Microwave‐Assisted Rapid Synthesis of MOF‐Based Single‐Atom Ni Catalyst for CO2 Electroreduction at Ampere‐Level Current

• Published in: Angewandte Chemie International Edition 2024-03, Vol.63 (10), p.e202318338-n/a
• Main Authors: Wen, Ming, Sun, Nana, Jiao, Long, Zang, Shuang‐Quan, Jiang, Hai‐Long
• Format: Article
• Language: English
• Subjects: Carbon; Carbon dioxide; Catalysis; Catalysts; CO2 reduction; Electric heating; electrocatalysis; Electrowinning; Mass transfer; Metal-organic frameworks; microwave; Porosity; Pyrolysis; Rare gases; Single-atom catalysts; Synthesis
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202318338

Carbon‐based single‐atom catalysts (SACs) have attracted tremendous interest in heterogeneous catalysis. However, the common electric heating techniques to produce carbon‐based SACs usually suffer from prolonged heating time and tedious operations. Herein, a general and facile microwave‐assisted rapid pyrolysis method is developed to afford carbon‐based SACs within 3 min without inert gas protection. The obtained carbon‐based SACs present high porosity and comparable carbonization degree to those obtained by electric heating techniques. Specifically, the single‐atom Ni implanted N‐doped carbon (Ni1−N−C) derived from a Ni‐doped metal–organic framework (Ni‐ZIF‐8) exhibits remarkable CO Faradaic efficiency (96 %) with a substantial CO partial current density (jCO) up to 1.06 A/cm2 in CO2 electroreduction, far superior to the counterpart obtained by traditional pyrolysis with electric heating. Mechanism investigations reveal that the resulting Ni1−N−C presents abundant defective sites and mesoporous structure, greatly facilitating CO2 adsorption and mass transfer. This work establishes a versatile approach to rapid and large‐scale synthesis of SACs as well as other carbon‐based materials for efficient catalysis. A general and facile microwave‐assisted rapid pyrolysis method is developed to afford carbon‐based single‐atom catalysts within 3 min. Specifically, the optimized single‐atom Ni implanted N‐doped carbon materials (Ni1−N−C) based on a metal–organic framework precursor showcases a tremendous CO partial current density of 1.06 A cm−2 with a CO Faradaic efficiency up to 96 % in electrocatalytic CO2 reduction.