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聚乙烯亚胺增强的 Sn/Cu 泡沫树枝状自支撑催化阴极用于 CO 还原为 HCOOH。

Polyethyleneimine-reinforced Sn/Cu foam dendritic self-supporting catalytic cathode for CO reduction to HCOOH.

机构信息

College of Environmental Science and Engineering, Beijing Forestry University, Beijing, 100083, PR China.

College of Water Sciences, Beijing Normal University, Beijing, 100875, PR China.

出版信息

Chemosphere. 2022 Aug;301:134704. doi: 10.1016/j.chemosphere.2022.134704. Epub 2022 Apr 26.

Abstract

In this work, a novel catalytic cathode of polyethyleneimine (PEI)-Sn/Cu foam with dendritic structure was prepared by electrodeposition and impregnation. It was used in the electrocatalytic reduction of CO to HCOOH, and its performance in this process was evaluated. At -0.97 V vs. RHE, the faradaic efficiency and current density reached 92.3% and 57.1 mA cm, respectively, in a 0.5 M KHCO electrolyte. The HCOOH production rate reached 890.4 μmol h cm, which exceeds those for most reported Sn catalysts. Density functional theory calculations showed that use of Sn/Cu foam is more conducive to HCOOH formation than use of Cu or Sn alone, and *OCHO is the main intermediate in HCOOH formation. The results of OH adsorption experiments confirmed that the introduction of PEI enhanced the catalytic capacity of the Sn/Cu foam, stabilized CO· intermediates, and promoted HCOOH generation. These results will provide an attractive strategy for developing efficient catalysts with excellent activities and stabilities for CO electroreduction.

摘要

在这项工作中,通过电沉积和浸渍法制备了具有树枝状结构的新型聚乙烯亚胺(PEI)-Sn/Cu 泡沫催化阴极。它被用于 CO 电化学催化还原为 HCOOH,并评估了其在该过程中的性能。在 0.5 M KHCO3 电解质中,-0.97 V 对 RHE 的条件下,法拉第效率和电流密度分别达到 92.3%和 57.1 mA cm-2。HCOOH 的生成速率达到 890.4 μmol h cm-2,超过了大多数报道的 Sn 催化剂。密度泛函理论计算表明,与单独使用 Cu 或 Sn 相比,使用 Sn/Cu 泡沫更有利于 HCOOH 的形成,并且*OCHO 是 HCOOH 形成的主要中间产物。OH 吸附实验的结果证实,PEI 的引入增强了 Sn/Cu 泡沫的催化能力,稳定了 CO·中间体,并促进了 HCOOH 的生成。这些结果将为开发具有优异活性和稳定性的 CO 电催化还原高效催化剂提供有吸引力的策略。

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