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Nano Research 2023, 16(4): 4574-4581 https://doi.org/10.1007/s12274-022-4765-9
Research Article | Issue | Published: 22 August 2022

Bismuth stabilized by ZIF derivatives for electrochemical ammonia production: Proton donation effect of phosphorus dopants

Show Author's Information Qiaoling Wu1,  Ying Sun1( ),  Qin Zhao1,  Hui Li2,  Zhengnan Ju1,  Yu Wang1,  Xiaodong Sun1,  Baohua Jia2,  Jieshan Qiu3,  Tianyi Ma2( )
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province, College of Chemistry, Liaoning University, Shenyang 110036, China
School of Science, RMIT University, Melbourne, VIC 3000, Australia
College of Chemical Engineering, State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Keywords:
electrocatalysis, carbon nanoflakes, bismuth, N, N2 reduction, P co-doped
Topics:
Electrocatalysis Nanocatalysts
Cite this article:
Wu Q, Sun Y, Zhao Q, et al. Bismuth stabilized by ZIF derivatives for electrochemical ammonia production: Proton donation effect of phosphorus dopants. Nano Research, 2023, 16(4): 4574-4581. https://doi.org/10.1007/s12274-022-4765-9
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Abstract Full text Electronic supplementary material About this article

N2 electroreduction reaction (NRR) offers a feasible and promising alternative for NH3 production by using clean energy sources. However, it is still obstructed by the pretty low NH3 yield rate and Faradaic efficiency (FE) primarily due to the undesired competing hydrogen evolution reaction and the extremely stable N≡N bond. Herein, bismuth nanoparticles were successfully embedded in N and P co-doped carbon nanoflakes (Bi/NPC) by high-temperature pyrolyzation of Bi-zeolitic imidazole frameworks (ZIF) followed by phosphorization, and used as a high-efficiency catalyst toward N2 electroreduction to NH3. In 0.1 M KHCO3 electrolyte, Bi/NPC exhibits excellent NRR performances, including a high NH3 yield rate of 3.12 µg·h−1·cm−2 (−0.6 V vs. reversible hydrogen electrode (RHE)), an outstanding FE of 13.58% (−0.4 V vs. RHE), and a remarkable stability up to 36 h under ambient conditions. This outstanding NRR catalytic activity is mainly attributed to the intrinsic electrocatalytic NRR activity combined with the inert hydrogen evolution reaction (HER) activity of Bi, the adsorption and activation of N2 facilitated by N dopants, as well as the superior conductivity and the large specific surface area of the two-dimensional layered carbon matrix. Notably, the hydrogen source provided by P dopant promotes the hydrogenation of the adsorbed N, which further boosts the NRR performance in alkaline electrolyte. The ultralong durability of Bi/NPC is attributed to the highly dispersed bismuth catalytic active centers confined in the skeleton of N and P co-doped carbon nanoflakes, which inhibits the agglomeration of bismuth centers. This work presents a novel avenue for designation and fabrication of high-performance Bi-based electrocatalysts for NRR.


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Electronic supplementary material
About this article

Bismuth stabilized by ZIF derivatives for electrochemical ammonia production: Proton donation effect of phosphorus dopants

Show Author's information Qiaoling Wu1, Ying Sun1( ), Qin Zhao1, Hui Li2, Zhengnan Ju1, Yu Wang1, Xiaodong Sun1, Baohua Jia2, Jieshan Qiu3, Tianyi Ma2( )
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning Province, College of Chemistry, Liaoning University, Shenyang 110036, China
School of Science, RMIT University, Melbourne, VIC 3000, Australia
College of Chemical Engineering, State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China

Abstract

N2 electroreduction reaction (NRR) offers a feasible and promising alternative for NH3 production by using clean energy sources. However, it is still obstructed by the pretty low NH3 yield rate and Faradaic efficiency (FE) primarily due to the undesired competing hydrogen evolution reaction and the extremely stable N≡N bond. Herein, bismuth nanoparticles were successfully embedded in N and P co-doped carbon nanoflakes (Bi/NPC) by high-temperature pyrolyzation of Bi-zeolitic imidazole frameworks (ZIF) followed by phosphorization, and used as a high-efficiency catalyst toward N2 electroreduction to NH3. In 0.1 M KHCO3 electrolyte, Bi/NPC exhibits excellent NRR performances, including a high NH3 yield rate of 3.12 µg·h−1·cm−2 (−0.6 V vs. reversible hydrogen electrode (RHE)), an outstanding FE of 13.58% (−0.4 V vs. RHE), and a remarkable stability up to 36 h under ambient conditions. This outstanding NRR catalytic activity is mainly attributed to the intrinsic electrocatalytic NRR activity combined with the inert hydrogen evolution reaction (HER) activity of Bi, the adsorption and activation of N2 facilitated by N dopants, as well as the superior conductivity and the large specific surface area of the two-dimensional layered carbon matrix. Notably, the hydrogen source provided by P dopant promotes the hydrogenation of the adsorbed N, which further boosts the NRR performance in alkaline electrolyte. The ultralong durability of Bi/NPC is attributed to the highly dispersed bismuth catalytic active centers confined in the skeleton of N and P co-doped carbon nanoflakes, which inhibits the agglomeration of bismuth centers. This work presents a novel avenue for designation and fabrication of high-performance Bi-based electrocatalysts for NRR.

Keywords: electrocatalysis, carbon nanoflakes, bismuth, N, N2 reduction, P co-doped

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Publication history
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Acknowledgements

Publication history

Received: 25 May 2022
Revised: 20 June 2022
Accepted: 11 July 2022
Published: 22 August 2022
Issue date: April 2023

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was partly supported by the National Natural Science Foundation of China (No. 52071171), Liaoning Revitalization Talents Program-Pan Deng Scholars (No. XLYC1802005), Liaoning BaiQianWan Talents Program (No. LNBQW2018B0048), the Natural Science Fund of Liaoning Province for Excellent Young Scholars (No. 2019-YQ-04), the Key Project of Scientific Research of the Education Department of Liaoning Province (No. LZD201902), Shenyang Science and Technology Project (No. 21-108-9-04), the Young Scientific and Technological Talents Project of the Department of Education of Liaoning Province (No. LQN202008), the Foundation for Young Scholars of Liaoning University (No. LDQN2019007), Australian Research Council (ARC) through Future Fellowship (Nos. FT210100298 and FT210100806), Discovery Project (No. DP220100603), Linkage Project (Nos. LP210100467, LP210200504, and LP210200345), and Industrial Transformation Training Centre (No. IC180100005) schemes, CSIRO Energy Centre and Kick-Start Project. The Study Melbourne Research Partnerships program has been made possible by funding from the Victorian Government through Study Melbourne.

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