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Ni single atoms supported on hierarchically porous carbonized wood with highly active Ni–N4 sites as a self-supported electrode for superior CO2 electroreduction
Nanoscale ( IF 5.8 ) Pub Date : 2022-06-24 , DOI: 10.1039/d2nr01992b
Huaiyu Chang 1, 2 , Hui Pan 1 , Fang Wang 1 , Zhengguo Zhang 1 , Yaming Kang 2 , Shixiong Min 1
Affiliation  

Powdery N-doped carbon-supported single-atom catalysts (SACs) can be prepared on a large scale and are highly selective in converting CO2 to CO, but their practical application is restricted by their powdery texture. Herein, we report Ni single atoms supported on hierarchically porous N-doped carbonized wood (Ni SAs-NCW) as a self-supported electrode for efficient and durable CO2 electroreduction. The porous NCW matrix possesses an abundance of open aligned microchannels that allow unimpeded CO2 diffusion and electrolyte transportation while the uniformly dispersed Ni SAs in the NCW matrix in the Ni–N4 configuration afford ample highly active sites for CO2 electroreduction. This Ni SAs-NCW electrode exhibits a high CO2-to-CO faradaic efficiency (FECO) of 92.1% and a CO partial current density (jCO) of 11.4 mA cm−2 at −0.46 V versus the reversible hydrogen electrode (RHE) and maintains a stable FECO and jCO over a period of 9 h of electrolysis. This work provides an effective strategy to develop efficient SACs with potential to be integrated into flow cell systems for large-scale CO2 reduction.

中文翻译:

Ni 单原子负载在具有高活性 Ni-N4 位点的分级多孔碳化木材上作为自支撑电极,可实现卓越的 CO2 电还原

粉状N掺杂碳负载单原子催化剂(SACs)可以大规模制备,并且在将CO 2转化为CO方面具有很高的选择性,但其实际应用受到粉状结构的限制。在此,我们报道了负载在分级多孔 N 掺杂碳化木材 (Ni SAs-NCW) 上的 Ni 单原子作为自支撑电极,用于高效和持久的 CO 2电还原。多孔 NCW 基质拥有大量开放排列的微通道,允许畅通无阻地 CO 2扩散和电解质传输,而均匀分散在 Ni-N 4配置的 NCW 基质中的 Ni SA为 CO 2提供了充足的高活性位点电还原。可逆氢电极相比,该 Ni SAs-NCW 电极表现出 92.1% 的高 CO 2到 CO 法拉第效率 (FE CO ) 和在 -0.46 V 时为 11.4 mA cm -2的 CO 分电流密度 ( j CO ) ( RHE) 并在 9 小时的电解时间内保持稳定的 FE COj CO 。这项工作为开发高效的 SAC 提供了一种有效的策略,该 SAC 具有集成到流通池系统中以实现大规模 CO 2减少的潜力。
更新日期:2022-06-24
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