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  1. Free, publicly-accessible full text available July 1, 2023
  2. Atomically dispersed and nitrogen-coordinated single Ni sites ( i.e. , NiN x moieties) embedded in partially graphitized carbon have emerged as effective catalysts for CO 2 electroreduction to CO. However, much mystery remains behind the extrinsic and intrinsic factors that govern the overall catalytic CO 2 electrolysis performance. Here, we designed a high-performance single Ni site catalyst through elucidating the structural evolution of NiN x sites during thermal activation and other critical external factors ( e.g. , carbon particle sizes and Ni content) by using Ni–N–C model catalysts derived from nitrogen-doped carbon carbonized from a zeolitic imidazolate framework (ZIF)-8. The N coordination, metal–N bond length, and thermal wrinkling of carbon planes in Ni–N–C catalysts significantly depend on thermal temperatures. Density functional theory (DFT) calculations reveal that the shortening Ni–N bonds in compressively strained NiN 4 sites could intrinsically enhance the CO 2 RR activity and selectivity of the Ni–N–C catalyst. Notably, the NiN 3 active sites with optimal local structures formed at higher temperatures ( e.g. , 1200 °C) are intrinsically more active and CO selective than NiN 4 , providing a new opportunity to design a highly active catalyst via populating NiN 3 sites with increased density. We alsomore »studied how morphological factors such as the carbon host particle size and Ni loading alter the final catalyst structure and performance. The implementation of this catalyst in an industrial flow-cell electrolyzer demonstrated an impressive performance for CO generation, achieving a current density of CO up to 726 mA cm −2 with faradaic efficiency of CO above 90%, representing one of the best catalysts for CO 2 reduction to CO.« less
    Free, publicly-accessible full text available May 18, 2023
  3. Free, publicly-accessible full text available April 26, 2023
  4. Free, publicly-accessible full text available May 1, 2023
  5. The electrochemical CO 2 reduction reaction (CO 2 RR) to form highly valued chemicals is a sustainable solution to address the environmental issues caused by excessive CO 2 emissions. Generally, it is challenging to achieve high efficiency and selectivity simultaneously in the CO 2 RR due to multi-proton/electron transfer processes and complex reaction intermediates. Among the studied formulations, bimetallic catalysts have attracted significant attention with promising activity, selectivity, and stability. Engineering the atomic arrangement of bimetallic nanocatalysts is a promising strategy for the rational design of structures (intermetallic, core/shell, and phase-separated structures) to improve catalytic performance. This review summarizes the recent advances, challenges, and opportunities in developing bimetallic catalysts for the CO 2 RR. In particular, we firstly introduce the possible reaction pathways on bimetallic catalysts concerning the geometric and electronic properties of intermetallic, core/shell, and phase-separated structures at the atomic level. Then, we critically examine recent advances in crystalline structure engineering for bimetallic catalysts, aiming to establish the correlations between structures and catalytic properties. Finally, we provide a perspective on future research directions, emphasizing current challenges and opportunities.