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Design and Synthesis of Two-dimensional Conjugated MOFs and High-Efficiency Electrocatalytic Carbon Dioxide Reduction Have Been Improved

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Carbon dioxide conversion performance of HATNA-Cu-MOF

Global climate change is a major challenge of human existence. With the widespread use of petrochemical resources, the concentration of carbon dioxide in the atmosphere has rapidly increased from 278 ppm before the industrial revolution to 420 ppm, which has brought a profound impact on the global environment. Although China's carbon dioxide emissions have shown a downward trend, the total annual emissions are still close to one-third of global emissions. To this end, China has proposed a new nationally determined contribution measure of “strive to reach the peak of carbon dioxide emissions by 2030 and strive to achieve carbon neutrality by 2060”. "Doing a good job in carbon peaking and carbon neutrality" is one of the key tasks of China during the "14th Five-Year Plan" period. Carbon neutrality means that by 2060, various ways will be adopted to offset all the carbon dioxide emissions. Using renewable clean energy to capture and transform carbon dioxide through chemical methods is a way with great potential.

A few days ago, special associate researcher Li Pengfei of the Advanced Institute of Multidisciplinary Science of Beijing Institute of Technology and Professor Wang Bo from the School of Chemistry and Chemical Engineering designed and synthesized new two-dimensional copper-based conjugated MOFs material based on HATNA-6OH structural units. By rationally designing the reaction conditions and selectively using the catechol unit in the HATNA-6OH ligand to coordinate with the metal copper ion, a two-dimensional conjugated HATNA-Cu-MOF with CuO4 coordination center was obtained.

Because HATNA-Cu-MOF shows strong carbon dioxide adsorption capacity and good conductivity, they explored the electrocatalytic carbon dioxide reduction performance of HATNA-Cu-MOF. The research results show that HATNA-Cu-MOF exhibits high selectivity of carbon dioxide reduction to produce methane, Faraday efficiency of which is as high as 78%. In addition, HATNA-Cu-MOF has good stability, and its carbon dioxide reduction current density and selectivity have not been significantly attenuated during the 12-hour electrocatalytic process.

This work not only expands the types of ligands for two-dimensional MOFs, but also develops strategies for coordination mode regulation. The proposed two-dimensional MOFs catalyst design concept provides a new idea for improving the selectivity and stability of electrocatalytic carbon dioxide reduction.

The above research results were supported by the National Natural Science Foundation of China and Beijing Institute of Technology. Liu Yan, a doctoral student at the Advanced Institute of Multidisciplinary Science of BIT, is the first author, special associate researcher Li Pengfei and Professor Wang Bo are the co-corresponding authors, and BIT is the first correspondent institute.


Link to the paper:

https://onlinelibrary.wiley.com/doi/10.1002/anie.202105966