Citation: Tao Feng, Fengting Li, Xiaojun Hu, Ying Wang. Selective electroreduction of nitrate to ammonia via NbWO₆ perovskite nanosheets with oxygen vacancy[J]. Chinese Chemical Letters, ;2023, 34(5): 107862. doi: 10.1016/j.cclet.2022.107862 shu

Selective electroreduction of nitrate to ammonia via NbWO₆ perovskite nanosheets with oxygen vacancy

Tao Feng ^a ,
Fengting Li ^{b, c} ,
Xiaojun Hu ^{a, *,} ,
Ying Wang ^{b, c, *,}

a.
School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai 201418, China
b.
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
c.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

hu-xj@mail.tsinghua.edu.cn

yingwang@tongji.edu.cn

Received Date: 4 June 2022
Revised Date: 10 September 2022
Accepted Date: 26 September 2022
Available Online: 28 September 2022

Figures(5)

Electrocatalytic nitrate reduction to ammonia (NRA) under ambient conditions is significant for carbon-neutral synthetic fuels. Nevertheless, the lack of efficient electrocatalysts with tunable nanostructure for NRA remains a grand challenge. Herein, NbWO₆ nanosheets with oxygen vacancy (NbWO_6-x) was demonstrated via thermal treatment and exfoliation with NH₃ selectivity of 86.8% and Faradaic efficiency of 85.7% toward NRA. ¹H nuclear magnetic resonance spectra coupled with ¹⁵N isotope labeling experiments proved that NH₃ originated from NO₃⁻. The function of oxygen vacancy was revealed by computational studies in NRA. Moreover, the reaction mechanism and pathway of NRA could be deduced based on the results of online differential electrochemical mass spectrometry (DEMS). This work provides a selective NH₃ generation strategy to decarbonize the energy-chemical sector, bridging the gap between batteries and biofuels.
- Nitrate reduction,
- Ammonia generation,
- NbWO_6-x nanosheets,
- Oxygen vacancy,
- Adsorption energy
1. [1]
  D. Yao, C. Tang, L. Li, et al., Adv. Energy Mater. 10 (2020) 2001289. doi: 10.1002/aenm.202001289
2. [2]
  J. Wang, T. Feng, J. Chen, et al., Nano Energy 86 (2021) 106088. doi: 10.1016/j.nanoen.2021.106088
3. [3]
  M. Kitano, S. Kanbara, Y. Inoue, et al., Nat. Commun. 6 (2015) 6731–6739. doi: 10.1038/ncomms7731
4. [4]
  D. Bao, Q. Zhang, F.L. Meng, et al., Adv. Mater. 29 (2017) 1604799. doi: 10.1002/adma.201604799
5. [5]
  J. Wang, L. Ling, Z. Deng, W.X. Zhang, Sci. Bull. 65 (2020) 926–933. doi: 10.1016/j.scib.2020.02.015
6. [6]
  V. Rosca, M. Duca, M.T. d. Groot, M.T.M. Koper, Chem. Rev. 109 (2009) 2209–2244. doi: 10.1021/cr8003696
7. [7]
  D.E. Canfield, A.N. Glazer, P.G. Falkowski, Science 330 (2010) 192–196. doi: 10.1126/science.1186120
8. [8]
  T. Feng, J. Wang, Y. Wang, et al., Chem. Eng. J. 433 (2022) 133495. doi: 10.1016/j.cej.2021.133495
9. [9]
  F. Ni, Y. Ma, J. Chen, W. Luo, J. Yang, Chin. Chem. Lett. 32 (2021) 2073–2078. doi: 10.1016/j.cclet.2021.03.042
10. [10]
  H.O. Song, Y. Zhou, A.M. Li, S. Mueller, Chin. Chem. Lett. 23 (2012) 603–606. doi: 10.1016/j.cclet.2012.03.004
