Intrinsic Carbon‐Defect‐Driven Electrocatalytic Reduction of Carbon Dioxide,Advanced Materials

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Intrinsic Carbon‐Defect‐Driven Electrocatalytic Reduction of Carbon Dioxide,Advanced Materials

2024-01-09 18:56| 来源: 网络整理| 查看: 265

Heteroatom‐doped carbon catalysts are currently attracting enormous attention due to their excellent performance for the electrocatalytic carbon dioxide reduction reaction (ECRR). However, the origin of the high catalytic activities of doped‐carbon materials remains obscure with the role of intrinsic carbon defects in promoting the ECRR receiving little attention despite the abundance of carbon defects in all carbon‐based catalytic materials. Herein, a positive correlation is reported between the ECRR performance of carbon‐based catalysts and the content of intrinsic carbon defects contained within these catalysts. Further, it is demonstrated that defective porous carbon catalysts containing no active heteroatom dopants also show excellent catalytic performance for ECRR. C K‐edge near edge X‐ray absorption fine structure measurements and density functional theory calculations reveal that sp2 defects (octagonal and pentagonal) rather than edge defects are key to the excellent ECRR activity of the defective porous carbon catalysts. This work thus makes an important contribution to the understanding of the origin of the ECRR activity of carbon‐based catalysts, with heteroatom doping perhaps being less important than previously envisaged for achieving a high ECRR performance.

中文翻译:

二氧化碳的固有碳缺陷驱动电催化还原

杂原子掺杂的碳催化剂由于其在电催化二氧化碳还原反应(ECRR)中的出色性能,目前引起了极大的关注。然而,尽管所有碳基催化材料中都存在大量碳缺陷,但掺杂碳材料具有高催化活性的起源仍然难以理解,固有的碳缺陷在促进ECRR中的作用鲜为人知。本文报道了碳基催化剂的ECRR性能与这些催化剂中所含固有碳缺陷含量之间的正相关关系。此外,证明了不含活性杂原子掺杂剂的有缺陷的多孔碳催化剂也表现出优异的ECRR催化性能。2个缺陷(八边形和五边形)而不是边缘缺陷是有缺陷的多孔碳催化剂优异ECRR活性的关键。因此,这项工作为理解碳基催化剂的ECRR活性起了重要的作用,杂原子掺杂可能不如以前所想的那样实现高ECRR性能。



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