Citation: Yu Yan, Hongjiao Qu, Xiaonan Zheng, Kexin Zhao, Xiaoxiao Li, Yuan Yao, Yang Liu. Amorphous core/shell Ti-doped SnO₂ with synergistically improved N₂ adsorption/activation and electrical conductivity for electrochemical N₂ reduction[J]. Chinese Chemical Letters, ;2022, 33(10): 4655-4658. doi: 10.1016/j.cclet.2021.12.054 shu

Amorphous core/shell Ti-doped SnO₂ with synergistically improved N₂ adsorption/activation and electrical conductivity for electrochemical N₂ reduction

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150080, China

yyuan@hit.edu.cn

yang.liu@hit.edu.cn

Received Date: 30 September 2021
Revised Date: 17 December 2021
Accepted Date: 22 December 2021
Available Online: 26 December 2021

Figures(5)

Electrochemical nitrogen reduction reaction (NRR) has been considered as an appealing and sustainable method to produce ammonia from N₂ under ambient conditions, attracting increasing interest. Limited by low solubility of N₂ in water and high stability of NN triple bond, developing NRR electrocatalysts with both strong N₂ adsorption/activation and high electrical conductivity remain challenging. Here, we demonstrate an efficient strategy to develop NRR electrocatalyst with synergistically enhanced N₂ adsorption/activation and electrical conductivity by heteroatom doping. Combining computational and experimental study, the DFT-designed Ti-doped SnO₂ exhibits significantly enhanced NRR performance with ammonia yield rate of 13.09 µg h⁻¹ mg⁻¹ at −0.2 V vs. RHE. Particularly, the Faradaic efficiency reaches up to 42.6%, outperforming most of Sn-based electrocatalysts. The fundamental mechanism for improving NRR performance of SnO₂ by Ti doping is also revealed. Our work highlights a powerful strategy for developing high-activity electrocatalysts for NRR and beyond.
- Nitrogen reduction reaction,
- Electrocatalysts,
- Density functional theory,
- Heteroatom doping,
- Synergistical effect
1. [1]
  D. Chanda, R. Xing, T. Xu, et al., Chem. Commun. 57 (2021) 7335–7349. doi: 10.1039/d1cc01451j
2. [2]
  R. Wang, C. He, W. Chen, C. Zhao, J. Huo, Chin. Chem. Lett. 32 (2021) 3821–3824. doi: 10.1016/j.cclet.2021.05.024
3. [3]
  M.M. Shi, D. Bao, B.R. Wulan, et al., Adv. Mater. 29 (2017) 1606550. doi: 10.1002/adma.201606550
4. [4]
  M. Wang, S. Liu, T. Qian, et al., Nat. Commun. 10 (2019) 341. doi: 10.1038/s41467-018-08120-x
5. [5]
  W. Qiu, X.Y. Xie, J. Qiu, et al., Nat. Commun. 9 (2018) 3485. doi: 10.1038/s41467-018-05758-5
6. [6]
  X. Zhang, T. Wu, H. Wang, et al., ACS Catal. 9 (2019) 4609–4615. doi: 10.1021/acscatal.8b05134
7. [7]
  M. Kitano, S. Kanbara, Y. Inoue, et al., Nat. Commun. 6 (2015) 6731. doi: 10.1038/ncomms7731
8. [8]
  J. Wang, L. Yu, L. Hu, et al., Nat. Commun. 9 (2018) 1795. doi: 10.1038/s41467-018-04213-9
9. [9]
  Z. Du, J. Liang, S. Li, et al., J. Mater. Chem. A 9 (2021) 13861–13866. doi: 10.1039/d1ta02424h
10. [10]
  H. Chen, J. Liang, L. Li, et al., ACS Appl. Mater. Interfaces 13 (2021) 41715–41722. doi: 10.1021/acsami.1c11872
11. [11]
  P. Wang, Y. Ji, Q. Shao, Y. Li, X. Huang, Sci. Bull. 65 (2020) 350–358. doi: 10.1016/j.scib.2019.12.019
12. [12]
  F. He, Z. Wang, S. Wei, J. Zhao, Appl. Surf. Sci. 506 (2020) 144943. doi: 10.1016/j.apsusc.2019.144943
13. [13]
