Citation: Jiazhi Wang, Kai Li, Qi Hao, Dongxue Liu, Xinbo Zhang. Electroreduction NO to NH₃ over single metal atom anchored on pyrrole type defective graphene: A DFT study[J]. Chinese Chemical Letters, ;2023, 34(5): 107567. doi: 10.1016/j.cclet.2022.05.081 shu

Electroreduction NO to NH₃ over single metal atom anchored on pyrrole type defective graphene: A DFT study

Jiazhi Wang ^{a, b} ,
Kai Li ^a ,
Qi Hao ^{a, c} ,
Dongxue Liu ^c ,
Xinbo Zhang ^{a, b, *,}

a.
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
b.
University of Science and Technology of China, Hefei 230026, China
c.
Key Laboratory of Automobile Materials, Ministry of Education, Jilin University, Changchun 130022, China

xbzhang@ciac.ac.cn

Received Date: 30 April 2022
Revised Date: 5 May 2022
Accepted Date: 26 May 2022
Available Online: 29 May 2022

Figures(5)

Electrochemical is considered an attractive approach to recycling the pollution NO (NORR) and producing the valuable NH₃, which could simultaneously solve the two challenging problems, i.e., NO removal and NH₃ synthesis. Current research efforts focus less on NORR due to the lack of effective catalysts. Herein, based on DFT calculation, we try to explore effective pyrrole-type TM-N₄ (TM = V, Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Ta) catalysts for achieving the direct NORR. Among the investigated systems, Fe-N₄ exhibits excellent catalytic activity and high NH₃ selectivity. Moreover, the free energy of adsorption of N^* has been proposed as a descriptor to predict and screen the effective TM-N₄ catalyst for NORR and the crystal orbital halmilton populations (COHP) is used to describe the intrinsic relationship between metal atoms and the adsorption free energy of N^* intermediate. This work has provided a theoretical picture of TM-N₄ catalyzing NO to NH₃, which will establish guidelines for the rational design of NORR catalysts and other electrochemical reactions.
- DFT calculation,
- Pyrrole-type,
- Descriptor,
- NORR,
- COHP
1. [1]
  K. Li, D.J. Jacob, H. Liao, et al., Nat. Geosci. 12 (2019) 906–910. doi: 10.1038/s41561-019-0464-x
2. [2]
  H. He, Y. Wang, Q. Ma, et al., Sci. Rep. 4 (2014) 4172. doi: 10.1038/srep04172
3. [3]
  Z. Liu, S. Ihl Woo, Catal. Rev. 48 (2006) 43–89. doi: 10.1080/01614940500439891
4. [4]
  C. Liu, J.W. Shi, C. Gao, C. Niu, Appl. Catal. A 522 (2016) 54–69. doi: 10.1016/j.apcata.2016.04.023
5. [5]
  L. Han, S. Cai, M. Gao, et al., Chem. Rev. 19 (2019) 10916–10976. doi: 10.1021/acs.chemrev.9b00202
6. [6]
  J.H. Montoya, C. Tsai, A. Vojvodic, J.K. Nørskov, ChemSusChem 8 (2015) 2180–2186. doi: 10.1002/cssc.201500322
7. [7]
  C. Ling, X. Niu, Q. Li, A. Du, J. Wang, J. Am. Chem. Soc. 140 (2018) 14161–14168. doi: 10.1021/jacs.8b07472
8. [8]
  K. Chu, Y. Luo, P. Shen, et al., Adv. Energy Mater. 12 (2022) 2103022. doi: 10.1002/aenm.202103022
9. [9]
  Y. Yang, Y. Wang, X. Wang, et al., Adv. Mater. Interfaces 9 (2022) 2101842. doi: 10.1002/admi.202101842
10. [10]
  L. Zhang, J. Liang, Y. Wang, et al., Angew. Chem. Int. Ed. 60 (2021) 25263–25268. doi: 10.1002/anie.202110879
11. [11]
  Z. Wang, J. Zhao, J. Wang, C.R. Cabrera, Z. Chen, J. Mater. Chem. A 6 (2018) 7547–7556. doi: 10.1039/C8TA00875B
12. [12]
  H. Niu, Z. Zhang, X. Wang, et al., Small 17 (2021) e2102396. doi: 10.1002/smll.202102396
13. [13]
  H. Fei, J. Dong, M.J. Arellano-Jimenez, et al., Nat. Commun. 6 (2015) 8668. doi: 10.1038/ncomms9668
14. [14]
  T. Mineva, I. Matanovic, P. Atanassov, et al., ACS Catal. 9 (2019) 9359–9371. doi: 10.1021/acscatal.9b02586
