Citation: Zhenfei Tang, Yunwu Zhang, Zhiyuan Yang, Haifeng Yuan, Tong Wu, Yue Li, Guixiang Zhang, Xingzhi Wang, Bin Chang, Dehui Sun, Hong Liu, Lili Zhao, Weijia Zhou. Iron-doping regulated light absorption and active sites in LiTaO₃ single crystal for photocatalytic nitrogen reduction[J]. Chinese Chemical Letters, ;2025, 36(3): 110107. doi: 10.1016/j.cclet.2024.110107 shu

Iron-doping regulated light absorption and active sites in LiTaO₃ single crystal for photocatalytic nitrogen reduction

Zhenfei Tang ^{a, 1} ,
Yunwu Zhang ^{a, 1} ,
Zhiyuan Yang ^c ,
Haifeng Yuan ^a ,
Tong Wu ^a ,
Yue Li ^a ,
Guixiang Zhang ^a ,
Xingzhi Wang ^a ,
Bin Chang ^a ,
Dehui Sun ^a ,
Hong Liu ^{a, b} ,
Lili Zhao ^{a, *,} ,
Weijia Zhou ^{a, *,}

a.
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, University of Jinan, Ji’nan 250022, China
b.
State Key Laboratory of Crystal Materials, Shandong University, Ji’nan 250100, China
c.
Jinan Institute of Quantum Technology, Ji’nan 250101, China

ifc_zhaoll@ujn.edu.cn

ifc_zhouwj@ujn.edu.cn

Received Date: 25 January 2024
Revised Date: 8 May 2024
Accepted Date: 11 June 2024
Available Online: 12 June 2024

Figures(4)

