4.8 Article

A strategy to address the challenge of electrochemical CO2 and N2 coupling to synthesis urea on two-dimensional metal borides (MBenes) by computational screening

期刊

MATERIALS TODAY PHYSICS
卷 26, 期 -, 页码 -

出版社

ELSEVIER
DOI: 10.1016/j.mtphys.2022.100726

关键词

Metal borides (MBenes); Coupling urea production; CO2 electroreduction; Electrochemical synthesis; Computational screening; Descriptors

资金

  1. China Scholarship Council [CSC: 201808440416]
  2. National Natural Science Foundation of China [52002338]
  3. Science and Technology Planning Project of Sichuan Province [2021ZYD0053]
  4. Science and Technology Planning Project of Sichuan Province

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A new approach for synthesizing urea on 2D metal borides (MBenes) via electrocatalytic C-N coupling was proposed, utilizing sustainable energy (solar energy) to address the challenge of activating CO2 and N-2 molecules. Computational screening was used to identify efficient catalysts for urea electrosynthesis based on the C-N coupling mechanism.
To achieve efficient urea formation via electrocatalytic C-N coupling, we proposed a new route for synthesizing urea on 2D metal borides (MBenes) by theoretical prediction. It has been reported that inert CO2 and N-2 molecules can be converted into urea via electrocatalytic C-N bond coupling, which is a promising alternative method to industrial processes. However, due to the weak adsorption of and difficulty in activating CO2 and N-2 molecules, the reaction of C-N coupling is challenging to achieve. To ensure C-N bond coupling between *N equivalent to N* and *CO to form *NCON intermediates, which act as the key precursor to urea formation, the utilization of sustainable energy (solar energy) can be helpful in addressing the challenge of electrochemically synthesizing urea. Furthermore, computational screening provides an effective way to gain insight into the mechanisms of the C-N coupling and protonation steps. It is also beneficial for guiding the development of the sustainable synthesis of carbon nitride chemicals via C-N coupling, and we believe it will attract full attention in the future. A new theoretical strategy was used to screen efficient catalysts for urea electrosynthesis based on coupling CO2 and N-2 to generate H2NCONH2. We established the Gibbs free energy landscape and calculated the limiting potential based on the rate-determining step, and a volcano plot was constructed as a function of delta G(*NCON) to predict MBenes for urea formation. It included the kinetic stability, CO2 and N-2 adsorbability, catalytic activity, and urea synthesis selectivity. It is demonstrated that Mo2B2 and Ru2B4 are suitable urea electrosynthesis catalysts with high activity and selectivity. This work can contribute to the application of C-N coupling electrochemical reactions.

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