Promoting CO<sub>2</sub>Dynamic Activation via Micro‐Engineering Technology for Enhancing Electrochemical CO<sub>2</sub>Reduction
Shanhe Gong, Shaokang Yang, Wenbo Wang, Runqing Lu, Haotan Wang, Han Xu, Guilong Wang, Jimin Xie, Dewei Rao, Chundu Wu, Jun Liu, Shouyan Shao, Xiaomeng Lv
Abstract
Abstract Optimizing the coordination structure and microscopic reaction environment of isolated metal sites is promising for boosting catalytic activity for electrocatalytic CO 2 reduction reaction (CO 2 RR) but is still challenging to achieve. Herein, a newly electrostatic induced self‐assembly strategy for encapsulating isolated Ni‐C 3 N 1 moiety into hollow nano‐reactor as I‐Ni SA/NHCRs is developed, which achieves FE CO of 94.91% at −0.80 V, the CO partial current density of ≈−15.35 mA cm −2 , superior to that with outer Ni‐C 2 N 2 moiety (94.47%, ≈−12.06 mA cm −2 ), or without hollow structure (92.30%, ≈−5.39 mA cm −2 ), and high FE CO of ≈98.41% at 100 mA cm −2 in flow cell. COMSOL multiphysics finite‐element method and density functional theory (DFT) calculation illustrate that the excellent activity for I‐Ni SA/NHCRs should be attributed to the structure‐enhanced kinetics process caused by its hollow nano‐reactor structure and unique Ni‐C 3 N 1 moiety, which can enrich electron on Ni sites and positively shift d‐band center to the Fermi level to accelerate the adsorption and activation of CO 2 molecule and *COOH formation. Meanwhile, this strategy also successfully steers the design of encapsulating isolated iron and cobalt sites into nano‐reactor, while I‐Ni SA/NHCRs‐based zinc‐CO 2 battery assembled with a peak power density of 2.54 mW cm− −2 is achieved.