Asymmetrical Interactions between Ni Single Atomic Sites and Ni Clusters in a 3D Porous Organic Framework for Enhanced CO2 Photoreduction

• DOI: 10.1002/advs.202401508
• Publication Date: 2024-03-16T06:34:36Z
• Authors: Fang‐Qin Yan; Xiao‐Yu Dong; Yi‐Man Wang; Qian‐You Wang; Shan Wang; Shuang‐Quan Zang
• Keywords: Nanoclusters; Inert

Abstract 3D porous organic frameworks, which possess the advantages of high surface area and abundant exposed active sites, are considered ideal platforms to accommodate single atoms (SAs) metal nanoclusters (NCs) in high‐performance catalysts; however, very little research has been conducted this field. In present work, a framework containing Ni 1 SAs n NCs is prepared through metal‐assisted one‐pot polycondensation tetraaldehyde hexaaminotriptycene. The sites clusters confined space created favorable micro‐environment that facilitated activation chemically inert CO 2 molecules, thus promoting overall photoconversion efficiency selectivity reduction. 3D‐NiSAs/NiNCs‐POPs, as photoreduction catalyst, demonstrated an exceptional production rate 6.24 mmol g −1 h , 98%, excellent stability. theoretical calculations uncovered asymmetrical interaction between not only favored bending molecules reducing reduction energy, but also regulated electronic structure catalyst leading optimal binding strength intermediates.