Formation and stabilization of combustion-generated, environmentally persistent radicals on Ni(II)O supported on a silica surface.
Formation and stabilization of combustion-generated, environmentally persistent radicals on Ni(II)O supported on a silica surface.
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DOI：
10.1021/es301136d
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发表时间：
2012-09-04
影响因子：
11.4
通讯作者：
Dellinger, Barry
中科院分区：
文献类型：
--
作者：
Vejerano, Eric;Lomnicki, Slawomir M.;Dellinger, Barry
以往的研究表明，环境持久性自由基（EPFRs）形成时，羟基和氯取代的芳烃化学吸附在Cu（II）O和Fe（III）2O3表面，并通过与表面金属阳离子的相互作用稳定。目前的研究报告，我们的实验室调查EPFRs的形成和稳定的Ni（II）O表面。EPFR是通过吸附物在负载的金属氧化物表面上的化学吸附和电子从吸附物转移到金属中心，导致金属阳离子的还原而产生的。根据温度和吸附物的性质，形成一种以上的有机自由基。观察到一个g值在2.0029和2.0044之间的菲类自由基和一个g值在2.0050到高达2.0081之间的半醌类自由基。在Ni（II）O上的半衰期较长，为1.5至5.2天，与在Fe（III）2O3上观察到的半衰期相似。在Ni（II）O上形成的EPFR的产率比在Cu（II）O上高约8倍，比在Fe（III）2O3上高约50倍。
Previous studies have indicated Environmentally Persistent Free Radicals (EPFRs) are formed when hydroxyl- and chlorine-substituted aromatics chemisorbed on Cu(II)O and Fe(III)2O3 surfaces and were stabilized through their interactions with the surface metal cation. The current study reports our laboratory investigation on the formation and stabilization of EPFRs on an Ni(II)O surface. The EPFRs were produced by the chemisorption of adsorbates on the supported metal oxide surface and transfer of an electron from the adsorbate to the metal center, resulting in reduction of the metal cation. Depending on the temperature and the nature of the adsorbate, more than one type of organic radical was formed. A phenoxyl-type radical, with g-value between 2.0029 and 2.0044, and a semiquinone-type radical, with g-value from 2.0050 to as high as 2.0081, were observed. The half-lives on Ni(II)O were long and ranged from 1.5 to 5.2 days, which were similar to what were observed on Fe(III)2O3,. The yields of the EPFRs formed on Ni(II)O was ~ 8x higher than on Cu(II)O and ~50x higher than on Fe(III)2O3.
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影响因子：
4.1
作者：
Smith, KR;Aust, AE
通讯作者：
Aust, AE
影响因子：
10.4
作者：
Gurgueira SA;Lawrence J;Coull B;Murthy GG;González-Flecha B
通讯作者：
González-Flecha B
影响因子：
4.4
作者：
Altarawneh, Mohammednoor;Radny, Marian W.;Stampfl, Catherine
通讯作者：
Stampfl, Catherine
影响因子：
3.9
作者：
LEZNA, RO;DETACCONI, NR;ARVIA, AJ
通讯作者：
ARVIA, AJ
影响因子：
11.4
作者：
Khachatryan, Lavrent;Adounkpe, Julien;Dellinger, Barry
通讯作者：
Dellinger, Barry