<p>Hybrid systems that integrate electrochemical CO<sub>2</sub> reduction with microbial upgrading offer a viable route to high value organic compounds from CO<sub>2</sub> at ambient conditions. However, electrocatalyst deactivation in microbial growth media remains a key barrier, limiting efficiency and increasing cost. Here we show that a bioadaptive single-atom nickel catalyst (Ni SAC), coupled with genetically engineered <i>Clostridium ljungdahlii</i>, enables robust electrosynthesis of isopropanol (IPA) from CO<sub>2</sub> via a CO-mediated pathway. Instead of relying on H<sub>2</sub> as an electron carrier, the system applies high-rate CO formation in complex growth media, maintaining a tunable CO Faradaic efficiency up to 92%, which is 9.4 to 52.7 times greater than conventional Ag catalysts. This performance supports stable IPA production at current density of 10.8 A/m<sup>2</sup> and production rate of 161.3 mg/L/day. In situ Raman and X-ray absorption spectroscopy, together with theoretical calculations, indicate that the Ni SAC can resist competing organic adsorption and retain its coordination structure during CO<sub>2</sub> reduction in bioelectrolytes, providing a mechanistic basis for the catalyst stability and integrated process performance.</p>

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Bioadaptive Ni single atoms unlock high rate microbial electrosynthesis of isopropanol from CO2

  • Guangye Zhou,
  • Jonathan R. Humphreys,
  • Dongfang Cheng,
  • Shan Jiang,
  • Wei-Ling Huang,
  • Guangming Cheng,
  • Nan Yao,
  • Wei Xiong,
  • Jeffrey T. Miller,
  • Katherine Chou,
  • Johannes B. M. Klok,
  • Hongxu Chen,
  • James Christopher Dykstra,
  • Zhiyong Jason Ren

摘要

Hybrid systems that integrate electrochemical CO2 reduction with microbial upgrading offer a viable route to high value organic compounds from CO2 at ambient conditions. However, electrocatalyst deactivation in microbial growth media remains a key barrier, limiting efficiency and increasing cost. Here we show that a bioadaptive single-atom nickel catalyst (Ni SAC), coupled with genetically engineered Clostridium ljungdahlii, enables robust electrosynthesis of isopropanol (IPA) from CO2 via a CO-mediated pathway. Instead of relying on H2 as an electron carrier, the system applies high-rate CO formation in complex growth media, maintaining a tunable CO Faradaic efficiency up to 92%, which is 9.4 to 52.7 times greater than conventional Ag catalysts. This performance supports stable IPA production at current density of 10.8 A/m2 and production rate of 161.3 mg/L/day. In situ Raman and X-ray absorption spectroscopy, together with theoretical calculations, indicate that the Ni SAC can resist competing organic adsorption and retain its coordination structure during CO2 reduction in bioelectrolytes, providing a mechanistic basis for the catalyst stability and integrated process performance.