Proton feeding from defect-rich carbon support to cobalt phthalocyanine for efficient CO2 electroreduction

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-07-01 DOI:10.1016/S1872-2067(24)60061-6
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Abstract

Electrocatalytic CO2 reduction reaction (CO2RR) holds significant promise for sustainable energy conversion, with cobalt phthalocyanine (CoPc) emerging as a notable catalyst due to its high CO selectivity. However, CoPc's efficacy is hindered by its limited ability to provide sufficient proton for the protonation process, particularly at industrial current densities. Herein, we introduce defect-engineered carbon nanotubes (d-CNT) to augment proton feeding for CO2RR over CoPc, achieved by expediting water dissociation. Our kinetic measurements and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy reveal d-CNT significantly enhances proton feeding, thereby facilitating CO2 activation to *COOH in CoPc. Density functional theory calculations corroborate these findings, illustrating that d-CNT decreases the barrier to water dissociation. Consequently, the CoPc/d-CNT mixture demonstrates robust performance, achieving 500 mA cm–2 for CO2RR with CO selectivity exceeding 96%. Notably, CoPc/d-CNT remains stability for a duration of 20 h under a substantial current density of 150 mA cm–2. The study broadens the scope of practical applications for molecular catalysts in CO2RR, marking a significant step towards sustainable energy conversion.

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从富含缺陷的碳支持物向酞菁钴提供质子,实现高效的二氧化碳电还原
电催化二氧化碳还原反应(CO2RR)在可持续能源转换方面大有可为,其中酞菁钴(CoPc)因其高二氧化碳选择性而成为一种引人注目的催化剂。然而,CoPc 为质子化过程提供足够质子的能力有限,这阻碍了它的功效,尤其是在工业电流密度下。在此,我们引入了缺陷工程碳纳米管(d-CNT),通过加速水的解离来增加 CO2RR 对 CoPc 的质子供给。我们的动力学测量和原位衰减全反射表面增强红外吸收光谱显示,d-CNT 能显著增强质子馈入,从而促进 CO2 在 CoPc 中活化为 *COOH。密度泛函理论计算证实了这些发现,说明 d-CNT 降低了水解离的障碍。因此,CoPc/d-CNT 混合物表现出强劲的性能,CO2RR 达到 500 mA cm-2,CO 选择性超过 96%。值得注意的是,在 150 mA cm-2 的大电流密度下,CoPc/d-CNT 可在 20 小时内保持稳定。这项研究拓宽了分子催化剂在 CO2RR 中的实际应用范围,标志着向可持续能源转换迈出了重要一步。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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