2021
DOI: 10.1021/acscatal.1c00314
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Mechanically Constrained Catalytic Mn(CO)3Br Single Sites in a Two-Dimensional Covalent Organic Framework for CO2 Electroreduction in H2O

Abstract: The development of CO2 electroreduction (CO2RR) catalysts based on covalent organic frameworks (COFs) is an emerging strategy to produce synthetic fuels. However, our understanding on catalytic mechanisms and structure–activity relationships for COFs is still limited but essential to the rational design of these catalysts. Herein, we report a newly devised CO2 reduction catalyst by loading single-atom centers, {fac-Mn­(CO)3S}, (S = Br, CH3CN, H2O), within a bipyridyl-based COF (COFbpyMn ). COFbpyMn shows a lo… Show more

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Cited by 48 publications
(62 citation statements)
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“…In 2021, Lloret-Fillol et al prepared a Mn( i )-metalated COF as a CO 2 RR electrocatalyst by grafting Mn(CO) 5 Br on COF bpy via CO–bipyridine ligand exchange. 246 The COF bpyMn |NT composite, composed of COF bpyMn and multiwalled carbon nanotubes, exhibits higher CO 2 RR activity than the corresponding molecular electrocatalyst composite fac -Mn(2,2′-bipyridine)(CO) 3 Br|NT. In 0.5 M NaHCO 3 solution, the CO faradaic efficiency of COF bpyMn |NT was 62% under optimized conditions, while that of fac -Mn(2,2′-bipyridine)(CO) 3 Br|NT was only 13%, and the TOF of COF bpyMn |NT was 627 h −1 , which was 15.7 times higher than that of fac -Mn(2,2′-bipyridine)(CO) 3 Br|NT.…”
Section: Application Of Metalated Cofsmentioning
confidence: 99%
See 1 more Smart Citation
“…In 2021, Lloret-Fillol et al prepared a Mn( i )-metalated COF as a CO 2 RR electrocatalyst by grafting Mn(CO) 5 Br on COF bpy via CO–bipyridine ligand exchange. 246 The COF bpyMn |NT composite, composed of COF bpyMn and multiwalled carbon nanotubes, exhibits higher CO 2 RR activity than the corresponding molecular electrocatalyst composite fac -Mn(2,2′-bipyridine)(CO) 3 Br|NT. In 0.5 M NaHCO 3 solution, the CO faradaic efficiency of COF bpyMn |NT was 62% under optimized conditions, while that of fac -Mn(2,2′-bipyridine)(CO) 3 Br|NT was only 13%, and the TOF of COF bpyMn |NT was 627 h −1 , which was 15.7 times higher than that of fac -Mn(2,2′-bipyridine)(CO) 3 Br|NT.…”
Section: Application Of Metalated Cofsmentioning
confidence: 99%
“…Briefly, post-synthetic metalation is a general and versatile method for 2,2′-bipyridine-COF metalation that has been widely used for the synthesis of metalated 2,2′-bipyridine-COFs, as summarized in Table 2. 136,141,146,229–254…”
Section: Synthetic Strategy Of Metalated Cofsmentioning
confidence: 99%
“…In summary, the strategies for the synthesis of carbon-supported SACs can be classified into the four above-mentioned categories. The molecular skeleton encapsulation method is commonly used in specific mesoporous carbon materials (MOFs, 65 COFs, 66 HOFs, etc. ).…”
Section: Sacs For Simple C1 Productsmentioning
confidence: 99%
“…In addition to these, several other COFs for the highly efficient electrocatalytic CO 2 reduction to CO in recent years were also worth mentioning. These unique structures include a single Mn atom loaded on bipyridyl-based COFs (COF bpyMn ) via post-modification (Dubed Bandomo et al, 2021), a crown ether B18C6 embedded Co(TAPP)-COF (An et al, 2021), and a zwitterionic ultrathin cobalt tetraamino phthalocyaninesquaraine based COFs (COP-SA) (Song et al, 2021). All these ingenuous works guide the rational design of novel COF electrocatalysts for CO production from CO 2 .…”
Section: Co 2 Reduction To Comentioning
confidence: 99%