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Defective Titanium Dioxide Nanobamboo Arrays Architecture for Photocatalytic Nitrogen Fixation up to 780 nm

Zhang, Yuanzheng and Chen, Xiang and Zhang, Siyao and Yin, Lifeng and Yang, Yang (2020) Defective Titanium Dioxide Nanobamboo Arrays Architecture for Photocatalytic Nitrogen Fixation up to 780 nm. Chemical Engineering Journal, 401 . Art. No. 126033. ISSN 1385-8947. https://resolver.caltech.edu/CaltechAUTHORS:20200629-130700118

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Abstract

Solar-driven nitrogen fixation is a potential solution to satisfying industrial and agricultural demand, but is severely hampered by the difficulties in capturing, activating and cleaving the dinitrogen (N₂). Here, the defect TiO₂ nanobamboo arrays (DTiO₂ NBAs) is designed with an electro-reduction strategy, which, for the first time, successfully converted N₂ to ammonia (NH₃) in the visible and near infrared light range under ambient conditions, without any sacrificial agent or noble-metal co-catalysts. A highly selective NH₃ yield of 48.3 mg m⁻² h⁻¹ (178 μmol g⁻¹ h⁻¹, no N₂H₄ formation) is obtained on the DTiO₂ NBAs haired titanium foil. The apparent quantum efficiency (AQE) was measured to be 0.39% at 365 nm, 0.12% at 405 nm, 0.11% at 450 nm, 0.15% at 532 nm, 0.24% at 650 nm, and 0.07% at 780 nm. It is found that the electro-reduction process creates amorphous surface layer with modest oxygen vacancy (O_(vac)) density so as to greatly enhance light harvesting, charge carrier, photo-thermal effect, as well as nitrogen adsorption and hydrogenation activity. The alternating photo-fixation pathway is also confirmed by density functional theory (DFT) calculations. This novel nanobamboo TiO_x architecture shows a potential as a new artificial nitrogen fixation for environmentally friendly NH₃ production.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1016/j.cej.2020.126033DOIArticle
ORCID:
AuthorORCID
Yang, Yang0000-0002-4956-2034
Additional Information:© 2020 Elsevier B.V. Received 12 May 2020, Revised 19 June 2020, Accepted 21 June 2020, Available online 28 June 2020. This work was financially supported by the National Natural Science Foundation of China (Grant 21777009), the Bill and Melinda Gates Foundation (BMGF RTTC Grants OPP1111246 and OPP1149755), Beijing Natural Science Foundation (Grant 8182031), and Major Science and Technology Program for Water Pollution Control and Treatment (Grant 2018ZX07109). The authors declare no conflict of interest.
Funders:
Funding AgencyGrant Number
National Natural Science Foundation of China21777009
Bill and Melinda Gates FoundationOPP1111246
Bill and Melinda Gates FoundationOPP1149755
Beijing Natural Science Foundation8182031
Major Science and Technology Program for Water Pollution Control and Treatment2018ZX07109
Subject Keywords:Defect TiO2; nanobamboo; nitrogen fixation; photocatalysis; near infrared light
Record Number:CaltechAUTHORS:20200629-130700118
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200629-130700118
Official Citation:Yuanzheng Zhang, Xiang Chen, Siyao Zhang, Lifeng Yin, Yang Yang, Defective titanium dioxide nanobamboo arrays architecture for photocatalytic nitrogen fixation up to 780 nm, Chemical Engineering Journal, Volume 401, 2020, 126033, ISSN 1385-8947, https://doi.org/10.1016/j.cej.2020.126033. (http://www.sciencedirect.com/science/article/pii/S1385894720321616)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:104132
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:29 Jun 2020 20:17
Last Modified:02 Jul 2020 15:59

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