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Potassium-Assisted Fabrication of Intrinsic Defects in Porous Carbons for Electrocatalytic CO2 Reduction
Advanced Materials ( IF 29.4 ) Pub Date : 2022-08-10 , DOI: 10.1002/adma.202205933
Li-Li Ling 1 , Long Jiao 1 , Xiaoshuo Liu 2, 3 , Yun Dong 4 , Weijie Yang 2 , Hongjun Zhang 4 , Bangjiao Ye 4 , Jun Chen 5 , Hai-Long Jiang 1
Affiliation  

The fabrication of intrinsic carbon defects is usually tangled with doping effects, and the identification of their unique roles in catalysis remains a tough task. Herein, a K+-assisted synthetic strategy is developed to afford porous carbon (K-defect-C) with abundant intrinsic defects and complete elimination of heteroatom via direct pyrolysis of K+-confined metal–organic frameworks (MOFs). Positron-annihilation lifetime spectroscopy, X-ray absorption fine structure measurement, and scanning transmission electron microscopy jointly illustrate the existence of abundant 12-vacancy-type carbon defects (V12) in K-defect-C. Remarkably, the K-defect-C achieves ultrahigh CO Faradaic efficiency (99%) at −0.45 V in CO2 electroreduction, far surpassing MOF-derived carbon without K+ etching. Theoretical calculations reveal that the V12 defects in K-defect-C favor CO2 adsorption and significantly accelerate the formation of the rate-determining COOH* intermediate, thereby promoting CO2 reduction. This work develops a novel strategy to generate intrinsic carbon defects and provides new insights into their critical role in catalysis.

中文翻译:

用于电催化 CO2 还原的多孔碳本征缺陷的钾辅助制造

固有碳缺陷的制造通常与掺杂效应纠缠在一起,识别它们在催化中的独特作用仍然是一项艰巨的任务。在此,开发了一种 K +辅助合成策略,通过直接热解 K +限制的金属-有机框架 (MOF)来提供具有丰富固有缺陷和完全消除杂原子的多孔碳 (K-缺陷-C )。正电子湮没寿命光谱、X 射线吸收精细结构测量和扫描透射电子显微镜共同说明了 K 缺陷-C 中存在丰富的 12 空位型碳缺陷 (V 12 )。值得注意的是,K-缺陷-C 在 CO 2中在 -0.45 V 时实现了超高 CO 法拉第效率 (99%)电还原,远远超过没有 K +蚀刻的 MOF 衍生碳。理论计算表明,K-缺陷-C中的V 12缺陷有利于CO 2的吸附,显着加速了COOH*中间体的形成,从而促进了CO 2的还原。这项工作开发了一种产生内在碳缺陷的新策略,并为它们在催化中的关键作用提供了新的见解。
更新日期:2022-08-10
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