The progress of high-efficiency electrocatalysis of CO2 by a single-atom catalyst in Fujian Institute of Industrial Structure

In recent years, due to the massive use of traditional energy sources, the concentration of CO2 in the atmosphere has increased sharply, leading to problems such as the greenhouse effect and the deterioration of the environmental climate. Therefore, measures need to be taken to reduce the concentration of CO2. Turning CO2 into usable chemicals is a way to turn waste into treasure. The use of electricity generated by sustainable energy for electrocatalytic CO2 conversion has the advantages of mildness and environmental protection. However, there are still shortcomings such as low selectivity, high overpotential, and low current density that need to be overcome, so finding a suitable catalyst is the key.

Monoatomic catalysts have the highest atomic utilization rate, and exhibit high activity and selectivity in many catalytic reactions. However, the activity of different monoatomic metal catalysts is different, and the reason remains to be clarified. Recently, the team of Cao Rong and Huang Yuanbiao, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, with the support of the Key R & D Program of the Ministry of Science and Technology, the Fund Committee, the Pioneer and Frontier Program Project of the Chinese Academy of Sciences, and the Excellent Member Program of the Youth Promotion Association of the Chinese Academy of Sciences, adopted the previous The team prepared a single-atom stable porous porphyrin triazine framework material (ACS Energy Lett., 2018, 3, 883-889; J. Mater. Chem. A, 2019, 7, 1252), and prepared the carrier stable Ni, Cu, Fe and Co series of single-atom catalysts, and systematically studied their electrocatalytic reduction of carbon dioxide. Compared with other metal single-atom catalysts, the prepared Ni single-atom catalysts have a far-reaching efficiency of CO production of more than 90% in a wider voltage test range (-0.6 — -1.2 V vs. RHE), and in- The selectivity is close to 100% (98%) at 0.8 V, and its TOF value is as high as 13462 h-1 at -1.2 V. The calculation shows that the electrochemical potential of Ni and Fe catalysts is smaller than that of Co and Cu catalysts, so the Ni and Fe catalysts exhibit higher activity; while the energy barrier of Ni catalysts for HER is higher than that of CO2RR, so the hydrogen Generated, while the Fe catalyst has a higher energy barrier for desorbing CO, so the Ni catalyst exhibits a high CO2RR capability. This work provides new ideas for the design and synthesis of highly efficient single-atom non-noble metal catalysts, and provides an important reference for the development of new high-efficiency electrocatalysts. The relevant research results were published in CCS Chem., 2019, 1, 384–395, the flagship journal of the Chinese Chemical Society.

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