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This work reports a metal–organic framework (MOF) with less‐coordinated copper dimers, which displays excellent electrochemical CO2 reduction (eCO2RR) performance with an advantageous current density of 0.9 A cm−2 and a high Faradaic efficiency of 71% to C2 products. In comparison with MOF with Cu monomers that are present as Cu1O4 with a coordination number of 3.8 ± 0.2, Cu dimers exist as O3Cu1...
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