High-Efficiency "Working-in-Tandem" Nitrogen Photofixation Achieved by Assembling Plasmonic Gold Nanocrystals on Ultrathin Titania Nanosheets.
High-Efficiency "Working-in-Tandem" Nitrogen Photofixation Achieved by Assembling Plasmonic Gold Nanocrystals on Ultrathin Titania Nanosheets.
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DOI：
10.1021/jacs.8b03537
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发表时间：
2018-06
影响因子：
15
通讯作者：
Jianhua Yang;Yanzhen Guo;R. Jiang;F. Qin;Han Zhang;Wenzheng Lu;Jianfang Wang;Jimmy C. Yu
中科院分区：
文献类型：
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作者：
Jianhua Yang;Yanzhen Guo;R. Jiang;F. Qin;Han Zhang;Wenzheng Lu;Jianfang Wang;Jimmy C. Yu
将大气中的N2固定为NH3是维持生命的重要过程。一个巨大的挑战是开发有效的催化剂在环境条件下光固定N2。在此，我们报告了一种全无机催化剂，Au纳米晶体锚定在具有氧空位的TiO 2纳米片上。它可以在室温和大气压下完成光驱动的N2固定在“串联工作”的途径。TiO 2纳米片上的氧空位化学吸附并活化N2分子，N2分子随后通过由Au纳米晶体的等离子体激元激发产生的热电子还原为NH3。在550 nm处，入射光子转化为NH3的表观量子效率为0.82%，高于迄今为止报道的那些。与单独使用的Au纳米球相比，用Au纳米球和纳米棒的混合物优化整个可见光范围内的吸收进一步将N2光固定率提高了66.2%。这项工作提供了一种新的方法，合理设计的高效催化剂对可持续的N2固定通过一个能源需求较少的光化学过程相比，工业哈伯-博世过程。
The fixation of atmospheric N2 to NH3 is an essential process for sustaining life. One grand challenge is to develop efficient catalysts to photofix N2 under ambient conditions. Herein we report an all-inorganic catalyst, Au nanocrystals anchored on ultrathin TiO2 nanosheets with oxygen vacancies. It can accomplish photodriven N2 fixation in the "working-in-tandem" pathway at room temperature and atmospheric pressure. The oxygen vacancies on the TiO2 nanosheets chemisorb and activate N2 molecules, which are subsequently reduced to NH3 by hot electrons generated from plasmon excitation of the Au nanocrystals. The apparent quantum efficiency of 0.82% at 550 nm for the conversion of incident photons to NH3 is higher than those reported so far. Optimizing the absorption across the overall visible range with the mixture of Au nanospheres and nanorods further enhances the N2 photofixation rate by 66.2% in comparison with Au nanospheres used alone. This work offers a new approach for the rational design of efficient catalysts toward sustainable N2 fixation through a less energy-demanding photochemical process compared to the industrial Haber-Bosch process.