  X. Zheng, Y. Liu, Y. Yan, X. Li, Y. Yao, Chin. Chem. Lett. 33 (2022) 1455–1458. doi: 10.1016/j.cclet.2021.08.102
14. [14]
  Q. Qin, Y. Zhao, M. Schmallegger, et al., Angew. Chem. Int. Ed. 58 (2019) 13101–13106. doi: 10.1002/anie.201906056
15. [15]
  X. Zhu, S. Mou, Q. Peng, et al., J. Mater. Chem. A 8 (2020) 1545–1556. doi: 10.1039/c9ta13044f
16. [16]
  Y. Yang, M. Luo, W. Zhang, et al., Chem 4 (2018) 2054–2083. doi: 10.1016/j.chempr.2018.05.019
17. [17]
  C. Guo, J. Ran, A. Vasileff, S.Z. Qiao, Energy Environ. Sci. 11 (2018) 45–56. doi: 10.1039/C7EE02220D
18. [18]
  X.W. Lv, Y. Liu, R. Hao, W. Tian, Z.Y. Yuan, ACS Appl. Mater. Interfaces 12 (2020) 17502–17508. doi: 10.1021/acsami.0c00647
19. [19]
  K. Chu, J. Wang, Y.P. Liu, Q.Q. Li, Y.L. Guo, J. Mater. Chem. A 8 (2020) 7117–7124. doi: 10.1039/d0ta01688h
20. [20]
  Y. Tan, Y. Xu, Z. Ao, Phys. Chem. Chem. Phys. 22 (2020) 13981–13988. doi: 10.1039/d0cp01963a
21. [21]
  X. Zheng, Y. Liu, Y. Yao, Chem. Eng. J. 426 (2021) 130745. doi: 10.1016/j.cej.2021.130745
22. [22]
  X. Zheng, Y. Yao, Y. Wang, Y. Liu, Nanoscale 12 (2020) 9696–9707. doi: 10.1039/d0nr00072h
23. [23]
  D. Jiao, Y. Liu, Q. Cai, J. Zhao, J. Mater. Chem. A 9 (2021) 1240–1251. doi: 10.1039/d0ta09496j
24. [24]
  X. Liu, H. Zhou, S. Pei, S. Xie, S. You, Chem. Eng. J. 381 (2020) 122740. doi: 10.1016/j.cej.2019.122740
25. [25]
  H. Li, Z. Zhao, Q. Cai, L. Yin, J. Zhao, J. Mater. Chem. A 8 (2020) 4533–4543. doi: 10.1039/c9ta13599e
26. [26]
  L. Zhang, X. Ren, Y. Luo, et al., Chem. Commun. 54 (2018) 12966–12969. doi: 10.1039/c8cc06524a
27. [27]
  M.A. Légaré, G. Bélanger-Chabot, R.D. Dewhurst, et al., Science 359 (2018) 896–900. doi: 10.1126/science.aaq1684
28. [28]
  J. Deng, J.A. Iñiguez, C. Liu, Joule 2 (2018) 846–856. doi: 10.1016/j.joule.2018.04.014
29. [29]
  X. Cui, C. Tang, Q. Zhang, Adv. Energy Mater. 8 (2018) 1800369. doi: 10.1002/aenm.201800369
30. [30]
  L. Zhang, X. Ji, X. Ren, et al., Adv. Mater. 30 (2018) 1800191. doi: 10.1002/adma.201800191
31. [31]
  Z. Geng, Y. Liu, X. Kong, et al., Adv. Mater. 30 (2018) 1803498. doi: 10.1002/adma.201803498
32. [32]
  Y.P. Liu, Y.B. Li, H. Zhang, K. Chu, Inorg. Chem. 58 (2019) 10424–10431. doi: 10.1021/acs.inorgchem.9b01823
33. [33]
  X. Zhang, X. Huang, D. Liu, et al., Int. J. Hydrog. Energy 43 (2018) 21428–21440. doi: 10.1016/j.ijhydene.2018.09.169
34. [34]
  X. Yang, Y. Ma, Y. Liu, et al., ACS Appl. Mater. Interfaces 13 (2021) 19864–19872. doi: 10.1021/acsami.0c22623
35. [35]
  Z. Lin, C. Guo, Q. Fu, W. Song, Mater. Lett. 102-103 (2013) 47–49. doi: 10.1016/j.matlet.2013.03.104
36. [36]
  M. Motola, L. Satrapinskyy, M. Čaplovicová, et al., Appl. Surf. Sci. 434 (2018) 1257–1265. doi: 10.1016/j.apsusc.2017.11.253
37. [37]
  Y. Shang, W. Shi, R. Zhao, et al., Chin. Chem. Lett. 31 (2020) 2055–2058. doi: 10.1016/j.cclet.2020.01.009
38. [38]
  Q. Tian, W. Wei, J. Dai, et al., Appl. Catal. B Environ. 244 (2019) 45–55. doi: 10.1016/j.apcatb.2018.11.045
39. [39]
  C. Lv, C. Yan, G. Chen, et al., Angew. Chem. Int. Ed. 57 (2018) 6073–6076. doi: 10.1002/anie.201801538
40. [40]
  B. Liu, H.C. Zeng, Small 1 (2005) 566–571. doi: 10.1002/smll.200500020
41. [41]
  Y. Zhao, R. Shi, X. Bian, et al., Adv. Sci. 6 (2019) 1802109. doi: 10.1002/advs.201802109
42. [42]