In contrast to research on active sites in nanomaterials, lithium tantalate single crystals, known for their exceptional optical properties and long-range ordered lattice structure, present a promising avenue for in-depth exploration of photocatalytic reaction systems with fewer constraints imposed by surface chemistry. Typically, the isotropy of a specific facet provides a perfect support for studying heteroatom doping. Herein, this work delves into the intrinsic catalytic sites for photocatalytic nitrogen fixation in iron-doped lithium tantalate single crystals. The presence of iron not only modifies the electronic structure of lithium tantalate, improving its light absorption capacity, but also functions as an active site for the nitrogen adsorption and activation. The photocatalytic ammonia production rate of the iron-doped lithium tantalate in pure water is maximum 26.95 µg cm⁻² h⁻¹, which is three times higher than that of undoped lithium tantalate. The combination of first-principles simulations with in situ characterizations confirms that iron doping promotes the rate-determining step and changes the pathway of hydrogenation to associative alternating. This study provides a new perspective on in-depth investigation of intrinsic catalytic active sites in photocatalysis and other catalytic processes.
- Nitrogen reduction,
- Photocatalysis,
- Fe doping,
- Single crystal,
- Lithium tantalate crystal
1. [1]
  D.E. Canfield, A.N. Glazer, P.G. Falkowski, Science 330 (2010) 192–196. doi: 10.1126/science.1186120
2. [2]
  H. Wang, J. Si, T. Zhang, et al., Appl. Catal. B: Environ. 270 (2020) 118892. doi: 10.1016/j.apcatb.2020.118892
3. [3]
  C. Bin, H. Yuan, L. Li, et al., Appl. Catal. B: Environ. 320 (2023) 119622.
4. [4]
  B. Chang, Z. Cao, Y. Ren, et al., ACS Nano 18 (2023) 288–298. doi: 10.37015/audt.2023.220024
5. [5]
  Y. Liu, Y. Xue, L. Hui, et al., Nano Energy 89 (2021) 106333. doi: 10.1016/j.nanoen.2021.106333
6. [6]
  B. Sun, Z. Liang, Y. Qian, et al., ACS Appl. Mater. Interfaces. 12 (2020) 7257–7269. doi: 10.1021/acsami.9b20767
7. [7]
  D. Ripepi, R. Zaffaroni, H. Schreuders, et al., ACS Energy Lett. 6 (2021) 3817–3823. doi: 10.1021/acsenergylett.1c01568
8. [8]
  B. Chang, L. Li, D. Shi, et al., Appl. Catal. B: Environ. 283 (2021) 119622. doi: 10.1016/j.apcatb.2020.119622
9. [9]
  Z.K. Shen, M. Cheng, Y.J. Yuan, et al., Appl. Catal. B: Environ. 295 (2021) 120274. doi: 10.1016/j.apcatb.2021.120274
10. [10]
  Y. Zhao, Y. Zhao, G.I.N. Waterhouse, et al., Adv. Mater. 29 (2017) 1703828. doi: 10.1002/adma.201703828
11. [11]
  S. Zhang, Y. Zhao, R. Shi, et al., Adv. Energy Mater. 10 (2020) 1901973. doi: 10.1002/aenm.201901973
12. [12]
  D. Li, Y. Zhao, Y. Miao, et al., Adv. Mater. 34 (2022) 2207793. doi: 10.1002/adma.202207793
13. [13]
  N. Zhang, A. Jalil, D. Wu, et al., J. Am. Chem. Soc. 140 (2018) 9434–9443. doi: 10.1021/jacs.8b02076
14. [14]
  W. Zhao, J. Zhang, X. Zhu, et al., Appl. Catal. B: Environ. 144 (2014) 468–477. doi: 10.1016/j.apcatb.2013.07.047
15. [15]
  Q. Meng, C. Lv, J. Sun, et al., Appl. Catal. B: Environ. 256 (2019) 117781. doi: 10.1016/j.apcatb.2019.117781
16. [16]
  Q. Song, C. Sun, Z. Wang, et al., Mater. Today Phys. 21 (2021) 100563. doi: 10.1016/j.mtphys.2021.100563
17. [17]
  Y. Bo, H. Wang, Y. Lin, et al., Angew. Chem. Int. Ed. 60 (2021) 16085–16092. doi: 10.1002/anie.202104001
18. [18]
  B. Jia, Y. Zhao, X. Zhang, Chin. Sci. Bull. 55 (2010) 11–15. doi: 10.1007/s11434-009-0600-x
19. [19]
  L. Wan, C. Wu, Y. Yuan, et al., App. Surf. Sci. 622 (2023) 156978. doi: 10.1016/j.apsusc.2023.156978
20. [20]