15. [15]
  I. Vinogradov, S. Singh, H. Lyle, et al., Nat. Mater. 21 (2022) 88–94. doi: 10.1038/s41563-021-01118-9
16. [16]
  S. Chen, W.H. Li, W. Jiang, et al., Angew. Chem. Int. Ed. 61 (2022) e202114450.
17. [17]
  M. Li, H. Wang, W. Luo, et al., Adv. Mater. 32 (2020) e2001848. doi: 10.1002/adma.202001848
18. [18]
  L. Zhong, L. Zhang, S. Li, ACS Mater. Lett. 3 (2020) 110–120.
19. [19]
  S. Ding, Z. Lyu, H. Zhong, et al., Small 17 (2021) e2004454. doi: 10.1002/smll.202004454
20. [20]
  L. Zong, K. Fan, W. Wu, et al., Adv. Funct. Mater. 31 (2021) 2104864. doi: 10.1002/adfm.202104864
21. [21]
  J. Li, Y.F. Jiang, Q. Wang, et al., Nat. Commun. 12 (2021) 6806. doi: 10.1038/s41467-021-27143-5
22. [22]
  L. Yan, L. Xie, X.L. Wu, et al., Carbon Energy 3 (2021) 856–865. doi: 10.1002/cey2.135
23. [23]
  R. Christensen, H.A. Hansen, C.F. Dickens, J.K. Nørskov, T. Vegge, J. Phys. Chem. C 120 (2016) 24910–24916. doi: 10.1021/acs.jpcc.6b09141
24. [24]
  J. Zhao, Z. Chen, J. Am. Chem. Soc. 139 (2017) 12480–12487. doi: 10.1021/jacs.7b05213
25. [25]
  W. Yang, Z. Gao, X. Liu, et al., Fuel 243 (2019) 262–270. doi: 10.1016/j.fuel.2019.01.125
26. [26]
  Q. Wu, W. Wei, X. Lv, et al., J. Phys. Chem. C 123 (2019) 31043–31049. doi: 10.1021/acs.jpcc.9b08827
27. [27]
  J. Long, S. Chen, Y. Zhang, et al., Angew. Chem. Int. Ed. 59 (2020) 9711–9718. doi: 10.1002/anie.202002337
28. [28]
  Q. Wu, H. Wang, S. Shen, et al., J. Mater. Chem. A 9 (2021) 5434–5441. doi: 10.1039/D0TA11209G
29. [29]
  J.C. Liu, X.L. Ma, Y. Li, et al., Nat. Commun. 9 (2018) 1610. doi: 10.1038/s41467-018-03795-8
30. [30]
  C. Wei, Y. Sun, G.G. Scherer, et al., J. Am. Chem. Soc. 142 (2020) 7765–7775. doi: 10.1021/jacs.9b12005
1. [1]
  Dan-Ying Xing , Xiao-Dan Zhao , Chuan-Shu He , Bo Lai . Kinetic study and DFT calculation on the tetracycline abatement by peracetic acid. Chinese Chemical Letters, 2024, 35(9): 109436-. doi: 10.1016/j.cclet.2023.109436
2. [2]
  Haibin Yang , Duowen Ma , Yang Li , Qinghe Zhao , Feng Pan , Shisheng Zheng , Zirui Lou . Mo doped Ru-based cluster to promote alkaline hydrogen evolution with ultra-low Ru loading. Chinese Journal of Structural Chemistry, 2023, 42(11): 100031-100031. doi: 10.1016/j.cjsc.2023.100031
3. [3]
  Jing Wang , Zhongliao Wang , Jinfeng Zhang , Kai Dai . Single-layer crystalline triazine-based organic framework photocatalysts with different linking groups for H2O2 production. Chinese Journal of Structural Chemistry, 2023, 42(12): 100202-100202. doi: 10.1016/j.cjsc.2023.100202
4. [4]
  Guangchang Yang , Shenglong Yang , Jinlian Yu , Yishun Xie , Chunlei Tan , Feiyan Lai , Qianqian Jin , Hongqiang Wang , Xiaohui Zhang . Regulating local chemical environment in O3-type layered sodium oxides by dual-site Mg²⁺/B³⁺ substitution achieves durable and high-rate cathode. Chinese Chemical Letters, 2024, 35(9): 109722-. doi: 10.1016/j.cclet.2024.109722
5. [5]
  Linshan Peng , Qihang Peng , Tianxiang Jin , Zhirong Liu , Yong Qian . Highly efficient capture of thorium ion by citric acid-modified chitosan gels from aqueous solution. Chinese Chemical Letters, 2024, 35(5): 108891-. doi: 10.1016/j.cclet.2023.108891
6. [6]
  Ya-Nan Yang , Zi-Sheng Li , Sourav Mondal , Lei Qiao , Cui-Cui Wang , Wen-Juan Tian , Zhong-Ming Sun , John E. McGrady . Metal-metal bonds in Zintl clusters: Synthesis, structure and bonding in [Fe₂Sn₄Bi₈]^3– and [Cr₂Sb₁₂]^3–. Chinese Chemical Letters, 2024, 35(8): 109048-. doi: 10.1016/j.cclet.2023.109048
7. [7]
