Ambient electrosynthesis of ammonia with efficient denitration

Xianyun Peng; Yuying Mi; Haihong Bao; Yifan Liu; Defeng Qi; Yuan Qiu; Longchao Zhuo; Shunzheng Zhao; Jiaqiang Sun; Xiaolong Tang; Jun Luo; Xijun Liu

doi:10.1016/j.nanoen.2020.105321

Ambient electrosynthesis of ammonia with efficient denitration

Xianyun Peng, Yuying Mi, Haihong Bao, Yifan Liu, Defeng Qi, Yuan Qiu, Longchao Zhuo, Shunzheng Zhao, Jiaqiang Sun, Xiaolong Tang, Jun Luo, Xijun Liu

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124 Scopus citations

Abstract

The NH₃ electrosynthesis under ambient conditions represents an attractive alternative to the traditional Haber−Bosch industrial process, and NO is one of the major air pollutants. Here, with single-atom-site Nb catalyst, the ambient electrochemical denitration of NO exhibited a record high NH₃ yield rate of 8.2 × 10⁻⁸ mol cm⁻² s⁻¹, which is two orders of magnitude larger than those achieved by the best-reported catalysts for the ambient NH₃ electrosynthesis and approaches the US Department of Energy target. Theoretical calculations reveal that the single-atomic Nb sites not only facilitate the NO adsorption but also lower the energy barrier of the potential-determining step.

Original language	English
Article number	105321
Journal	Nano Energy
Volume	78
DOIs	https://doi.org/10.1016/j.nanoen.2020.105321
State	Published - Dec 2020
Externally published	Yes

Funding

Based on our previous works [ 26–28] about single-atom-site catalysts, the method to prepare single-atom (SA) Nb sites supported on B,N co-doped carbon nanotubes (denoted as Nb-SA/BNC) is developed as: firstly mixing Nb(V) oxalate hydrate with polyethylene glycol, urea and boric acid, then using a commercial melamine foam to adsorb the resulting complexes, and heating the melamine foam at 900 °C in Ar (Fig. 1a and Figs. S1 and S2; see Materials and Methods in the Supporting Information for more details). M-SA/BNC (M = Al, Mn, Fe and Cu) and BNC were also synthesized by the same protocol as above, except that different metal precursors or no metal precursors were added (Figs. S3−S7).Besides, the single Nb sites supported on N doped carbon materials (Nb-SA/NC) was prepared as a reference. It was synthesized by a similar method to that of Nb-SA/BNC except no boric acid was added (please see more details in the Materials and Methods). The structure characterization results exhibit a nanosheet morphology of Nb-SA/NC (Fig. S15), and it gives a BET surface area of 589.4 m2 g−1 with a mesopore size of 5.1 nm (Figs. S10a and b). The Nb amount of the Nb-SA/NC was determined to be 1.87 wt% by ICP-AES. Additionally, the Nb–N bond can be detected at the binding energy of 204.3 eV in high-resolution Nb 3d spectrum of Nb-SA/NC (Fig. S15h).This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (51971157, 51808037, 21601136 and 51761165012), and Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800). The authors also thank the facility supports at the BL14W1 beamline of the Shanghai Synchrotron Radiation Facility (SSRF, China) and the Beijing Super Cloud Computing Center for providing the computational resources and materials studio. This work was financially supported by National Key R&D Program of China ( 2017YFA0700104 ), National Natural Science Foundation of China ( 51971157 , 51808037 , 21601136 and 51761165012 ), and Tianjin Science Fund for Distinguished Young Scholars ( 19JCJQJC61800 ). The authors also thank the facility supports at the BL14W1 beamline of the Shanghai Synchrotron Radiation Facility (SSRF, China) and the Beijing Super Cloud Computing Center for providing the computational resources and materials studio.

Keywords

Ambient NH electrosynthesis
Electrochemical denitration
NO reduction reaction
Record-level yield rate
Single-atomic Nb site

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10.1016/j.nanoen.2020.105321

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title = "Ambient electrosynthesis of ammonia with efficient denitration",

abstract = "The NH3 electrosynthesis under ambient conditions represents an attractive alternative to the traditional Haber−Bosch industrial process, and NO is one of the major air pollutants. Here, with single-atom-site Nb catalyst, the ambient electrochemical denitration of NO exhibited a record high NH3 yield rate of 8.2 × 10−8 mol cm−2 s−1, which is two orders of magnitude larger than those achieved by the best-reported catalysts for the ambient NH3 electrosynthesis and approaches the US Department of Energy target. Theoretical calculations reveal that the single-atomic Nb sites not only facilitate the NO adsorption but also lower the energy barrier of the potential-determining step.",

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T1 - Ambient electrosynthesis of ammonia with efficient denitration

AU - Peng, Xianyun

AU - Mi, Yuying

AU - Bao, Haihong

AU - Liu, Yifan

AU - Qi, Defeng

AU - Qiu, Yuan

AU - Zhuo, Longchao

AU - Zhao, Shunzheng

AU - Sun, Jiaqiang

AU - Tang, Xiaolong

AU - Luo, Jun

AU - Liu, Xijun

PY - 2020/12

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N2 - The NH3 electrosynthesis under ambient conditions represents an attractive alternative to the traditional Haber−Bosch industrial process, and NO is one of the major air pollutants. Here, with single-atom-site Nb catalyst, the ambient electrochemical denitration of NO exhibited a record high NH3 yield rate of 8.2 × 10−8 mol cm−2 s−1, which is two orders of magnitude larger than those achieved by the best-reported catalysts for the ambient NH3 electrosynthesis and approaches the US Department of Energy target. Theoretical calculations reveal that the single-atomic Nb sites not only facilitate the NO adsorption but also lower the energy barrier of the potential-determining step.

AB - The NH3 electrosynthesis under ambient conditions represents an attractive alternative to the traditional Haber−Bosch industrial process, and NO is one of the major air pollutants. Here, with single-atom-site Nb catalyst, the ambient electrochemical denitration of NO exhibited a record high NH3 yield rate of 8.2 × 10−8 mol cm−2 s−1, which is two orders of magnitude larger than those achieved by the best-reported catalysts for the ambient NH3 electrosynthesis and approaches the US Department of Energy target. Theoretical calculations reveal that the single-atomic Nb sites not only facilitate the NO adsorption but also lower the energy barrier of the potential-determining step.

KW - Ambient NH electrosynthesis

KW - Electrochemical denitration

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Ambient electrosynthesis of ammonia with efficient denitration

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Keywords

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