  G.W. Watt, J.D. Chrisp, Anal. Chem. 24 (1952) 2006–2008. doi: 10.1021/ac60072a044
43. [43]
  X. Chen, Y.T. Liu, C. Ma, J. Yu, B. Ding, J. Mater. Chem. A 7 (2019) 22235–22241. doi: 10.1039/c9ta04382a
44. [44]
  Y.T. Liu, D. Li, J. Yu, B. Ding, Angew. Chem. Int. Ed. 58 (2019) 16439–16444. doi: 10.1002/anie.201908415
45. [45]
  K. Chu, Y.P. Liu, Y.B. Li, J. Wang, H. Zhang, ACS Appl. Mater. Interfaces 11 (2019) 31806–31815. doi: 10.1021/acsami.9b08055
46. [46]
  L. Zhang, M. Cong, X. Ding, et al., Angew. Chem. Int. Ed. 59 (2020) 10888–10893. doi: 10.1002/anie.202003518
47. [47]
  C. Chen, Y. Liu, Y. Yao, Eur. J. Inorg. Chem. 2020 (2020) 3236–3241. doi: 10.1002/ejic.202000554
1. [1]
  Yuxiang Zhang , Jia Zhao , Sen Lin . Nitrogen doping retrofits the coordination environment of copper single-atom catalysts for deep CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(11): 100415-100415. doi: 10.1016/j.cjsc.2024.100415
2. [2]
  Jiayu Huang , Kuan Chang , Qi Liu , Yameng Xie , Zhijia Song , Zhiping Zheng , Qin Kuang . Fe-N-C nanostick derived from 1D Fe-ZIFs for Electrocatalytic oxygen reduction. Chinese Journal of Structural Chemistry, 2023, 42(10): 100097-100097. doi: 10.1016/j.cjsc.2023.100097
3. [3]
  Guoliang Gao , Guangzhen Zhao , Guang Zhu , Bowen Sun , Zixu Sun , Shunli Li , Ya-Qian Lan . Recent advancements in noble-metal electrocatalysts for alkaline hydrogen evolution reaction. Chinese Chemical Letters, 2025, 36(1): 109557-. doi: 10.1016/j.cclet.2024.109557
4. [4]
  Jiajun Wang , Guolin Yi , Shengling Guo , Jianing Wang , Shujuan Li , Ke Xu , Weiyi Wang , Shulai Lei . Computational design of bimetallic TM₂@g-C₉N₄ electrocatalysts for enhanced CO reduction toward C₂ products. Chinese Chemical Letters, 2024, 35(7): 109050-. doi: 10.1016/j.cclet.2023.109050
5. [5]
  Tingting Huang , Zhuanlong Ding , Hao Liu , Ping-An Chen , Longfeng Zhao , Yuanyuan Hu , Yifan Yao , Kun Yang , Zebing Zeng . Electron-transporting boron-doped polycyclic aromatic hydrocarbons: Facile synthesis and heteroatom doping positions-modulated optoelectronic properties. Chinese Chemical Letters, 2024, 35(4): 109117-. doi: 10.1016/j.cclet.2023.109117
6. [6]
  Xiangyuan Zhao , Jinjin Wang , Jinzhao Kang , Xiaomei Wang , Hong Yu , Cheng-Feng Du . Ni nanoparticles anchoring on vacuum treated Mo2TiC2Tx MXene for enhanced hydrogen evolution activity. Chinese Journal of Structural Chemistry, 2023, 42(10): 100159-100159. doi: 10.1016/j.cjsc.2023.100159
7. [7]
  Xue Xin , Qiming Qu , Islam E. Khalil , Yuting Huang , Mo Wei , Jie Chen , Weina Zhang , Fengwei Huo , Wenjing Liu . Hetero-phase zirconia encapsulated with Au nanoparticles for boosting electrocatalytic nitrogen reduction. Chinese Chemical Letters, 2024, 35(5): 108654-. doi: 10.1016/j.cclet.2023.108654
8. [8]
  Wei Chen , Pieter Cnudde . A minireview to ketene chemistry in zeolite catalysis. Chinese Journal of Structural Chemistry, 2024, 43(11): 100412-100412. doi: 10.1016/j.cjsc.2024.100412
9. [9]
  Jiao Li , Chenyang Zhang , Chuhan Wu , Yan Liu , Xuejian Zhang , Xiao Li , Yongtao Li , Jing Sun , Zhongmin Su . Defined organic-octamolybdate crystalline superstructures derived Mo₂C@C as efficient hydrogen evolution electrocatalysts. Chinese Chemical Letters, 2024, 35(6): 108782-. doi: 10.1016/j.cclet.2023.108782
10. [10]
