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Catalysts 2020, 10, 1287 14 of 25 3.1.4. Cu MOF Additionally, Cu-based metal-organic porous materials like HKUST-1, CuAdeAce, CuDTA and CuZnDTA were also reported to electrocatalytically convert CO2 to ethanol with FEs of 6%, 1%, 3% and 4%, respectively [91]. These catalysts possessing a relatively high surface area, accessibility, and exposure of Cu active sites yield many opportunities for further performance improvements. 3.1.5. N-doped Carbon Materials Apart from Cu-based catalysts, metal-free nitrogen-doped carbon materials have been reported recently for electroredution of CO2 to ethanol, and delivered comparable catalytic activities to Cu-based catalysts while possessing better durability. The electronegative nitrogen heteroatoms introduced into the carbon matrixes can increase charge density and convert the inert carbon structures to be highly active. Recently, Ajayan et al. developed nitrogen-doped graphene quantum dots with nanometre-size facilitating the production of ethanol with a FE of 16% at –0.75 V vs. RHE in 1 M KOH [80]. By doping mesoporous carbon with nitrogen, our group has explored a metal-free cylindrical mesoporous nitrogen-doped carbon as a robust catalyst for CO2 electroreduction, enabling the efficient production of ethanol with an extremely high FE of 77% at −0.56 V vs. RHE in 0.1 M KHCO3 (Figure 7) [81]. The superior electrocatalytic performance was abscribed to the synergy of nitrogen heteratoms and highly uniform cylindrical channel structures that can dramatically boost C–C bond formation in CO2 electroreduction. Inspired by the potential of tuning the nanostructure of catalyst to acquire C2 compounds, we further design a class of hierarchical porous N-doped carbon with medium micropores embedded in the channel walls of N-doped ordered mesoporous carbon by a pore-structure-engineering strategy [82]. The embedded medium micropores can not only enrich the exposed active sites (pyridinic and pyrrolic N), but also induce desolvation to accumulate electrolyte ions and enable high local electric potential. Both of them facilitate the activation of CO2 molecules and the C–C coupling of key intermediates. Therefore, by scaling up the medium micropore content, the production rate of ethanol is increased to 2.3 mmol·gcat−1·h−1, which is one order of magnitude higher than that of the counterpart without medium microproes (0.2 mmol·gcat−1·h−1). The FE towards ethanol generation could be maintained at a high value of 78% at −0.56 V vs. RHE. In another exciting example, boron and nitrogen co-doped nanodimond was reported for selective reduction of CO2 to ethanol with a maximum FE of 93.2% at −1.0 V vs. RHE in 0.1 M NaHCO3 [83]. The synegic effect of boron and nitrogen codoping and fine balance between nitrogen content and H2 evolution potential drives the highly selective ethanol formation. These results open new insight into electrochemical conversion of CO2 to clean fuel ethanol.PDF Image | Advances in Clean Fuel Ethanol Production from CO2 Reduction
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