Yang Jingjing, Ruan Zhoushilin, Jiang Shenlong, Xia Pengfei, Yang Qinghua, Zhang Qun, Xiao Chong, Xie Yi
Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
Institute of Energy, Hefei Comprehensive National Science Center, Hefei, Anhui 230031, P. R. China.
J Phys Chem Lett. 2021 Nov 25;12(46):11295-11302. doi: 10.1021/acs.jpclett.1c03207. Epub 2021 Nov 15.
Nitrate acts as a fundamental raw material in modern industrial and agricultural fields. Recently, photocatalytic nitrogen oxidation into nitrate has been expected to be an alternative method to replace the industrial nitrate synthesis process, which encounters many challenges, i.e., huge energy consumption and greenhouse gas emission. We synthesized Ce-doped WO nanowires (Ce-WO) to realize photocatalytic nitrogen oxidation into nitrate under mild conditions. The defect state generated by coupling of Ce introduction and surface plasma state acts as an "electron trap" to restrain photogenerated electrons, so as to facilitate the separation of photogenerated electron-hole pairs and prolong their lifetime. WO doped with 5 mol % Ce exhibited the highest yield of nitrate (319.97 μg g h) without any sacrificial agent, which is about 5 times higher than that of pristine WO. This work provides new insight into achieving high-efficiency photocatalytic nitrate evolution activity from direct N oxidation by controlling the energy band structure of photocatalysts.
硝酸盐是现代工农业领域的一种重要原材料。近年来,光催化氮氧化制备硝酸盐有望成为替代工业硝酸盐合成工艺的一种方法,因为该工艺面临诸多挑战,如能耗巨大和温室气体排放等问题。我们合成了铈掺杂的WO纳米线(Ce-WO),以实现在温和条件下光催化氮氧化制备硝酸盐。铈引入与表面等离子体状态耦合产生的缺陷态作为“电子陷阱”来抑制光生电子,从而促进光生电子-空穴对的分离并延长其寿命。掺杂5 mol%铈的WO在无任何牺牲剂的情况下表现出最高的硝酸盐产率(319.97 μg g h),约为原始WO的5倍。这项工作为通过控制光催化剂的能带结构从直接氮氧化实现高效光催化硝酸盐析出活性提供了新的见解。