• 文献标题:   Photoprompted Hot Electrons from Bulk Cross-Linked Graphene Materials and Their Efficient Catalysis for Atmospheric Ammonia Synthesis
  • 文献类型:   Article
  • 作  者:   LU YH, YANG Y, ZHANG TF, GE Z, CHANG HC, XIAO PS, XIE YY, HUA L, LI QY, LI HY, MA B, GUAN NJ, MA YF, CHEN YS
  • 作者关键词:   graphene, photoprompted, hot electron, ammonia synthesi, atmospheric pressure
  • 出版物名称:   ACS NANO
  • ISSN:   1936-0851 EI 1936-086X
  • 通讯作者地址:   Nankai Univ
  • 被引频次:   43
  • DOI:   10.1021/acsnano.6b06472
  • 出版年:   2016

▎ 摘  要

Ammonia synthesis is the single most important chemical process in industry and has used the successful heterogeneous Haber-Bosch catalyst for over 100 years and requires processing under both high temperature (300-500 degrees C) and pressure (200-300 atm); thus, it has huge energy costs accounting for about 1-3% of human's energy consumption. Therefore, there has been a long and vigorous exploration to find a milder alternative process. Here, we demonstrate that by using an iron- and graphene-based catalyst, Fe@3DGraphene, hot (ejected) electrons from this composite catalyst induced by visible light in a wide range of wavelength up to red could efficiently facilitate the activation of N-2 and generate ammonia with H-2 directly at ambient pressure using light (including simulated sun light) illumination directly. No external voltage or electrochemical or any other agent is needed. The production rate increases with increasing light frequency under the same power and with increasing power under the same frequency. The mechanism is confirmed by the detection of the intermediate N2H4 and also with a measured apparent activation energy only similar to 1/4 of the iron based Haber-Bosch catalyst. Combined with the morphology control using alumina as the structural promoter, the catalyst retains its activity in a 50 h test.