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Advanced functional materials: Lewis base structure facilitates electrochemical nitrogen fixation under dual control of thermodynamics and kinetics

wallpapers News 2020-09-15

ammonia is widely used in social production is an important basic raw material for various industries. Based on the current research dem under mild environmental conditions using renewable energy as the driving force using electrochemical technology to reduce nitrogen to synthesize ammonia to replace the 100 year old Haber Bosch process is known as the most promising synthesis strategy. The successful construction of efficient electrochemical ammonia synthesis system depends on the continuous improvement of the yield efficiency of the catalytic reaction but it is still limited by the following two key scientific issues: first the critical step of nitrogen reduction is the breaking of n ≡ n triple bond which has a very high dissociation energy (941 kJ) Secondly due to the extremely low solubility of nitrogen in water the diffusion ability of the gas at the reaction interface is reduced due to the collision aggregation of gas molecules finally the performance of the system is greatly limited due to the insufficient mass transfer of reactants. Therefore it is of great significance to systematically study the thermodynamic kinetic mechanism of electrochemical reaction interface reasonably control it.   

Qian Tao team of

Suzhou University simplified decomposed the complex problem of improving the macro performance of electrochemical ammonia synthesis into targeted regulation of thermodynamics kinetics of micro interface innovatively proposed that by introducing a large number of Lewis base groups into the electrocatalytic materials reasonably controlling the interface process the excellent electrocatalytic activity selection of electrochemical ammonia synthesis can be realized Sex. First principles calculations show that Lewis base group can effectively control the electronic structure of the catalyst greatly reduce the n ≡ n fracture barrier accelerate the dissociation process of nitrogen. In addition the molecular dynamics simulation results show that such abundant Lewis base groups will help to enhance the surface heterogeneity of the catalyst the enhanced intermolecular force between nitrogen catalyst will drive the efficient mass transfer of nitrogen at the interface which will help the subsequent reaction process. The electrochemical test results show that the Faraday efficiency of the proof of concept system reaches 62.9% at a low potential of - 0.2 V vs rhe. In this work the thermodynamic kinetic mechanism of the electrochemical ammonia synthesis system was analyzed through experiments theories which provided a universal design strategy for the electrochemical ammonia synthesis system.

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