通过六次甲基四胺 (HMTA) 与MOF孔道中的金属位点 (M-TCP

The coordination of hexamethylenetetramine (HMTA) with the metal sites (M-TCPP) in the MOF channel greatly increases the CO2 adsorption performance and catalytic selectivity of MOF, and the introduction of N sites makes MOF CO2 adsorption The enthalpy has been doubled and the catalytic selectivity has been nearly tripled. The experimental results show that the FECO of the composite is close to 100% at -0.7 V. The material also exhibits excellent photoelectric coupling catalytic performance. Under light irradiation, the CO2RR electrocatalytic selectivity reaches over 90% in a wide voltage range, and the energy utilization efficiency and CO production rate are greatly improved. Theoretical calculations show that the addition of multi-site Lewis bases reduces the adsorption capacity of active sites for intermediates and the energy barrier of the rate-determining step in the CO2→CO conversion process; thus, the CO2 electrocatalytic reduction performance is improved by loading HMTA.

The coordination of hexamethylenetetramine (HMTA) with the metal site (M-TCPP) in the MOF pore greatly enhances the adsorption performance and catalytic selectivity of MOF for CO2. The introduction of the N site increases the adsorption enthalpy of MOF for CO2 by two times, and the catalytic selectivity by nearly two times. The experimental results indicate that the FECO of the composite material is close to 100% at -0.7 V. This material also exhibits excellent optoelectronic coupling catalytic performance. Under illumination, the CO2RR electrocatalytic selectivity reaches over 90% over a wide voltage range, greatly improving energy utilization efficiency and CO production rate. Theoretical calculations show that the addition of multi site Lewis bases reduces the adsorption capacity of active site on intermediates and the energy barrier of the decisive step in the CO2 → CO conversion process; Therefore, improving the CO2 electrocatalytic reduction performance by loading HMTA.

The coordination of hexamethylenetetramine (HMTA) with the metal site (M-TCPP) in MOF pores greatly increased the adsorption performance and catalytic selectivity of MOF for CO2, and the introduction of N site increased the adsorption enthalpy and catalytic selectivity of MOF for CO2 by two times. The experimental results show that the FECO of the composite is close to 100% at-0.7 V. The material also showed excellent photoelectric coupling catalytic performance. Under illumination, the electrocatalytic selectivity of CO2RR reached more than 90% in a wide voltage range, and the energy utilization efficiency and the rate of CO production were greatly improved. Theoretical calculation shows that the addition of multi-site Lewis base reduces the adsorption capacity of active sites to intermediates and the energy barrier of the decisive step in the process of CO2→CO conversion. Therefore, the electrocatalytic reduction performance of CO2 is improved by loading HMTA.