Altering Hydrogenation Pathways in Photocatalytic Nitrogen Fixation by Tuning Local Electronic Structure of Oxygen Vacancy with Dopant.

Angewandte Chemie
Yanan BoYujie Xiong

Abstract

To avoid the energy-consuming step of direct N≡N bond cleavage, photocatalytic N2 fixation undergoing the associative pathways has been developed for mild-condition operation. However, it is a fundamental yet challenging task to gain comprehensive understanding on how the associative pathways (i.e., alternating vs. distal) are influenced and altered by the fine structure of catalysts, which eventually holds the key to significantly promote the practical implementation. Herein, we introduce Fe dopants into TiO2 nanofibers to stabilize oxygen vacancies and simultaneously tune their local electronic structure. The combination of in situ characterizations with first-principles simulations reveals that the modulation of local electronic structure by Fe dopants turns the hydrogenation of N2 from associative alternating pathway to associative distal pathway. This work provides fresh hints for rationally controlling the reaction pathways toward efficient photocatalytic nitrogen fixation.

References

Jan 26, 2017·ACS Applied Materials & Interfaces·Hanna HeHaiyan Wang
Jul 18, 2017·Journal of the American Chemical Society·Hiroaki HirakawaTakayuki Hirai
Mar 31, 2018·Science·Daniel SippelOliver Einsle
Jul 18, 2018·Nature Chemistry·Yansong ZhouEdward H Sargent
May 1, 2019·Journal of the American Chemical Society·Canyu HuYujie Xiong
Sep 20, 2019·Journal of the American Chemical Society·Zhiyong ZhangSen Zhang
Nov 9, 2019·Journal of the American Chemical Society·Jing ZhangJun Lou
Jun 17, 2020·Nature Chemistry·Chen ChenShuangyin Wang

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