Citation: Wenjuan Yang, Yating Zhu, Junjun Li, Zheng Chen, Farhat Nosheen, Qitao Zhang, Zhicheng Zhang. Understanding the dehydrogenation mechanism over iron nanoparticles catalysts based on density functional theory[J]. Chinese Chemical Letters, ;2021, 32(1): 286-290. doi: 10.1016/j.cclet.2020.10.040 shu

Understanding the dehydrogenation mechanism over iron nanoparticles catalysts based on density functional theory

Wenjuan Yang ^{a, c} ,
Yating Zhu ^b ,
Junjun Li ^b ,
Zheng Chen ^d ,
Farhat Nosheen ^e ,
Qitao Zhang ^{a, *,} ,
Zhicheng Zhang ^{b, *,}

a.
SZU-NUS Collaborative Innovation Center for Optoelectronic Science & Technology, International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, China
b.
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072, China
c.
Hanshan Normal University, Chaozhou 521041, China
d.
Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Key Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241000, China
e.
Department of Chemistry, Division of Science & Technology, University of Education, Lahore, Pakistan

qitao-zhang@szu.edu.cn

zczhang19@tju.edu.cn

Received Date: 29 September 2020
Revised Date: 21 October 2020
Accepted Date: 23 October 2020
Available Online: 28 October 2020

Figures(4)

