Divergent Paths, Same Goal: A Pair‐Electrosynthesis Tactic for Cost‐Efficient and Exclusive Formate Production by Metal–Organic‐Framework‐Derived 2D Electrocatalysts. Issue 25 (14th May 2021)

• Record Type: Journal Article
• Authors: Cao, Changsheng; Ma, Dong‐Dong; Jia, Jingchun; Xu, Qiang; Wu, Xin‐Tao; Zhu, Qi‐Long
• Is Part Of: Advanced materials. Volume 33:Issue 25(2021)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-05-14
• Subjects: CO 2 reduction reaction -- formic acid -- metal–organic frameworks -- methanol oxidation reaction -- pair‐electrosynthesis; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adma.202008631
• Languages: English
• ISSNs: 0935-9648

Abstract

Abstract: Electrosynthesis of formic acid/formate is a promising alternative protocol to industrial processes. Herein, a pioneering pair‐electrosynthesis tactic is reported for exclusively producing formate via coupling selectively electrocatalytic methanol oxidation reaction (MOR) and CO2 reduction reaction (CO2 RR), in which the electrode derived from Ni‐based metal–organic framework (Ni‐MOF) nanosheet arrays (Ni‐NF‐Af), as well as the Bi‐MOF‐derived ultrathin bismuthenes (Bi‐enes), both obtained through an in situ electrochemical conversion process, are used as efficient anodic and cathodic electrocatalysts, respectively, achieving concurrent yielding of the same high‐value product at both electrodes with greatly reduced energy input. The as‐prepared Ni‐NF‐Af only needs quite low potentials to reach large current densities (e.g., 100 mA cm −2 @1.345 V) with ≈100% selectivity for anodic methanol‐to‐formate conversion. Meanwhile, for CO2 RR in the cathode, the as‐prepared Bi‐enes can simultaneously exhibit near‐unity selectivity, large current densities, and good stability in a wide potential window toward formate production. Consequently, the coupled MOR//CO2 RR system based on the distinctive MOF‐derived catalysts displays excellent performance for pair‐electrosynthesis of formate, delivering high current densities and nearly 100% selectivity for formate production in both the anode and the cathode. This work provides a novel way to design advanced MOF‐derived electrocatalysts and innovative electrolytic systems for electrochemical production of value‐added feedstocks. Abstract : A pair‐electrosynthesis tactic for concurrent formate production is pioneeringly developed by coupling electrocatalytic methanol oxidation and CO2 reduction reactions, which can achieve highly efficient and selective value‐added synthesis in both electrodes with lower energy consumption, using in situ metal–organic‐framework‐derived high‐performance 2D electrocatalysts.