解吸
离域电子
过渡金属
电解质
石墨氮化碳
镁
材料科学
化学
质子化
催化作用
分析化学(期刊)
吸附
金属
电极
物理化学
离子
有机化学
光催化
生物化学
色谱法
作者
Qiyou Wang,Kang Liu,Junwei Fu,Chao Cai,Huangjingwei Li,Long Yan,Shanyong Chen,Bao Liu,Hongmei Li,Wenzhang Li,Xiaoqing Qiu,Ning Zhang,Junhua Hu,Hao Pan,Min Liu
标识
DOI:10.1002/ange.202109329
摘要
Abstract Atomically dispersed transition metal sites have been extensively studied for CO 2 electroreduction reaction (CO 2 RR) to CO due to their robust CO 2 activation ability. However, the strong hybridization between directionally localized d orbits and CO vastly limits CO desorption and thus the activities of atomically dispersed transition metal sites. In contrast, s‐block metal sites possess nondirectionally delocalized 3s orbits and hence weak CO adsorption ability, providing a promising way to solve the suffered CO desorption issue. Herein, we constructed atomically dispersed magnesium atoms embedded in graphitic carbon nitride (Mg‐C 3 N 4 ) through a facile heat treatment for CO 2 RR. Theoretical calculations show that the CO desorption on Mg sites is easier than that on Fe and Co sites. This theoretical prediction is demonstrated by experimental CO temperature program desorption and in situ attenuated total reflection infrared spectroscopy. As a result, Mg‐C 3 N 4 exhibits a high turnover frequency of ≈18 000 per hour in H‐cell and a large current density of −300 mA cm −2 in flow cell, under a high CO Faradaic efficiency ≥90 % in KHCO 3 electrolyte. This work sheds a new light on s‐block metal sites for efficient CO 2 RR to CO.
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