  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
8. [8]
  Ruonan Yang , Jiajia Li , Dongmei Zhang , Xiuqi Zhang , Xia Li , Han Yu , Zhanhu Guo , Chuanxin Hou , Gang Lian , Feng Dang . Grain-refining Co_0.85Se@CNT cathode catalyst with promoted Li₂O₂ growth kinetics for lithium-oxygen batteries. Chinese Chemical Letters, 2024, 35(12): 109595-. doi: 10.1016/j.cclet.2024.109595
9. [9]
  Xiangyu Chen , Aihao Xu , Dong Wei , Fang Huang , Junjie Ma , Huibing He , Jing Xu . Atomic cerium-doped CuO_x catalysts for efficient electrocatalytic CO₂ reduction to CH₄. Chinese Chemical Letters, 2025, 36(1): 110175-. doi: 10.1016/j.cclet.2024.110175
10. [10]
  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
11. [11]
  Yan Guo , Hongtao Bian , Le Yu , Jiani Ma , Yu Fang . Photochemical reaction mechanism of benzophenone protected guanosine at N7 position. Chinese Chemical Letters, 2025, 36(3): 109971-. doi: 10.1016/j.cclet.2024.109971
12. [12]
  He Yao , Wenhao Ji , Yi Feng , Chunbo Qian , Chengguang Yue , Yue Wang , Shouying Huang , Mei-Yan Wang , Xinbin Ma . Copper-catalyzed and biphosphine ligand controlled 3,4-boracarboxylation of 1,3-dienes with carbon dioxide. Chinese Chemical Letters, 2025, 36(4): 110076-. doi: 10.1016/j.cclet.2024.110076
13. [13]
  Quan Xu , Ye-Qing Du , Pan-Pan Chen , Yili Sun , Ze-Nan Yang , Hui Zhang , Bencan Tang , Hong Wang , Jia Li , Yue-Wei Guo , Xu-Wen Li . Computation assisted chemical study of photo-induced late-stage skeleton transformation of marine natural products towards new scaffolds with biological functions. Chinese Chemical Letters, 2025, 36(5): 110141-. doi: 10.1016/j.cclet.2024.110141
14. [14]
  Chunyan Yang , Qiuyu Rong , Fengyin Shi , Menghan Cao , Guie Li , Yanjun Xin , Wen Zhang , Guangshan Zhang . Rationally designed S-scheme heterojunction of BiOCl/g-C₃N₄ for photodegradation of sulfamerazine: Mechanism insights, degradation pathways and DFT calculation. Chinese Chemical Letters, 2024, 35(12): 109767-. doi: 10.1016/j.cclet.2024.109767
15. [15]
  Qian Huang , Zhaowei Li , Jianing Zhao , Ao Yu . Quantum Chemical Calculations Reveal the Details Below the Experimental Phenomenon. University Chemistry, 2024, 39(3): 395-400. doi: 10.3866/PKU.DXHX202309018
16. [16]
  Xiumei LI , Yanju HUANG , Bo LIU , Yaru PAN . Syntheses, crystal structures, and quantum chemistry calculation of two Ni(Ⅱ) coordination polymers. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 2031-2039. doi: 10.11862/CJIC.20240109
17. [17]
  Anjing Liao , Wei Sun , Yaming Liu , Han Yan , Zhi Xia , Jian Wu . Pyrrole and pyrrolidine analogs: The promising scaffold in discovery of pesticides. Chinese Chemical Letters, 2025, 36(3): 110094-. doi: 10.1016/j.cclet.2024.110094
18. [18]
  Zhuwen Wei , Jiayan Chen , Congzhen Xie , Yang Chen , Shifa Zhu . Divergent de novo construction of α-functionalized pyrrole derivatives via coarctate reaction. Chinese Chemical Letters, 2024, 35(12): 109677-. doi: 10.1016/j.cclet.2024.109677
19. [19]
  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
20. [20]
  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

Get Citation

PDF

XML

Metrics

PDF Downloads(6)
Abstract views(1029)
HTML views(70)

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

Electroreduction NO to NH3 over single metal atom anchored on pyrrole type defective graphene: A DFT study

Metrics

通讯作者: 陈斌, bchen63@163.com

Electroreduction NO to NH₃ over single metal atom anchored on pyrrole type defective graphene: A DFT study