Metal-Free Nitrogen- and Boron-Codoped Mesoporous Carbons for Primary Amides Synthesis from Primary Alcohols via Direct Oxidative Dehydrogenation
Metal-Free Nitrogen- and Boron-Codoped Mesoporous Carbons for Primary Amides Synthesis from Primary Alcohols via Direct Oxidative Dehydrogenation
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用于通过直接氧化脱氢从伯醇合成伯酰胺的无金属氮和硼共掺杂介孔碳
DOI：
10.1021/acscatal.8b02889
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发表时间：
2018-11-01
期刊：
影响因子：
12.9
通讯作者：
Gao, Shuang
中科院分区：
文献类型：
--
作者：
Shang, Sensen;Chen, Pei-Pei;Gao, Shuang
无金属催化剂显示出环境友好性和成本效益，以及对金属和金属氧化物催化剂中毒的敏感性较低。在这方面，我们提出了无金属介孔氮和硼共掺杂的纳米碳（meso-N，B/C）的合成和表征，它表现出良好的催化性能，转化率为89%，选择性为83%，对伯醇使用NH 4 OAc作为氨源在氧气气氛下合成酰胺。通过热解富氮配体4，5-二氮杂芴-9-酮吖嗪（DAA）和分别作为氮和硼含量调节剂的H3 BO 3来执行简单的共掺杂合成策略。对比实验表明，该反应是通过脱氨缩合后的半缩醛胺直接氧化脱氢进行的，这与以往文献中的结果有很大不同。密度泛函理论（DFT）计算进一步表明，选择性偏好…
Metal-free catalysts show environmental friendliness and cost-effectiveness, as well as less susceptibility to poisoning over metal and metal oxide catalysts. In this respect, we present the synthesis and characterization of metal-free mesoporous nitrogen- and boron-codoped nanocarbon (meso-N,B/C), which exhibits good catalytic performance with conversion of 89% and selectivity of 83% toward amide synthesis from primary alcohols using NH4OAc as an ammonia resource under an oxygen atmosphere. The facile codoping synthetic strategy was executed by pyrolysis of nitrogen-enriched ligand 4,5-diazafluorene-9-one azine (DAA) and H3BO3 as a nitrogen and boron content modulator, respectively. Significantly, control experiments revealed that the reaction proceeded through direct oxidative dehydrogenation of hemiaminal after aldehyde-ammonia condensation, which was remarkably different from that in the previous literature. Density functional theory (DFT) calculations further demonstrate that the selective preference...