Tri(Thiophene‐Nitrile) Covalent Organic Frameworks With Low HOMO/LUMO Donor/Acceptor for High‐Potential‐Plateau Zinc Batteries

ABSTRACT Covalent organic frameworks (COFs) featuring desirable redox‐active sites have become competitive cathode materials for aqueous zinc‐organic batteries (ZOBs). However, multi‐active COFs, albeit with high capacity, are often confined to their sloping and low redox potential (<0.8 V) caused by high molecular orbital energy levels (HOMO/LUMO) of active moieties. Here we report a capacity‐voltage trade‐off‐breaking design of COFs by pairing low‐HOMO trithiophene donor (−6.04 eV) with low‐LUMO trinitrile acceptor (−3.82 eV) via robust olefin linkages (TN‐COF), using high‐LUMO triazine acceptor (−1.75 eV) as the counterpart (TA‐COF). The tri(thiophene‐nitrile) donor‐acceptor enables low HOMO/LUMO energy…

• NN
  National Natural Science Foundation of China

  Awards: 22172111, 22272118, 22309134
• SR
  Shanghai Rising-Star Program

  Award: 23YF1449200
• FR
  Fundamental Research Funds for the Central Universities