  E. Trevisanello, R. Ruess, G. Conforto, et al., Adv. Energy Mater. 11 (2021) 2003400. doi: 10.1002/aenm.202003400
21. [21]
  F. Zhang, S. Xi, G. Lin, et al., Adv. Mater. 31 (2018) 1806552.
22. [22]
  W. Zhao, L. Zou, L. Zhang, et al., Small 18 (2022) 2107357. doi: 10.1002/smll.202107357
23. [23]
  L. Wu, F. Su, T. Liu, et al., J. Am. Chem. Soc. 144 (2022) 20620–20629. doi: 10.1021/jacs.2c07313
24. [24]
  X. Deng, R. Zhang, K. Zhou, et al., Energy Environ. Mater. 6 (2022) e12331.
25. [25]
  X. Wang, T. Li, R. Yu, et al., J. Mater. Chem. A 4 (2016) 8682–8689. doi: 10.1039/C6TA02039A
26. [26]
  X.X. Gong, M. Fang, G.T. Fei, et al., RSC Adv. 5 (2015) 31615–31621. doi: 10.1039/C5RA03209A
27. [27]
  R. Hu, Y. Zhang, Y. Zhao, et al., Chem. Eng. J. 392 (2020) 124807. doi: 10.1016/j.cej.2020.124807
28. [28]
  A.V. Yatsenko, M.N. Palatnikov, N.V. Sidorov, Crystallogr. 64 (2019) 36–40. doi: 10.1134/s1063774519010310
29. [29]
  X. Xiao, Q. Xu, S. Liang, et al., RSC Adv. 12 (2022) 19091–19100. doi: 10.1039/d2ra02775e
30. [30]
  S.D. Villalobos Mendoza, J.T. Holguín Momaca, J.T. Elizalde Galindo, et al., Crystals 10 (2020) 41–46. doi: 10.3390/cryst10010041
31. [31]
  J.E. Sosa-Márquez, L. Zamarrón-Montes, S.F. Olive-Méndez, et al., J, Am. Ceram. 105 (2022) 5956–5965. doi: 10.1111/jace.18530
32. [32]
  L. Shi, Y. Kong, W. Yan, et al., Solid State Commun. 135 (2005) 251–256. doi: 10.1016/j.ssc.2005.04.024
33. [33]
  s.m. kostritskii, p. bourson, m. aillerie, et al., Appl. Phys. B 135 (2005) 251–256.
34. [34]
  V.S. Gorelik, N.V. Sidorov, A.I. Vodchits, et al., Phys. Wave Phenom. 25 (2017) 10–19. doi: 10.3103/S1541308X17010022
35. [35]
  L. Zhao, T. Dong, J. Du, et al., Sol. RRL 5 (2020) 2000415.
36. [36]
  H. Liu, L. Zhao, J. Yu, et al., Chem. Eng. J. 436 (2022) 131673. doi: 10.1016/j.cej.2021.131673
37. [37]
  S. Wu, Z. Chen, W. Yue, et al., ACS Catal. 11 (2021) 4362–4371. doi: 10.1021/acscatal.1c00072
38. [38]
  H. Li, S. Gu, Z. Sun, et al., J. Mater. Chem. A 8 (2020) 13038–13048. doi: 10.1039/d0ta04251j
39. [39]
  H. Li, M. Xia, B. Chong, et al., ACS Catal. 12 (2022) 10361–10372. doi: 10.1021/acscatal.2c02282
40. [40]
  S. Shang, W. Xiong, C. Yang, et al., ACS Nano 15 (2021) 9670–9678. doi: 10.1021/acsnano.0c10947
41. [41]
  T. Liu, L. Sun, Z. Cao, et al., J. Alloys Compd. 962 (2023) 171181. doi: 10.1016/j.jallcom.2023.171181
42. [42]
  Y. Shen, J. Shou, L. Chen, et al., Appl. Catal. A: Gen. 643 (2022) 118739. doi: 10.1016/j.apcata.2022.118739
43. [43]
  K. Li, C. Sun, Z. Chen, et al., Chem. Eng. J. 429 (2022) 132440. doi: 10.1016/j.cej.2021.132440
44. [44]
  T. Wang, J. Liu, P. Wu, et al., J. Mater. Chem. A 8 (2020) 16590–16598. doi: 10.1039/c9ta13902h
45. [45]
  Y. Zhao, F. Li, W. Li, et al., Angew. Chem. Int. Ed. 60 (2021) 20331–20341. doi: 10.1002/anie.202104918
46. [46]
  Y. Zhao, Y. Zhao, R. Shi, et al., Adv. Mater. 31 (2019) 1806482. doi: 10.1002/adma.201806482
47. [47]
  G. Dong, X. Huang, Y. Bi, Angew. Chem. Int. Ed. 61 (2022) e202204271. doi: 10.1002/anie.202204271
48. [48]
  Z. Lu, S.E. Saji, J. Langley, et al., Appl. Catal. B: Environ. 294 (2021) 120240. doi: 10.1016/j.apcatb.2021.120240
49. [49]
  Y. Zhang, J. Di, X. Qian, et al., Appl. Catal. B: Environ. 299 (2021) 120680. doi: 10.1016/j.apcatb.2021.120680
1. [1]
  Min Chen , Boyu Peng , Xuyun Guo , Ye Zhu , Hanying Li . Polyethylene interfacial dielectric layer for organic semiconductor single crystal based field-effect transistors. Chinese Chemical Letters, 2024, 35(4): 109051-. doi: 10.1016/j.cclet.2023.109051
2. [2]
