Single-atom dispersed Co-N-C catalyst: structure identification and performance for hydrogenative coupling of nitroarenes.
Single-atom dispersed Co-N-C catalyst: structure identification and performance for hydrogenative coupling of nitroarenes.
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单原子分散Co-N-C催化剂：硝基芳烃氢化偶联的结构鉴定和性能
DOI：
10.1039/c6sc02105k
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发表时间：
2016-09-01
期刊：
影响因子：
8.4
通讯作者：
Zhang T
中科院分区：
文献类型：
--
作者：
Liu W;Zhang L;Yan W;Liu X;Yang X;Miao S;Wang W;Wang A;Zhang T
具有CoN 4C 8 -1- 2 O2结构的单原子Co-N-C催化剂在温和的反应条件下对硝基芳烃的选择性加氢反应具有良好的催化性能。Co-N-C催化剂在电催化和有机转化中是很有希望的替代铂的候选者。然而，高温热解产生的钴物种的异质性，obebers活性位点的结构识别。本文中，我们报道了自支撑Co-N-C催化剂，其中钴仅以单个原子分散。通过亚分辨HAADF-STEM结合XAFS和DFT计算，确定了Co-N-C的结构为CoN 4C 8 -1- 2 O2，其中Co中心原子与石墨层中的4个吡啶N原子配位，而2个氧分子在垂直于Co-N4平面的Co原子上弱吸附。这种单原子分散的Co-N-C催化剂在温和的反应条件下对硝基芳烃的选择性加氢反应具有优异的催化性能。
The single-atom Co–N–C catalyst with the structure of CoN4C8-1-2O2 shows excellent performance for the chemoselective hydrogenation of nitroarenes to produce azo compounds under mild reaction conditions. Co–N–C catalysts are promising candidates for substituting platinum in electrocatalysis and organic transformations. The heterogeneity of the Co species resulting from high-temperature pyrolysis, however, encumbers the structural identification of active sites. Herein, we report a self-supporting Co–N–C catalyst wherein cobalt is dispersed exclusively as single atoms. By using sub-Ångström-resolution HAADF-STEM in combination with XAFS and DFT calculation, the exact structure of the Co–N–C is identified to be CoN4C8-1-2O2, where the Co center atom is coordinated with four pyridinic N atoms in the graphitic layer, while two oxygen molecules are weakly adsorbed on Co atoms in perpendicular to the Co–N4 plane. This single-atom dispersed Co–N–C catalyst presents excellent performance for the chemoselective hydrogenation of nitroarenes to produce azo compounds under mild reaction conditions.
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