11. [11]
  N. Barrabés, J. Sá, Appl. Catal. B 104 (2011) 1–5. doi: 10.1016/j.apcatb.2011.03.011
12. [12]
  R. Jia, Y. Wang, C. Wang, et al., ACS Catal. 10 (2020) 3533–3540. doi: 10.1021/acscatal.9b05260
13. [13]
  J. Wang, T. Feng, J. Chen, J.H. He, X. Fang, Research 2022 (2022) 9837012.
14. [14]
  D. Guo, S. You, F. Li, Y. Liu, Chin. Chem. Lett. 33 (2022) 1–10. doi: 10.1016/j.cclet.2021.06.027
15. [15]
  Y. Ren, Y. Liu, F. Liu, et al., Chin. Chem. Lett. 32 (2021) 2519–2523. doi: 10.1016/j.cclet.2021.02.007
16. [16]
  W. Zheng, Y. Liu, W. Liu, et al., Water Res. 194 (2021) 116961. doi: 10.1016/j.watres.2021.116961
17. [17]
  Z. Sun, R. Huo, C. Choi, et al., Nano Energy 62 (2019) 869–875. doi: 10.1016/j.nanoen.2019.06.019
18. [18]
  K. Chu, F. Liu, J. Zhu, et al., Adv. Energy Mater. 11 (2021) 2003799. doi: 10.1002/aenm.202003799
19. [19]
  Y. Liu, J. Xiong, S. Luo, et al., Chem. Commun. 51 (2015) 15125–15128. doi: 10.1039/C5CC05788D
20. [20]
  J. Wang, Y. Ren, H. Liu, et al., Adv. Mater. 34 (2021) e2104958.
21. [21]
  N. Zhang, X. Li, H. Ye, et al., J. Am. Chem. Soc. 138 (2016) 8928–8935. doi: 10.1021/jacs.6b04629
22. [22]
  T. Zheng, W. Sang, Z. He, et al., Nano Lett. 17 (2017) 7968–7973. doi: 10.1021/acs.nanolett.7b04430
23. [23]
  N. Zhang, X. Li, Y. Liu, et al., Small 13 (2017) 1701354. doi: 10.1002/smll.201701354
24. [24]
  H. Xu, J. Wu, W. Luo, et al., Small 16 (2020) e2001775. doi: 10.1002/smll.202001775
25. [25]
  L. Wang, M. Li, C. Feng, et al., J. Electroanal. Chem. 773 (2016) 13–21. doi: 10.1016/j.jelechem.2016.04.025
26. [26]
  C. Li, K. Li, C. Chen, et al., Sep. Purif. Technol. 237 (2020) 116485. doi: 10.1016/j.seppur.2019.116485
27. [27]
  L. Mattarozzi, S. Cattarin, N. Comisso, et al., Electrochim. Acta 89 (2013) 488–496. doi: 10.1016/j.electacta.2012.11.074
28. [28]
  D. Yin, Y. Liu, P. Song, et al., Electrochim. Acta 324 (2019) 134846. doi: 10.1016/j.electacta.2019.134846
29. [29]
  M. Chen, H. Wang, Y. Zhao, et al., Nanoscale 10 (2018) 19023–19030. doi: 10.1039/C8NR06360E
30. [30]
  W. Li, C. Xiao, Y. Zhao, et al., Catal. Lett. 146 (2016) 2585–2595. doi: 10.1007/s10562-016-1894-3
1. [1]
  Jijoe Samuel Prabagar , Kumbam Lingeshwar Reddy , Dong-Kwon Lim . Visible-light responsive gold nanoparticle and nano-sized Bi2O3-x sheet heterozygote structure for efficient photocatalytic conversion of N2 to NH3. Chinese Journal of Structural Chemistry, 2025, 44(4): 100564-100564. doi: 10.1016/j.cjsc.2025.100564
2. [2]
  Shenghui Tu , Anru Liu , Hongxiang Zhang , Lu Sun , Minghui Luo , Shan Huang , Ting Huang , Honggen Peng . Oxygen vacancy regulating transition mode of MIL-125 to facilitate singlet oxygen generation for photocatalytic degradation of antibiotics. Chinese Chemical Letters, 2024, 35(12): 109761-. doi: 10.1016/j.cclet.2024.109761
3. [3]
