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Enhancing the p‐orbital delocalization of a Bi catalyst (termed as POD‐Bi) via layer coupling of the short inter‐layer Bi−Bi bond facilitates the adsorption of intermediate *OCHO of CO2 and thus boosts the CO2 reduction reaction (CO2RR) rate to formate. X‐ray absorption fine spectroscopy shows that the POD‐Bi catalyst has a shortened inter‐layer bond after the catalysts are electrochemically reduced...
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