Hematite nanostructures: An old material for a new story. Simultaneous photoelectrochemical oxidation of benzylamine and hydrogen production through Ti doping

Hematite nanostructures: An old material for a new story. Simultaneous photoelectrochemical oxidation of benzylamine and hydrogen production through Ti doping
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DOI:
10.1016/j.nanoen.2019.04.013
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发表时间:
2019-07-01
期刊:
影响因子:
17.6
通讯作者:
Vomiero, Alberto
Vomiero, Alberto
中科院分区:
材料科学1区
文献类型:
--
作者:
Mazzaro, Raffaello;Bibi, Sara Boscolo;Vomiero, Alberto

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总体而言,水分解代表了太阳能转换和储存的最有前途的方法之一,然而,这受到析氧反应(OER)的四电子/四质子性质的严重挑战。克服这个问题的一个选择是用更有用的反应代替OER,以同时生产氢气和感兴趣的化学品。为此,在本文中,廉价的,水热制备的钛掺杂纳米结构的赤铁矿光阳极首次采用高稳定性,多相催化剂的低偏压,高效和高选择性的光诱导氧化苄胺N-亚苄基苄胺,并在双溶剂/环境电池中同时产生氢气。初步估计表明,有可能获得类似于150 μ mol h(-1)H-2的生产,与化学计量的苄叉N-苄胺在5 × 5 cm(2)面积的电极的当代生产。这项研究有助于克服40年来由于赤铁矿的性能差和氧气生产缺乏经济价值而限制赤铁矿在工业光电化学太阳光转换和储存中使用的持续问题,为赤铁矿在工业重要性的替代氧化反应中的使用提供坚实的证据。
Overall water splitting represents one of the most promising approaches toward solar energy conversion and storage, which is, however, severely challenged by the four-electron/four-proton nature of the oxygen evolution reaction (OER). One option to overcome this issue is to replace OER with a more useful reaction, for simultaneous production of both hydrogen and chemicals of interest. For the purpose, in this paper a cheap, hydrothermally prepared Ti-doped nanostructured hematite photoanode was employed for the first time as highly stable, heterogeneous catalyst for the low bias, efficient and highly selective photoinduced oxidation of benzylamine to N-benzylidenebenzylamine, and for the simultaneous production of hydrogen in a double solvent/environment cell. A preliminary estimate indicates the possibility to obtain a similar to 150 mu mol h(-1) H-2 production, with the contemporary production of stoichiometric benzylidene N-benzylamine in a 5 x 5 cm(2) area electrode. This study contributes to overcome the 40-year lasting issues limiting the use of hematite in industrial photo-electrochemical sunlight conversion and storage, due to poor performance of hematite and lack of economic value of oxygen production, providing solid evidence for the use of hematite in alternative oxidation reactions of industrial importance.