Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO(2).
Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO(2).
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DOI：
10.1038/s41467-017-01035-z
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发表时间：
2017-10-16
影响因子：
16.6
通讯作者：
Strasser P
中科院分区：
文献类型：
--
作者：
Ju W;Bagger A;Hao GP;Varela AS;Sinev I;Bon V;Roldan Cuenya B;Kaskel S;Rossmeisl J;Strasser P
利用可再生电力将二氧化碳直接电化学还原为燃料和化学品引起了人们的极大关注，部分原因是与反应性和选择性有关的根本挑战，部分原因是它对工业二氧化碳消耗气体扩散阴极的重要性。在这里，我们介绍了金属和氮掺杂的含有催化活性的M-NX部分(M = ，Mn，Fe，Co，Ni，Cu)的多孔炭在CO_2到CO电催化方面的研究进展。我们考察了它们的本征催化活性、CO转化率和CO法拉第效率，证明了Fe-N-C，特别是Ni-N-C催化剂与Au和Ag基催化剂相竞争。我们用密度泛函理论对催化活性的M-NX基团进行了模拟，并将理论结合能与实验进行了关联，给出了反应选择性的参数。这有助于从原子尺度上理解M-NX基团的势相关CO和碳氢化合物选择性，并为选择性碳基CO2还原催化剂的合理设计提供预测性指导。廉价和选择性的二氧化碳减排电催化剂为可持续燃料生产带来了希望。在这里，作者报道了N配位的、非贵金属掺杂的多孔炭作为二氧化碳转化为CO的高效和选择性的电催化剂。
Direct electrochemical reduction of CO2 to fuels and chemicals using renewable electricity has attracted significant attention partly due to the fundamental challenges related to reactivity and selectivity, and partly due to its importance for industrial CO2-consuming gas diffusion cathodes. Here, we present advances in the understanding of trends in the CO2 to CO electrocatalysis of metal- and nitrogen-doped porous carbons containing catalytically active M–Nx moieties (M = Mn, Fe, Co, Ni, Cu). We investigate their intrinsic catalytic reactivity, CO turnover frequencies, CO faradaic efficiencies and demonstrate that Fe–N–C and especially Ni–N–C catalysts rival Au- and Ag-based catalysts. We model the catalytically active M–Nx moieties using density functional theory and correlate the theoretical binding energies with the experiments to give reactivity-selectivity descriptors. This gives an atomic-scale mechanistic understanding of potential-dependent CO and hydrocarbon selectivity from the M–Nx moieties and it provides predictive guidelines for the rational design of selective carbon-based CO2 reduction catalysts. Inexpensive and selective electrocatalysts for CO2 reduction hold promise for sustainable fuel production. Here, the authors report N-coordinated, non-noble metal-doped porous carbons as efficient and selective electrocatalysts for CO2 to CO conversion.
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DOI：
10.1039/c2cp41957b
发表时间：
2012-09-07
期刊：
Physical chemistry chemical physics : PCCP
影响因子：
--
作者：
Kramm UI;Herranz J;Larouche N;Arruda TM;Lefèvre M;Jaouen F;Bogdanoff P;Fiechter S;Abs-Wurmbach I;Mukerjee S;Dodelet JP
通讯作者：
Dodelet JP
影响因子：
7.3
作者：
Jovanov, Zarko P.;Hansen, Heine A.;Chorkendorff, Ib
通讯作者：
Chorkendorff, Ib
影响因子：
16.6
作者：
Kumar, Bijandra;Asadi, Mohammad;Salehi-Khojin, Amin
通讯作者：
Salehi-Khojin, Amin
影响因子：
2.1
作者：
Bahn, SR;Jacobsen, KW
通讯作者：
Jacobsen, KW
影响因子：
32.5
作者：
Kuhl, Kendra P.;Cave, Etosha R.;Jaramillo, Thomas F.
通讯作者：
Jaramillo, Thomas F.