2.6% cm–2 Single-Pass CO2-to-CO Conversion Using Ni Single Atoms Supported on Ultra-Thin Carbon Nanosheets in a Flow Electrolyzer,ACS Catalysis

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2.6% cm–2 Single-Pass CO2-to-CO Conversion Using Ni Single Atoms Supported on Ultra-Thin Carbon Nanosheets in a Flow Electrolyzer
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-10-03 , DOI: 10.1021/acscatal.1c03231
Yang Zhang _{1,

2} , Kun Qi ₂ , Ji Li ₃ , Bonito A. Karamoko ₂ , Luc Lajaunie ₄ , Franck Godiard ₅ , Erwan Oliviero ₅ , Xiaoqiang Cui ₆ , Ying Wang ₆ , Yupeng Zhang ₁ , Huali Wu ₂ , Wensen Wang ₂ , Damien Voiry ₂

Affiliation

The CO₂ reduction reaction (CO₂RR) using a renewable energy source is a promising strategy for its utilization. Such a technology, however, requires the development of catalysts with optimized activity and selectivity that can be integrated into the device architectures. Flow electrolyzers have recently been proposed for facilitating the electrochemical CO₂RR thanks to their unique ability to perform electroreduction at high reaction rates via the creation of the three-phase interface. While some examples of flow electrolyzers for the conversion of CO₂ have recently been reported, the influence of the CO₂ and electrolyte streams on the overall catalytic mechanism remained ambiguous. Here, we synthesized single-atom nickel on two-dimensional nitrogen-doped carbon nanosheets (SA Ni-NC) for the CO₂-to-CO conversion. Taking advantage of this model catalyst, we explored the correlation between the applied potential and the feeds in both electrolyte and CO₂, on the one hand, and the performance metrics, on the other hand. By regulating the feed stream’s conditions, the SA Ni-NC achieves energy efficiencies as high as 85% at j_CO = 7.2 mA cm^–2 and 56% at j_CO = 170 mA cm^–2, whereas the single-pass CO₂-to-CO conversion efficiency (SPCC) reaches 2.6% cm^–2. We finally demonstrated the scalability of the flow electrolyzers by stacking three 1 cm2 reactors and reached a record-high CO yield rate of 31.5 L min^–1 m^–2 with near-unity CO selectivity and an SPCC of 8.9% from three.

中文翻译：

2.6% cm-2 单程 CO2 到 CO 的转化，在流动电解槽中使用支持在超薄碳纳米片上的 Ni 单原子

使用可再生能源的 CO ₂还原反应 (CO ₂ RR) 是一种很有前景的利用策略。然而，这种技术需要开发具有优化活性和选择性的催化剂，这些催化剂可以集成到设备架构中。流动电解槽最近被提议用于促进电化学 CO ₂ RR，这要归功于它们通过创建三相界面以高反应速率进行电还原的独特能力。虽然最近报道了一些用于转化 CO ₂的流动电解槽的例子，但 CO ₂和电解质流对整体催化机制仍然不明确。在这里，我们在二维氮掺杂碳纳米片 (SA Ni-NC) 上合成了单原子镍，用于 CO ₂到 CO 的转化。利用该模型催化剂，我们一方面探索了施加的电位与电解质和 CO _{2 中}的进料之间的相关性，另一方面探索了性能指标之间的相关性。通过调节进料流的条件，SA Ni-NC 在j _CO = 7.2 mA cm ^{–2 时}实现高达 85% 的能效，在j _CO = 170 mA cm ^{–2 时}实现高达56% 的能效，而单程 CO ₂一氧化碳转化效率 (SPCC) 达到 2.6% cm ^–2。我们最终通过堆叠三个 1 cm2 反应器证明了流动电解槽的可扩展性，并达到了创纪录的 31.5 L min ^–1 m ^{–2 的}CO 产率，CO 选择性接近统一，三个反应器的 SPCC 为 8.9%。

更新日期：2021-10-15

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