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Polyoxometalates 2024, 3(1): 9140044 https://doi.org/10.26599/POM.2023.9140044
Research Article | Open Access | Issue | Published: 08 December 2023

Hexanuclear nickel-added silicotungstates as high-efficiency electrocatalysts for nitrate reduction to ammonia

Show Author's Information Zhihui Ni ( ),  Ning Liu,  Chunhui Zhao,  Liwei Mi ( )
Center for Advanced Materials Research, Henan Key Laboratory of Functional Salt Materials, Zhongyuan University of Technology, Zhengzhou 450007, China
Keywords:
electrocatalyst, polyoxometalates, metal-added, nitrate reduction
Cite this article:
Ni Z, Liu N, Zhao C, et al. Hexanuclear nickel-added silicotungstates as high-efficiency electrocatalysts for nitrate reduction to ammonia. Polyoxometalates, 2024, 3(1): 9140044. https://doi.org/10.26599/POM.2023.9140044
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Abstract Full text Electronic supplementary material About this article

Ammonia (NH3) is widely used in a wide range of fields because of its high energy density, and NH3 is simple to liquefy and transport. Nitrate is also a source of pollution of the environment and drinking water sources. Therefore, there is a pressing demand for the design and production of high-efficiency catalysts for the nitrate reduction reaction (NO3RR). Herein, two nickel-added polyoxometalates (NiAPs), namely, [Ni(en)2][Ni6(μ3-OH)3(en)3(H2O)6(B-α-SiW9O34)]2·6H2O (Ni6en) and [Ni(enMe)2(H2O)2][Ni6(μ3-OH)3(H2O)6(enMe)3(B-α-SiW9O34)]2·8H2O (Ni6enMe) (en = ethylenediamine, enMe = 1,2-diaminopropane), were effectively synthesized under hydrothermal conditions that contained several electrons and were used as electrocatalytic nitrate reduction reaction (e-NO3RR) catalysts. The structures of the compounds were characterized by using various instruments such as powder X-ray diffraction (PXRD) spectroscopy, infrared (IR) spectroscopy, thermogravimetric analysis (TGA), Brunauer–Emmett–Teller (BET) method, scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). e-NO3RR tests were performed using electrochemical workstation. Results show that Ni6en and Ni6enMe have high-efficient electrochemical catalytic nitrogen reduction to NH3. The highest NH3 yield rate for Ni6en was 3.66 mg∙h−1∙mgcat.−1 with Faradaic efficiency (FE) of 89.32%, whereas that for Ni6enMe was 3.46 mg∙h−1∙mgcat.−1 with FE of 86.75% at a low voltage (−0.5 V vs. reversible hydrogen electrode (RHE)). This finding creates a novel path for manufacturing highly effective NO3RR electrocatalysts using metal-added polyoxometalate as the catalyst in ambient settings. Furthermore, the findings of this research provide practical advice for creating effective electrocatalytic catalysts.


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Electronic supplementary material
About this article

Hexanuclear nickel-added silicotungstates as high-efficiency electrocatalysts for nitrate reduction to ammonia

Show Author's information Zhihui Ni ( ), Ning Liu, Chunhui Zhao, Liwei Mi ( )
Center for Advanced Materials Research, Henan Key Laboratory of Functional Salt Materials, Zhongyuan University of Technology, Zhengzhou 450007, China

Abstract

Ammonia (NH3) is widely used in a wide range of fields because of its high energy density, and NH3 is simple to liquefy and transport. Nitrate is also a source of pollution of the environment and drinking water sources. Therefore, there is a pressing demand for the design and production of high-efficiency catalysts for the nitrate reduction reaction (NO3RR). Herein, two nickel-added polyoxometalates (NiAPs), namely, [Ni(en)2][Ni6(μ3-OH)3(en)3(H2O)6(B-α-SiW9O34)]2·6H2O (Ni6en) and [Ni(enMe)2(H2O)2][Ni6(μ3-OH)3(H2O)6(enMe)3(B-α-SiW9O34)]2·8H2O (Ni6enMe) (en = ethylenediamine, enMe = 1,2-diaminopropane), were effectively synthesized under hydrothermal conditions that contained several electrons and were used as electrocatalytic nitrate reduction reaction (e-NO3RR) catalysts. The structures of the compounds were characterized by using various instruments such as powder X-ray diffraction (PXRD) spectroscopy, infrared (IR) spectroscopy, thermogravimetric analysis (TGA), Brunauer–Emmett–Teller (BET) method, scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). e-NO3RR tests were performed using electrochemical workstation. Results show that Ni6en and Ni6enMe have high-efficient electrochemical catalytic nitrogen reduction to NH3. The highest NH3 yield rate for Ni6en was 3.66 mg∙h−1∙mgcat.−1 with Faradaic efficiency (FE) of 89.32%, whereas that for Ni6enMe was 3.46 mg∙h−1∙mgcat.−1 with FE of 86.75% at a low voltage (−0.5 V vs. reversible hydrogen electrode (RHE)). This finding creates a novel path for manufacturing highly effective NO3RR electrocatalysts using metal-added polyoxometalate as the catalyst in ambient settings. Furthermore, the findings of this research provide practical advice for creating effective electrocatalytic catalysts.

Keywords: electrocatalyst, polyoxometalates, metal-added, nitrate reduction

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Received: 29 August 2023
Revised: 29 October 2023
Accepted: 21 November 2023
Published: 08 December 2023
Issue date: March 2024

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© The Author(s) 2023. Published by Tsinghua University Press.

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Acknowledgements

This work was financially supported by the Natural Science Foundation of Henan Province (No. 232300420386) and University Natural Science Foundation of Zhongyuan Institute of Technology (No. K2023QN004)

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