Electrochemical Reduction of CO2 Catalyzed by Fe-N-C Materials: A Structure-Selectivity Study
Electrochemical Reduction of CO2 Catalyzed by Fe-N-C Materials: A Structure-Selectivity Study
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DOI：
10.1021/acscatal.6b03353
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发表时间：
2017-03-01
期刊：
影响因子：
12.9
通讯作者：
Fontecave, Marc
中科院分区：
文献类型：
--
作者：
Huan, Tran Ngoc;Ranjbar, Nastaran;Fontecave, Marc
将CO选择性电化学还原为能量密集的有机化合物是使用CO作为碳源的一种有前途的策略。在这里，我们研究了一系列的铁基催化剂合成的热解的Fe-，N-，和C-含前体的CO，CO在水溶液条件下的电还原，并证明这些材料的选择性CO2还原质子还原是由隔离的FeN 4网站与Fe基纳米粒子的比例。该比率可以被综合地调节以产生产生受控的CO/H-2比率的电催化剂。它特别允许制备仅含有FeN 4位点的材料，其能够在水溶液中选择性地将CO还原为CO，法拉第产率超过90%并且在低过电位下。
Selective electrochemical reduction of CO, into energy-dense organic compounds is a promising strategy for using CO, as a carbon source. Herein, we investigate a series of iron-based catalysts synthesized by pyrolysis of Fe-, N-, and C-containing precursors for the electroreduction of CO, to CO under aqueous conditions and demonstrate that the selectivity of these materials for CO2 reduction over proton reduction is governed by the ratio of isolated FeN4 sites vs Fe-based nanoparticles. This ratio can be synthetically tuned to generate electrocatalysts producing controlled CO/H-2 ratios. It notably allows preparing materials containing only FeN4 sites, which are able to selectively reduce CO, to CO in aqueous solution with Faradaic yields of over 90% and at low overpotential.