  Gang Hu , Chun Wang , Qinqin Wang , Mingyuan Zhu , Lihua Kang . The controlled oxidation states of the H₄PMo₁₁VO₄₀ catalyst induced by plasma for the selective oxidation of methacrolein. Chinese Chemical Letters, 2025, 36(2): 110298-. doi: 10.1016/j.cclet.2024.110298
4. [4]
  Yunxia Liu , Guandong Wu , Lin Li , Yiming Niu , Bingsen Zhang , Botao Qiao , Junhu Wang . Construction of sintering-resistant gold catalysts via ascorbic-acid inducing strong metal-support interactions. Chinese Chemical Letters, 2025, 36(4): 110608-. doi: 10.1016/j.cclet.2024.110608
5. [5]
  Ying Chen , Xingyuan Xia , Lei Tian , Mengying Yin , Ling-Ling Zheng , Qian Fu , Daishe Wu , Jian-Ping Zou . Constructing built-in electric field via CuO/NiO heterojunction for electrocatalytic reduction of nitrate at low concentrations to ammonia. Chinese Chemical Letters, 2024, 35(12): 109789-. doi: 10.1016/j.cclet.2024.109789
6. [6]
  Ting Xie , Xun He , Lang He , Kai Dong , Yongchao Yao , Zhengwei Cai , Xuwei Liu , Xiaoya Fan , Tengyue Li , Dongdong Zheng , Shengjun Sun , Luming Li , Wei Chu , Asmaa Farouk , Mohamed S. Hamdy , Chenggang Xu , Qingquan Kong , Xuping Sun . CoSe₂ nanowire array enabled highly efficient electrocatalytic reduction of nitrate for ammonia synthesis. Chinese Chemical Letters, 2024, 35(11): 110005-. doi: 10.1016/j.cclet.2024.110005
7. [7]
  Hong-Rui Li , Xia Kang , Rui Gao , Miao-Miao Shi , Bo Bi , Ze-Yu Chen , Jun-Min Yan . Interfacial interactions of Cu/MnOOH enhance ammonia synthesis from electrochemical nitrate reduction. Chinese Chemical Letters, 2025, 36(2): 109958-. doi: 10.1016/j.cclet.2024.109958
8. [8]
  Xue Zhao , Mengshan Chen , Dan Wang , Haoran Zhang , Guangzhi Hu , Yingtang Zhou . Ultrafine nano-copper derived from dopamine polymerization & synchronous adsorption achieve electrochemical purification of nitrate to ammonia in complex water environments. Chinese Chemical Letters, 2024, 35(8): 109327-. doi: 10.1016/j.cclet.2023.109327
9. [9]
  Sajid Mahmood , Haiyan Wang , Fang Chen , Yijun Zhong , Yong Hu . Recent progress and prospects of electrolytes for electrocatalytic nitrogen reduction toward ammonia. Chinese Chemical Letters, 2024, 35(4): 108550-. doi: 10.1016/j.cclet.2023.108550
10. [10]
  Yiwen Xu , Chaozheng He , Chenxu Zhao , Ling Fu . Single-atom Ti doping on S-vacancy two-dimensional CrS₂ as a catalyst for ammonia synthesis: A DFT study. Chinese Chemical Letters, 2025, 36(4): 109797-. doi: 10.1016/j.cclet.2024.109797
11. [11]
  Luyan Shi , Ke Zhu , Yuting Yang , Qinrui Liang , Qimin Peng , Shuqing Zhou , Tayirjan Taylor Isimjan , Xiulin Yang . Phytic acid-derivative Co₂B-CoPO_x coralloidal structure with delicate boron vacancy for enhanced hydrogen generation from sodium borohydride. Chinese Chemical Letters, 2024, 35(4): 109222-. doi: 10.1016/j.cclet.2023.109222
12. [12]
  Feibin Wei , Yongfang Rao , Yu Huang , Wei Wang , Hui Mei . The new challenges for the development of NH₃-SCR catalysts under new situation of energy transition in power generation industry. Chinese Chemical Letters, 2024, 35(6): 108931-. doi: 10.1016/j.cclet.2023.108931
