Login / Signup

Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites.

Le LiAdnan OzdenShuyi GuoF Pelayo García de ArquerChuanhao WangMingzhe ZhangJin ZhangHaoyang JiangWei WangHao DongDavid SintonEdward H SargentMiao Zhong
Published in: Nature communications (2021)
Electrochemical reduction of CO2 (CO2R) to formic acid upgrades waste CO2; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO2R operation. Active Sn-Bi/SnO2 surfaces formed in situ on homogeneously alloyed Bi0.1Sn crystals stabilize the CO2R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm-2. This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ -0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO- solution (3.4 molar, 15 wt%) over 100 h.
Keyphrases
  • high resolution
  • heavy metals
  • escherichia coli
  • staphylococcus aureus
  • climate change
  • risk assessment
  • biofilm formation
  • human health
  • dna binding
  • sewage sludge
  • label free