The conversion of chemical feedstock materials into high value-added products accompanied with dehydrogenation is of great value in the chemical industry. However, the catalytic dehydrogenation reaction is inhibited by a limited number of expensive noble metal catalysts and lacks understanding of dehydrogenation mechanism. Here, we report the use of heterogeneous non-noble metal iron nanoparticles (NPs) incorporated mesoporous nitrogen-doped carbon to investigate the dehydrogenation mechanism based on experiment observation and density functional theory (DFT) method. Fe NPs catalyst displays excellent performance in the dehydrogenation of 1, 2, 3, 4-tetrahydroquinoline (THQ) with 100% selectivity and 100% conversion for 10-12 h at room temperature. The calculated adsorption energy implies that THQ prefers to adsorb on Fe NPs as compared with absence of Fe NPs. What is more, the energy barrier of transition state is relatively low, illustrating the dehydrogenation is feasible. This work provides an atomic scale mechanism guidance for the catalytic dehydrogenation reaction and points out the direction for the design of new catalysts.
- Dehydrogenation mechanism,
- Fe nanoparticles,
- Density functional theory,
- Transition states,
- 1, 2, 3, 4-Tetrahydroquinoline,
- Theoretical calculations
1. [1]
  Y. Men, J. Su, X. Wang, et al., Chin. Chem. Lett. 30(2019) 634-637. doi: 10.1016/j.cclet.2018.11.010
2. [2]
  Z. Wang, E. Li, Z. He, J. Chen, Y. Huang, Acta Phys. Chim. Sin. 35(2019) 906-912. doi: 10.3866/PKU.WHXB201811038
3. [3]
  Z. Zhang, B. Xu, X. Wang, Chem. Soc. Rev. 43(2014) 7870-7886. doi: 10.1039/C3CS60389J
4. [4]
  Y. Wu, Z. Chen, W.C. Cheong, et al., Chem. Sci. 10(2019) 5345-5352. doi: 10.1039/C9SC00475K
5. [5]
  I. Muthukrishnan, V. Sridharan, J.C. Menendez, Chem. Rev. 119(2019) 5057-5191. doi: 10.1021/acs.chemrev.8b00567
6. [6]
  B. Yan, J. Sheng, B. Qiu, D. Wang, A. Lu, Sci. Sin. Chim. 50(2020) 832. doi: 10.1360/SSC-2020-0014
7. [7]
  F. Chen, S. Zhao, T. Yang, et al., Acta Phys. Chim. Sin. 35(2019) 1422-1423. doi: 10.3866/PKU.WHXB201907026
8. [8]
  T. Mitsudome, Y. Mikami, H. Funai, et al., Angew. Chem. Int. Ed. 47(2008) 138-141. doi: 10.1002/anie.200703161
9. [9]
  Z. Li, F. Zhai, H. Qiu, et al., Rare Met. 39(2020) 383-391. doi: 10.1007/s12598-016-0711-x
10. [10]
  Y. Yu, X. Wang, C. Liu, et al., J. Energy Chem. 40(2020) 212. doi: 10.1016/j.jechem.2019.04.017
11. [11]
  A.M.S. Pembere, C. Cui, H. Wu, Z. Luo, Chin. Chem. Lett. 30(2019) 1000-1004. doi: 10.1016/j.cclet.2018.12.019
12. [12]
  F. Nosheen, N. Wasfi, S. Aslam, et al., Nanoscale 12(2020) 4219-4237. doi: 10.1039/C9NR09557H
13. [13]
  K. Wu, Acta Phys. Chim. Sin. 35(2019) 349-350. doi: 10.3866/PKU.WHXB201805023
14. [14]
  M. Liu, Acta Phys. Chim. Sin. 35(2019) 1041-1042. doi: 10.3866/PKU.WHXB201905045
15. [15]
  J. Zhang, C. Zheng, M. Zhang, et al., Nano Res. 13(2020) 3082-3087. doi: 10.1007/s12274-020-2977-4
16. [16]
  Y. Han, Z. Wang, R. Xu, et al., Angew. Chem. Int. Ed. 57(2018) 11262-11266. doi: 10.1002/anie.201805467
17. [17]
  H. Wei, X. Liu, A. Wang, et al., Nat. Commun. 5(2014) 5634. doi: 10.1038/ncomms6634
18. [18]
  Z. Chen, W. Yang, Y. Wu, et al., Nano Res. 13(2020) 3075-3081. doi: 10.1007/s12274-020-2975-6
19. [19]
  G. Jaiswal, V.G. Landge, D. Jagadeesan, E. Balaraman, Nat. Commun. 8(2017) 2147. doi: 10.1038/s41467-017-01603-3
20. [20]
  J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77(1996) 3865-3868. doi: 10.1103/PhysRevLett.77.3865
21. [21]
  G. Kresse, J. Furthmüller, Phys. Rev. B 54(1996) 11169-11186. doi: 10.1103/PhysRevB.54.11169
22. [22]
  B. Qiao, A. Wang, X. Yang, et al., Nat. Chem. 3(2011) 634-641. doi: 10.1038/nchem.1095
23. [23]
  G. Rollmann, Phys. Rev. B 69(2004) 165107. doi: 10.1103/PhysRevB.69.165107
24. [24]
  J.J. Tang, B. Liu, J. Phys. Chem. C 120(2016) 6642-6650. doi: 10.1021/acs.jpcc.6b00374
25. [25]
  Z. Chen, Y. Mao, J. Chen, et al., ACS Catal. 7(2017) 4281-4290. doi: 10.1021/acscatal.7b00541
26. [26]
  G. Chen, Y. Zhao, G. Fu, et al., Science 344(2014) 495-499. doi: 10.1126/science.1252553
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]
  Jin Li , Xin Chen , Aling Chen , Zhi-Qiang Wang , Dengsong Zhang . Theoretical insight into the active sites for chlorobenzene oxidation: From phosphate to M₃ clusters. Chinese Chemical Letters, 2025, 36(8): 110527-. doi: 10.1016/j.cclet.2024.110527
3. [3]
  Zhen Liu , Zhi-Yuan Ren , Chen Yang , Xiangyi Shao , Li Chen , Xin Li . Asymmetric alkenylation reaction of benzoxazinones with diarylethylenes catalyzed by B(C₆F₅)₃/chiral phosphoric acid. Chinese Chemical Letters, 2024, 35(5): 108939-. doi: 10.1016/j.cclet.2023.108939
4. [4]
  Teng Wang , Jiachun Cao , Juan Li , Didi Li , Zhimin Ao . A novel photocatalytic mechanism of volatile organic compounds degradation on BaTiO₃ under visible light: Photo-electrons transfer from photocatalyst to pollutant. Chinese Chemical Letters, 2025, 36(3): 110078-. doi: 10.1016/j.cclet.2024.110078
5. [5]
  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
6. [6]
  Xu Huang , Kai-Yin Wu , Chao Su , Lei Yang , Bei-Bei Xiao . Metal-organic framework Cu-BTC for overall water splitting: A density functional theory study. Chinese Chemical Letters, 2025, 36(4): 109720-. doi: 10.1016/j.cclet.2024.109720
7. [7]
  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
8. [8]
  Mianfeng Li , Haozhi Wang , Zijun Yang , Zexiang Yin , Yuan Liu , Yingmei Bian , Yang Wang , Xuerong Zheng , Yida Deng . Synergistic enhancement of alkaline hydrogen evolution reaction by role of Ni-Fe LDH introducing frustrated Lewis pairs via vacancy-engineered. Chinese Chemical Letters, 2025, 36(3): 110199-. doi: 10.1016/j.cclet.2024.110199
9. [9]
  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
10. [10]
  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
11. [11]
  Chaozheng He , Menghui Xi , Chenxu Zhao , Ran Wang , Ling Fu , Jinrong Huo . Highly N₂ dissociation catalyst: Ir(100) and Ir(110) surfaces. Chinese Chemical Letters, 2025, 36(3): 109671-. doi: 10.1016/j.cclet.2024.109671
12. [12]
  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
13. [13]
  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
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]
  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
17. [17]
  Yubang Liu , Jiaxin Lin , Huayu Liang , Yinwu Li , Zhuofeng Ke . Computational insights into three-centre four-electron bridging hydride bond in boryl type PBP-M dihydride complexes^{✰ ✩}. Chinese Chemical Letters, 2025, 36(5): 110291-. doi: 10.1016/j.cclet.2024.110291
18. [18]
  Yanhui Lu , Chengang Pei , Wenqiang Li , Qing Liu , Huan Pang , Xu Yu . Tailoring active sites of cerium and nitrogen Co-doped rhenium disulfide for enhanced hydrogen evolution reaction. Chinese Chemical Letters, 2025, 36(12): 111646-. doi: 10.1016/j.cclet.2025.111646
19. [19]
  Min Jie Wang , Jiao Yang , Lishan Peng , Yongjie Bai , Zehui Liu , Xiaoliang Yang , Huijuan Lu , Bingjie Zhou , Ningtao Jiang , Guoxu He , Han-Ming Zhang , Liwei Mi , Yonghui Deng . Optimizing the size and electronic effects of core-shell heterostructures via well-constructed Ru clusters encapsulated in N-doped carbon layers. Chinese Chemical Letters, 2025, 36(12): 110573-. doi: 10.1016/j.cclet.2024.110573
20. [20]
  Wei Sun , Yongjing Wang , Kun Xiang , Saishuai Bai , Haitao Wang , Jing Zou , Arramel , Jizhou Jiang . CoP Decorated on Ti₃C₂T_x MXene Nanocomposites as Robust Electrocatalyst for Hydrogen Evolution Reaction. Acta Physico-Chimica Sinica, 2024, 40(8): 2308015-0. doi: 10.3866/PKU.WHXB202308015

Get Citation

PDF

XML

Metrics

PDF Downloads(6)
Abstract views(1725)
HTML views(199)

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