Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO2 Electroreduction into CO.,ChemPhysChem

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Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO2 Electroreduction into CO.
ChemPhysChem ( IF 2.3 ) Pub Date : 2020-07-28 , DOI: 10.1002/cphc.202000576
Yongzhi Zhong ₁ , Xiangdong Kong ₂ , Zhigang Geng ₂ , Jie Zeng ₂ , Xuan Luo ₁ , Lin Zhang ₁

Affiliation

Electroreduction of CO₂ into carbonaceous fuels or industrial chemicals using renewable energy sources is an ideal way to promote global carbon recycling. Thus, it is of great importance to develop highly selective, efficient, and stable catalysts. Herein, we prepared cobalt single atoms (Co SAs) coordinated with phthalocyanine (Co SAs‐Pc). The anchoring of phthalocyanine with Co sites enabled electron transfer from Co sites to CO₂ effectively via the π‐conjugated system, resulting in high catalytic performance of CO₂ electroreduction into CO. During the process of CO₂ electroreduction, the Faradaic efficiency (FE) of Co SAs‐Pc for CO was as high as 94.8 %. Meanwhile, the partial current density of Co SAs‐Pc for CO was −11.3 mA cm⁻² at −0.8 V versus the reversible hydrogen electrode (vs RHE), 18.83 and 2.86 times greater than those of Co SAs (−0.60 mA cm⁻²) and commercial Co phthalocyanine (−3.95 mA cm⁻²), respectively. In an H‐cell system operating at −0.8 V vs RHE over 10 h, the current density and FE for CO of Co SAs‐Pc dropped by 3.2 % and 2.5 %. A mechanistic study revealed that the promoted catalytic performance of Co SAs‐Pc could be attributed to the accelerated reaction kinetics and facilitated CO₂ activation.

中文翻译：

单个钴位点的分子修饰可提高将CO2电还原为CO的催化活性。

使用可再生能源将CO ₂电还原为碳质燃料或工业化学品是促进全球碳循环的理想方法。因此，开发高度选择性，有效和稳定的催化剂非常重要。在此，我们制备了与酞菁（Co SAs-Pc）配位的钴单原子（Co SAs）。用Co酞菁位点的锚定启用从Co位点以CO的电子转移₂有效地通过上述π共轭体系，从而导致CO的高催化性能₂电解还原成CO。在CO的过程₂电还原时，Co SAs-Pc对CO的法拉第效率（FE）高达94.8％。同时，共同SAS-Pc的对CO的分电流密度为-11.3毫安厘米^-2在-0.8 V相对于可逆氢电极（VS RHE），18.83和比钴的SA（-0.60毫安厘米的大2.86倍^{- 2}）和市售Co酞菁（-3.95 mA cm ^-2）。在H电池系统中，相对于RHE在−0.8 V电压下运行10小时，Co SAs-Pc的电流密度和CO的FE分别下降了3.2％和2.5％。一项机理研究表明，Co SAs-Pc催化性能的提高可能归因于反应动力学的加快和CO _2的活化。

更新日期：2020-09-15

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