeneous process.
Subsequent homogeneous reactions are then performed to construct complex nitrogenous organic compounds, taking advantage of
both research methods.
Specifically, N2 gas and carbon are first fixed with LiH in a homemade reactor at 550oC (heterogeneous process) to form a reaction intermediate Li2CN2 with high selectivity and high efficiency.
Li2CN2 is then transferred to a glass flask and used as an organic synthesis to build carbodiimine and pyrimidine, building DNA/RNA (homogenization process).
In addition, the corresponding15N-labeled carbodiimide and pyrimidine can also be efficiently prepared using 15N2as a raw material, which may have a wide range of biochemical applications
.
Hydride (H-) plays a special role
in nitrogen fixation in our body.
It guides the different reaction pathways of N2 with mild and controllable
fixation and conversion reactions compared to traditional transition metals.
Our products can be conveniently obtained
in grams in the laboratory.
Further amplification of production by equipping a larger reactor would be straightforward
.
The homogeneous-heterogeneous synergistic strategies outlined here differ from those of the previous ones
.
In general, the formation of carbon-nitrogen bond 2 gas from N atoms requires the reduction of N2 to make it react
with electrophilic carbon.
However, under most conditions, reducing agents are incompatible
with carbon electrophiles.
In this study, the incompatibility problem
was solved by using elemental carbon directly as a carbon source.
The researchers plan to continue this strategy in the future to synthesize more useful organic compounds
.
This research was supported
by the National Natural Science Foundation of China "Basic Science Center for Translational Chemistry of Key Components of Air" (21988101).
There were no reports
of conflicts of interest.
