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Enhanced CO2 electroreduction with metal-nitrogen-doped carbons in a continuous flow reactor
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2021-05-28 , DOI: 10.1016/j.jcou.2021.101583
Miguel Duarte , Nick Daems , Jonas Hereijgers , Daniel Arenas-Esteban , Sara Bals , Tom Breugelmans

As part of a mitigation and adaptation approach to increasing carbon dioxide atmospheric concentrations, we report superior performance of various metal-nitrogen-doped carbon catalysts, synthesized using an easily up-scalable method, for the electrochemical reduction to carbon monoxide and/or formate at industrially relevant current densities up to 200 mAcm−2. Altering the embedded transition metal (i.e. Sn, Co, Fe, Mn and Ni) allowed to tune the selectivity towards the desired product. Mn-N-C and Fe-N-C performance was compromised by its high CO* binding energy, while Co-N-C catalyzed preferentially the HER. Ni-N-C and Sn-N-C revealed to be promising electrocatalysts, the latter being evaluated for the first time in a flow reactor. A productivity of 589 L CO m-2 h-1 at -1.39 VRHE with Ni-N-C and 751 g HCOO- m-2 h-1 at -1.47 VRHE with Sn-N-C was achieved with no signs of degradation detected after 24 h of operation at industrially relevant current densities (100 mAcm−2). Stable operation at 200 mAcm−2 led to turnover frequencies for the production of carbon products of up to 5176 h-1. These enhanced productivities, in combination with high stability, constitute an essential step towards the scalability and ultimately towards the economical valorization of CO2 electrolyzers using metal-containing nitrogen-doped catalysts.



中文翻译:

在连续流反应器中用金属氮掺杂的碳增强的CO 2电还原

作为缓解和适应方法中增加二氧化碳大气浓度的一部分,我们报告了使用易于升级的方法合成的各种金属掺杂氮的碳催化剂的优异性能,可将其电化学还原为工业相关电流密度高达 200 mAcm -2。改变嵌入的过渡金属(即 Sn、Co、Fe、Mn 和 Ni)可以调整对所需产物的选择性。Mn-NC 和 Fe-NC 的性能受到其高 CO* 结合能的影响,而 Co-NC 优先催化 HER。Ni-NC 和 Sn-NC 显示出是有前途的电催化剂,后者首次在流动反应器中进行评估。589 L CO m -2 h -1 的生产力在 -1.39 V RHE 下使用 Ni-NC 和 751 g HCOO-m -2 h -1在 -1.47 V RHE 下使用 Sn-NC 实现了在工业相关电流密度 (100 mAcm -2 )。在 200 mAcm -2 下的稳定操作导致生产碳产品的周转频率高达 5176 h -1。这些提高的生产率与高稳定性相结合,构成了使用含金属氮掺杂催化剂的 CO 2电解槽的可扩展性和最终经济升值的重要步骤。

更新日期:2021-05-28
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