  Weiping Xiao , Yuhang Chen , Qin Zhao , Danil Bukhvalov , Caiqin Wang , Xiaofei Yang . Constructing the synergistic active sites of nickel bicarbonate supported Pt hierarchical nanostructure for efficient hydrogen evolution reaction. Chinese Chemical Letters, 2024, 35(12): 110176-. doi: 10.1016/j.cclet.2024.110176
11. [11]
  Lian Sun , Honglei Wang , Ming Ma , Tingting Cao , Leilei Zhang , Xingui Zhou . Shape and composition evolution of Pt and Pt₃M nanocrystals under HCl chemical etching. Chinese Chemical Letters, 2024, 35(9): 109188-. doi: 10.1016/j.cclet.2023.109188
12. [12]
  Lingling Su , Qunyan Wu , Congzhi Wang , Jianhui Lan , Weiqun Shi . Theoretical design of polyazole based ligands for the separation of Am(Ⅲ)/Eu(Ⅲ). Chinese Chemical Letters, 2024, 35(8): 109402-. doi: 10.1016/j.cclet.2023.109402
13. [13]
  Yu-Hang Li , Shuai Gao , Lu Zhang , Hanchun Chen , Chong-Chen Wang , Haodong Ji . Insights on selective Pb adsorption via O 2p orbit in UiO-66 containing rich-zirconium vacancies. Chinese Chemical Letters, 2024, 35(8): 109894-. doi: 10.1016/j.cclet.2024.109894
14. [14]
  Xin-Tong Zhao , Jin-Zhi Guo , Wen-Liang Li , Jing-Ping Zhang , Xing-Long Wu . Two-dimensional conjugated coordination polymer monolayer as anode material for lithium-ion batteries: A DFT study. Chinese Chemical Letters, 2024, 35(6): 108715-. doi: 10.1016/j.cclet.2023.108715
15. [15]
  Fanjun Kong , Yixin Ge , Shi Tao , Zhengqiu Yuan , Chen Lu , Zhida Han , Lianghao Yu , Bin Qian . Engineering and understanding SnS_0.5Se_0.5@N/S/Se triple-doped carbon nanofibers for enhanced sodium-ion batteries. Chinese Chemical Letters, 2024, 35(4): 108552-. doi: 10.1016/j.cclet.2023.108552
16. [16]
  Ze Zhang , Lei Yang , Jin-Ru Liu , Hao Hu , Jian-Li Mi , Chao Su , Bei-Bei Xiao , Zhi-Min Ao . Improved oxygen electrocatalysis at FeN₄ and CoN₄ sites via construction of axial coordination. Chinese Chemical Letters, 2025, 36(2): 110013-. doi: 10.1016/j.cclet.2024.110013
17. [17]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
18. [18]
  Yanan Zhou , Li Sheng , Lanlan Chen , Wenhua Zhang , Jinlong Yang . Axial coordinated iron-nitrogen-carbon as efficient electrocatalysts for hydrogen evolution and oxygen redox reactions. Chinese Chemical Letters, 2025, 36(1): 109588-. doi: 10.1016/j.cclet.2024.109588
19. [19]
  Qin Cheng , Ming Huang , Qingqing Ye , Bangwei Deng , Fan Dong . Indium-based electrocatalysts for CO₂ reduction to C1 products. Chinese Chemical Letters, 2024, 35(6): 109112-. doi: 10.1016/j.cclet.2023.109112
20. [20]
  Qiyan Wu , Ruixin Zhou , Zhangyi Yao , Tanyuan Wang , Qing Li . Effective approaches for enhancing the stability of ruthenium-based electrocatalysts towards acidic oxygen evolution reaction. Chinese Chemical Letters, 2024, 35(10): 109416-. doi: 10.1016/j.cclet.2023.109416

Get Citation

PDF

XML

Metrics

PDF Downloads(2)
Abstract views(423)
HTML views(46)

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

Amorphous core/shell Ti-doped SnO2 with synergistically improved N2 adsorption/activation and electrical conductivity for electrochemical N2 reduction

Metrics

通讯作者: 陈斌, bchen63@163.com

Amorphous core/shell Ti-doped SnO₂ with synergistically improved N₂ adsorption/activation and electrical conductivity for electrochemical N₂ reduction