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Unveiling Active Sites of CO2 Reduction on Nitrogen-Coordinated and Atomically Dispersed Iron and Cobalt Catalysts
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-03-08 00:00:00 , DOI: 10.1021/acscatal.8b00398 Fuping Pan 1 , Hanguang Zhang 2 , Kexi Liu 3 , David Cullen , Karren More , Maoyu Wang 4 , Zhenxing Feng 4 , Guofeng Wang 3 , Gang Wu 2 , Ying Li 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-03-08 00:00:00 , DOI: 10.1021/acscatal.8b00398 Fuping Pan 1 , Hanguang Zhang 2 , Kexi Liu 3 , David Cullen , Karren More , Maoyu Wang 4 , Zhenxing Feng 4 , Guofeng Wang 3 , Gang Wu 2 , Ying Li 1
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Herein, we report the exploration of understanding the reactivity and structure of atomically dispersed M–N4 (M = Fe and Co) sites for the CO2 reduction reaction (CO2RR). Nitrogen coordinated Fe or Co site atomically dispersed into carbons (M–N–C) containing bulk- and edge-hosted M–N4 coordination were prepared by using Fe- or Co-doped metal–organic framework precursors, respectively, which were further studied as ideal model catalysts. Fe is intrinsically more active than Co in M–N4 for the reduction of CO2 to CO, in terms of a larger current density and a higher CO Faradaic efficiency (FE) (93% vs. 45%). First principle computations elucidated that the edge-hosted M–N2+2–C8 moieties bridging two adjacent armchair-like graphitic layers is the active sites for the CO2RR. They are much more active than previously proposed bulk-hosted M–N4–C10 moieties embedded compactly in a graphitic layer. During the CO2RR, when the dissociation of *COOH occurs on the M–N2+2–C8, the metal atom is the site for the adsorption of *CO and the carbon atom with a dangling bond next to an adjacent N is the other active center to bond *OH. In particular, on the Fe–N2+2–C8 sites, the CO2RR is more favorable over the hydrogen evolution reaction, thus resulting in a remarkable FE.
中文翻译：
在氮配位和原子分散的铁和钴催化剂上发现CO 2还原的活性位点
在这里，我们报告了探索了解原子分散的M–N 4（M = Fe和Co）位对于CO 2还原反应（CO2RR）的反应性和结构的探索。通过分别使用铁或钴掺杂的金属有机骨架前驱体制备了原子配位的Fe或Co配位原子，原子散布到碳中（M–N–C），其中包含主体和边缘托管的M–N 4配位。被研究为理想的模型催化剂。就更大的电流密度和更高的法拉第效率（FE）（93％比45％）而言，在M–N 4中，Fe本质上比Co具有更强的活性，可以将CO 2还原为CO 。第一原理计算阐明了边缘托管的M–N 2 + 2 –C桥接两个相邻的扶手椅状石墨层的8个部分是CO2RR的活性位点。它们比紧凑地嵌入石墨层中的先前提出的大量存在的M–N 4 –C 10部分更具活性。在CO2RR期间，当* COOH的解离发生在M–N 2 + 2 –C 8上时，金属原子是* CO的吸附位点，并且带有与相邻N相邻的悬挂键的碳原子是其他活性中心键合* OH。特别是，在Fe–N 2 + 2 –C 8位上，CO2RR优于析氢反应，因此产生了显着的FE。
更新日期：2018-03-08
中文翻译：
在氮配位和原子分散的铁和钴催化剂上发现CO 2还原的活性位点
在这里，我们报告了探索了解原子分散的M–N 4（M = Fe和Co）位对于CO 2还原反应（CO2RR）的反应性和结构的探索。通过分别使用铁或钴掺杂的金属有机骨架前驱体制备了原子配位的Fe或Co配位原子，原子散布到碳中（M–N–C），其中包含主体和边缘托管的M–N 4配位。被研究为理想的模型催化剂。就更大的电流密度和更高的法拉第效率（FE）（93％比45％）而言，在M–N 4中，Fe本质上比Co具有更强的活性，可以将CO 2还原为CO 。第一原理计算阐明了边缘托管的M–N 2 + 2 –C桥接两个相邻的扶手椅状石墨层的8个部分是CO2RR的活性位点。它们比紧凑地嵌入石墨层中的先前提出的大量存在的M–N 4 –C 10部分更具活性。在CO2RR期间，当* COOH的解离发生在M–N 2 + 2 –C 8上时，金属原子是* CO的吸附位点，并且带有与相邻N相邻的悬挂键的碳原子是其他活性中心键合* OH。特别是，在Fe–N 2 + 2 –C 8位上，CO2RR优于析氢反应，因此产生了显着的FE。
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