4.8 Article

High Yield of CO and Synchronous S Recovery from the Conversion of CO2 and H2S in Natural Gas Based on a Novel Electrochemical Reactor

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 55, Issue 21, Pages 14854-14862

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.est.1c04414

Keywords

H2S splitting; CO2 conversion; natural gas purification; synchronous recovery of S and CO

Funding

  1. National Key Research and Development Program of China [2018YFE0122300]
  2. National Natural Science Foundation of China [22076121]
  3. SJTU-AEMD

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This study proposes a method to convert H2S and CO2 into CO and S simultaneously using an electrochemical reactor, achieving high efficiency and yield. Through special designs in the anodic and cathodic chambers, the synchronized utilization of H2S and CO2 is successfully realized.
H2S and CO2 are the main impurities in raw natural gas, which needs to be purified before use. However, the comprehensive utilization of H2S and CO2 has been ignored. Herein, we proposed a fully resource-based method to convert toxic gas H2S and greenhouse gas CO2 synchronously into CO and elemental S by using a novel electrochemical reactor. The special designs include that, in the anodic chamber, H2S was oxidized rapidly to S based on the I-/I-3(-) cyclic redox system to avoid anode passivation. On the other hand, in the cathodic chamber, CO2 was rapidly and selectively reduced to CO based on a porous carbon gas diffusion electrode (GDE) modified with polytetrafluoroethylene and cobalt phthalocyanine (CoPc). A high Faraday efficiency (>95%) toward CO was achieved due to the enhanced mass transfer of CO2 on the GDE and the presence of the selective CoPc catalyst. The maximum energy efficiency of the system was more than 72.41% with a current density of over 50 mA/cm(2), which was 12.5 times higher than what was previously reported on the H2S treatment system. The yields of S and CO were 24.94 mg.cm(-2).h(-1) and 19.93 mL.cm(-2).h(-1), respectively. A model analysis determined that the operation cost of the synchronous utilization of H2S and CO2 method was slightly lower than that of the single utilization of H2S in the existing natural gas purification technology. Overall, this paper provides efficient and simultaneous conversion of H2S and CO2 into S and CO.

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