13. [13]
  Jianjun Fang , Kunchen Xie , Yongli Song , Kangyi Zhang , Fei Xu , Xiaoze Shi , Ming Ren , Minzhi Zhan , Hai Lin , Luyi Yang , Shunning Li , Feng Pan . Break the capacity limit of Li4Ti5O12 anodes through oxygen vacancy engineering. Chinese Journal of Structural Chemistry, 2025, 44(2): 100504-100504. doi: 10.1016/j.cjsc.2024.100504
14. [14]
  Tianbo Jia , Lili Wang , Zhouhao Zhu , Baikang Zhu , Yingtang Zhou , Guoxing Zhu , Mingshan Zhu , Hengcong Tao . Modulating the degree of O vacancy defects to achieve selective control of electrochemical CO₂ reduction products. Chinese Chemical Letters, 2024, 35(5): 108692-. doi: 10.1016/j.cclet.2023.108692
15. [15]
  Kunsong Hu , Yulong Zhang , Jiayi Zhu , Jinhua Mai , Gang Liu , Manoj Krishna Sugumar , Xinhua Liu , Feng Zhan , Rui Tan . Nano-engineered catalysts for high-performance oxygen reduction reaction. Chinese Chemical Letters, 2024, 35(10): 109423-. doi: 10.1016/j.cclet.2023.109423
16. [16]
  Jialin Cai , Yizhe Chen , Ruiwen Zhang , Cheng Yuan , Zeyu Jin , Yongting Chen , Shiming Zhang , Jiujun Zhang . Interfacial Pt-N coordination for promoting oxygen reduction reaction. Chinese Chemical Letters, 2025, 36(2): 110255-. doi: 10.1016/j.cclet.2024.110255
17. [17]
  Yizhe Chen , Yuzhou Jiao , Liangyu Sun , Cheng Yuan , Qian Shen , Peng Li , Shiming Zhang , Jiujun Zhang . Nonmetallic phosphorus alloying to regulate the oxygen reduction mechanisms of platinum catalyst. Chinese Chemical Letters, 2025, 36(4): 110789-. doi: 10.1016/j.cclet.2024.110789
18. [18]
  Shuqi Yu , Yu Yang , Keisuke Kuroda , Jian Pu , Rui Guo , Li-An Hou . Selective removal of Cr(Ⅵ) using polyvinylpyrrolidone and polyacrylamide co-modified MoS₂ composites by adsorption combined with reduction. Chinese Chemical Letters, 2024, 35(6): 109130-. doi: 10.1016/j.cclet.2023.109130
19. [19]
  Yan Zhu , Jia Liu , Meiheng Lv , Tingting Wang , Dongxiang Zhang , Rong Shang , Xin-Dong Jiang , Jianjun Du , Guiling Wang . Heavy-atom-free orthogonal configurative dye 1,7-di-anthra-aza-BODIPY for singlet oxygen generation. Chinese Chemical Letters, 2024, 35(10): 109446-. doi: 10.1016/j.cclet.2023.109446
20. [20]
  Yan Wang , Huixin Chen , Fuda Yu , Shanyue Wei , Jinhui Song , Qianfeng He , Yiming Xie , Miaoliang Huang , Canzhong Lu . Oxygen self-doping pyrolyzed polyacrylic acid as sulfur host with physical/chemical adsorption dual function for lithium-sulfur batteries. Chinese Chemical Letters, 2024, 35(7): 109001-. doi: 10.1016/j.cclet.2023.109001

Get Citation

PDF

XML

Metrics

PDF Downloads(6)
Abstract views(796)
HTML views(45)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Selective electroreduction of nitrate to ammonia via NbWO6 perovskite nanosheets with oxygen vacancy

Metrics

通讯作者: 陈斌, bchen63@163.com

Selective electroreduction of nitrate to ammonia via NbWO₆ perovskite nanosheets with oxygen vacancy