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Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction
Advanced Materials ( IF 29.4 ) Pub Date : 2018-02-09 , DOI: 10.1002/adma.201706287
Yi Cheng 1 , Shiyong Zhao 1 , Bernt Johannessen 2 , Jean‐Pierre Veder 3 , Martin Saunders 4 , Matthew R. Rowles 3 , Min Cheng 5 , Chang Liu 5 , Matthew F. Chisholm 6 , Roland Marco 1, 7, 8 , Hui‐Ming Cheng 5, 9, 10 , Shi‐Ze Yang 6 , San Ping Jiang 1
Affiliation  

Single‐atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1–2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen‐doped carbon nanotubes (MSA‐N‐CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA‐N‐CNTs, using a new multistep pyrolysis process. Among these materials, NiSA‐N‐CNTs show an excellent selectivity and activity for the electrochemical reduction of CO2 to CO, achieving a turnover frequency (TOF) of 11.7 s−1 at −0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.

中文翻译:

具有超高载量的碳纳米管上的原子分散过渡金属,用于选择性电化学还原二氧化碳

单原子催化剂(SAC)是催化反应的最小实体,预计具有高原子效率,出色的活性和选择性。但是,SAC的实际应用遭受的金属负载非常低,仅为1-2 wt%。在此,合成了一类基于氮掺杂碳纳米管(MSA-N-CNT,其中M = Ni,Co,NiCo,CoFe和NiPt)上原子分散的过渡金属的SAC,其金属负载非常高,例如,对于NiSA-N-CNT,采用新的多步热解工艺可达到20 wt%。在这些材料中,NiSA-N-CNT具有出色的选择性和电化学还原CO 2转化为CO的活性,实现的周转频率(TOF)为11.7 s -1 在-0.55 V(相对于可逆氢电极(RHE))下,比负载在CNT上的Ni纳米颗粒高两个数量级。
更新日期:2018-02-09
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