Construction of upconversion fluoride/attapulgite nanocomposite for visible-light-driven photocatalytic nitrogen fixatio
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RESEARCH ARTICLE
Construction of upconversion fluoride/attapulgite nanocomposite for visible-light-driven photocatalytic nitrogen fixation Xuhua YE1, Xiangyu YAN1, Xini CHU1, Shixiang ZUO1, Wenjie LIU1, Xiazhang LI (✉)1,2, and Chao YAO (✉)1 1 Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, Changzhou University, Changzhou 213164, China 2 Department of Materials Science and Engineering, University of Delaware, Newark, DE 19716, USA
© Higher Education Press 2020
ABSTRACT: Developing photocatalysts with wide spectrum absorption and strong nitrogen activation is critical for nitrogen fixation under mild conditions. Herein, onedimensional natural clay attapulgite (ATP) supported YF3:Sm3+ were successfully synthesized via microwave hydrothermal method, and the composites were employed as the catalyst for photocatalytic nitrogen fixation under visible-light irradiation. Results indicated that the production of ammonia reached as high as 41.2 mg$L-1 within 3 h when the molar ratio of Sm3+ and the mass fraction of YF3:Sm3+ were optimized. The enhanced fixation performance is mainly due to that the modified ATP fibber with abundant active sites and the doped fluoride with defective vacancy facilitate the adsorption and activation of N2. Furthermore, the upconversion property of YF3:Sm3+ increases the harvesting of visible-light energy, meanwhile the Z-scheme heterostructure built between YF3:Sm3+ and modified ATP inhibits the recombination of charge carriers and retains high redox potentials for N2 reduction. KEYWORDS:
photocatalysis; nitrogen fixation; attapulgite; upconversion; Z-scheme
Contents 1 Introduction 2 Experimental 2.1 Chemical resources 2.2 Synthesis of YF3:Sm3+/ATP nanocomposites 2.3 Characterization 2.4 Photocatalytic nitrogen fixation activity 3 Results and discussion Received May 28, 2020; accepted August 7, 2020 E-mails: [email protected] (X.L.), [email protected] (C.Y.)
3.1 3.2 3.3 3.4 3.5 3.6 3.7 3.8 3.9 3.10 3.11
XRD analysis UV–Vis analysis FT-IR analysis TEM analysis PL analysis EIS analysis XPS analysis ESR analysis Mott–Schottky analysis VB-XPS analysis N2 adsorption–desorption and transient photocurrent response
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Front. Mater. Sci.
3.12 Visible-light photocatalytic nitrogen fixation 3.13 Photocatalytic nitrogen fixation mechanism 4 Conclusions Disclosure of potential conflicts of interest Acknowledgements References
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Introduction
Ammonia (NH3) is an important resource and clean energy carrier for producing various chemical products [1–4]. Because of the strong bond of N≡N, most organisms can only absorb ammonia ion and nitrate ion rather than molecular nitrogen [5–7]. Up to date, the Haber–Bosch method has been widely used to produce ammonia from the reaction of nitrogen and hydrogen. Unfortunately, it requires high temperature and extreme pressure, which largely limits its development in industrial applications [8]. Therefore, it is important to develop new strategy for nitrogen fixation with low
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