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Creators/Authors contains: "Mohd Adli, Nadia"

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  1. null (Ed.)
  2. Abstract Atomically dispersed FeN4active sites have exhibited exceptional catalytic activity and selectivity for the electrochemical CO2reduction reaction (CO2RR) to CO. However, the understanding behind the intrinsic and morphological factors contributing to the catalytic properties of FeN4sites is still lacking. By using a Fe‐N‐C model catalyst derived from the ZIF‐8, we deconvoluted three key morphological and structural elements of FeN4sites, including particle sizes of catalysts, Fe content, and Fe−N bond structures. Their respective impacts on the CO2RR were comprehensively elucidated. Engineering the particle size and Fe doping is critical to control extrinsic morphological factors of FeN4sites for optimal porosity, electrochemically active surface areas, and the graphitization of the carbon support. In contrast, the intrinsic activity of FeN4sites was only tunable by varying thermal activation temperatures during the formation of FeN4sites, which impacted the length of the Fe−N bonds and the local strains. The structural evolution of Fe−N bonds was examined at the atomic level. First‐principles calculations further elucidated the origin of intrinsic activity improvement associated with the optimal local strain of the Fe−N bond. 
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