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Two-dimensional BCN matrix inlaid with single-atom-Cu driven electrochemical nitrate reduction reaction to achieve sustainable industrial-grade production of ammonia
Yunnan Univ, Peoples R China; Wuhan Univ, Peoples R China.
Yunnan Univ, Peoples R China.
Yunnan Univ, Peoples R China.
Wuhan Univ, Peoples R China.
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2021 (English)In: APPLIED MATERIALS TODAY, ISSN 2352-9407, Vol. 25, article id 101206Article in journal (Refereed) Published
Abstract [en]

Electrochemical methods have been proven to effectively eliminate nitrates in sewage and convert them into high value-added ammonia products. Here, after annealing treatment of metal boron cluster organic polymers formed by the combination of 1,10-phenanthroline, Cu2+ and closo-[B12H12](2)(-), a Cu single-atom doped BCN (B-doped CN) with a diamond-shaped nanosheet structure was obtained. In the electrochem-ical reduction reaction of nitrate, BCN-Cu exhibits excellent catalytic activity, specifically: 1) the ammonia yield rate reached as high as 498.85 mu g h(-1) cm(-2), 1047.14 mu g h(-1) cm(-2), 1900.07 mu g h(-1) cm(-2) and 3358.74 mu g h(-1) cm(-2) at -0.3 V, -0.4 V, -0.5 V and -0.6 V vs reversible hydrogen electrode, respectively, and Faradaic efficiency is 95.90%, 97.28%, 98.23% and 97.37%; 2) after repeated use of BCN-Cu 10 times or continuous operation for 16 h, the activity against electrochemical reduction reaction of nitrate anions is almost unchanged. The (NO3-)-N-15 isotopic labeling experiment proved that the detected NH3 comes from the reduction of NO3- on BCN-Cu. Control experiments show that the presence of Cu determines whether BCN-Cu has the possibility of catalyzing electrochemical reduction reactions of nitrate, and the presence of the B element enhances the catalytic activity of BCN-Cu. Density functional calculations indicate that in the water phase the process of reducing NO3- to NH3 on Cu-0 is an exothermic reaction, and that the adsorption process of NO3- on Cu-0 is the rate-determining step. (C) 2021 Elsevier Ltd. All rights reserved.

Place, publisher, year, edition, pages
ELSEVIER , 2021. Vol. 25, article id 101206
Keywords [en]
Synthetic ammonia; Electrocatalysis; Nitrate reduction; Nitrate removal; Single-atom Cu
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-180724DOI: 10.1016/j.apmt.2021.101206ISI: 000707755300008OAI: oai:DiVA.org:liu-180724DiVA, id: diva2:1607785
Note

Funding Agencies|National Key R&D Program of China [2019YFC1804400]; Special Project for So-cial Development of Yunnan Province [202103AC100001]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [U2002213, 22179100]; Double Tops Joint Fund of the Yunnan Science and Technol-ogy Bureau and Yunnan University [2019FY003025]; Double-First Class University Construction Project [C17622010 0 042, CZ21623201]; science and technology innovation Program of Hunan Province [2020RC5026, 2020GK4040]; Swedish Research CouncilSwedish Research CouncilEuropean Commission [2020-04600, SNIC 2020/3-29]; Olle Engkvist Byggmastare foundation [212-0178]

Available from: 2021-11-02 Created: 2021-11-02 Last updated: 2021-12-28

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