Abstract

AbstractQuinone‐based aqueous redox flow batteries (RFBs) have drawn much attention due to their high safety, two‐electron involvement, rapid reaction kinetics, property tunability, and potentially low cost. RFBs operating in neutral solution feature a wide electrochemical window of around 2.5 V, which provides much more space for the design of redox‐active materials (RAMs) to realize a high voltage. However, it is still challenging to achieve low potential in the neutral condition for quinone‐based RAMs, owing to inherently pH‐dependent behaviors and deep LUMO (the lowest unoccupied molecular orbital) energy level. Herein, we report three low‐potential quinone‐based RAMs (1,4‐BDPAQCl2, 1,5‐BDPAQCl2, and 1,8‐BDPAQCl2) by bis‐dimethylamino substitution. The half‐wave potential of the quinones in 0.5 M KCl is approximately −0.55 to −0.57 V versus a normal hydrogen electrode. The low potential is ascribed to the introduced functional groups with two effects. First, the intramolecular hydrogen bonds formed between C=O and H−N can weaken the association between protons and dianion Q2−, resulting in a favorable distribution of products. Second, the functional groups can effectively increase the LUMO over 0.22 eV, compared with anthraquinone. Paired with Fe(glycine)2Cl2, the theoretical open‐circuit voltage of full RFBs is achieved at 1.27–1.29 V. We test full batteries using these quinones as negative RAMs at a lower concentration (0.1 M). The results show that 1,8‐BDPAQCl2 displays stability during 300 charge‐discharge cycles. In contrast, the other two quinones exhibit poor cycling stability due to side reactions. We further execute a higher concentration (0.4 M) for 1,8‐BDPAQCl2. The cycling stability of the quinone−iron RFBs is outstanding, with 0.048 % capacity decay per cycle and 0.88 % capacity decay per day. Our finding offers a feasible strategy to design low‐potential quinone molecules for the neutral RFBs.

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