  Qiang Zhang , Weiran Gong , Huinan Che , Bin Liu , Yanhui Ao . S doping induces to promoted spatial separation of charge carriers on carbon nitride for efficiently photocatalytic degradation of atrazine. Chinese Journal of Structural Chemistry, 2023, 42(12): 100205-100205. doi: 10.1016/j.cjsc.2023.100205
3. [3]
  Ziruo Zhou , Wenyu Guo , Tingyu Yang , Dandan Zheng , Yuanxing Fang , Xiahui Lin , Yidong Hou , Guigang Zhang , Sibo Wang . Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(3): 100245-100245. doi: 10.1016/j.cjsc.2024.100245
4. [4]
  Jiaqi Ma , Lan Li , Yiming Zhang , Jinjie Qian , Xusheng Wang . Covalent organic frameworks: Synthesis, structures, characterizations and progress of photocatalytic reduction of CO2. Chinese Journal of Structural Chemistry, 2024, 43(12): 100466-100466. doi: 10.1016/j.cjsc.2024.100466
5. [5]
  Jiangqi Ning , Junhan Huang , Yuhang Liu , Yanlei Chen , Qing Niu , Qingqing Lin , Yajun He , Zheyuan Liu , Yan Yu , Liuyi Li . Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2 reduction by targeted electron transport. Chinese Journal of Structural Chemistry, 2024, 43(12): 100453-100453. doi: 10.1016/j.cjsc.2024.100453
6. [6]
  Yan Fan , Jiao Tan , Cuijuan Zou , Xuliang Hu , Xing Feng , Xin-Long Ni . Unprecedented stepwise electron transfer and photocatalysis in supramolecular assembly derived hybrid single-layer two-dimensional nanosheets in water. Chinese Chemical Letters, 2025, 36(4): 110101-. doi: 10.1016/j.cclet.2024.110101
7. [7]
  Ruiheng Liang , Huizhong Wu , Zhongzheng Hu , Ge Song , Xuyang Zhang , Omotayo A. Arotiba , Minghua Zhou . Hierarchical Fe-Bi/Bi₇O₉I₃/OVs microspheres coupled with natural air diffusion electrode to achieve efficient heterogeneous visible-light-driven photoelectro-Fenton degradation of tetracycline without aeration. Chinese Chemical Letters, 2025, 36(4): 110136-. doi: 10.1016/j.cclet.2024.110136
8. [8]
  Fabrice Nelly Habarugira , Ducheng Yao , Wei Miao , Chengcheng Chu , Zhong Chen , Shun Mao . Synergy of sodium doping and nitrogen defects in carbon nitride for promoted photocatalytic synthesis of hydrogen peroxide. Chinese Chemical Letters, 2024, 35(8): 109886-. doi: 10.1016/j.cclet.2024.109886
9. [9]
  Zhen Shi , Wei Jin , Yuhang Sun , Xu Li , Liang Mao , Xiaoyan Cai , Zaizhu Lou . Interface charge separation in Cu2CoSnS4/ZnIn2S4 heterojunction for boosting photocatalytic hydrogen production. Chinese Journal of Structural Chemistry, 2023, 42(12): 100201-100201. doi: 10.1016/j.cjsc.2023.100201
10. [10]
  Weixu Li , Yuexin Wang , Lin Li , Xinyi Huang , Mengdi Liu , Bo Gui , Xianjun Lang , Cheng Wang . Promoting energy transfer pathway in porphyrin-based sp2 carbon-conjugated covalent organic frameworks for selective photocatalytic oxidation of sulfide. Chinese Journal of Structural Chemistry, 2024, 43(7): 100299-100299. doi: 10.1016/j.cjsc.2024.100299
11. [11]
  Mengjun Zhao , Yuhao Guo , Na Li , Tingjiang Yan . Deciphering the structural evolution and real active ingredients of iron oxides in photocatalytic CO2 hydrogenation. Chinese Journal of Structural Chemistry, 2024, 43(8): 100348-100348. doi: 10.1016/j.cjsc.2024.100348
12. [12]
  Yanghanbin Zhang , Dongxiao Wen , Wei Sun , Jiahe Peng , Dezhong Yu , Xin Li , Yang Qu , Jizhou Jiang . State-of-the-art evolution of g-C3N4-based photocatalytic applications: A critical review. Chinese Journal of Structural Chemistry, 2024, 43(12): 100469-100469. doi: 10.1016/j.cjsc.2024.100469
13. [13]
  Tianhao Li , Wenguang Tu , Zhigang Zou . In situ photocatalytically enhanced thermogalvanic cells for electricity and hydrogen production. Chinese Journal of Structural Chemistry, 2024, 43(1): 100195-100195. doi: 10.1016/j.cjsc.2023.100195
14. [14]
  Guixu Pan , Zhiling Xia , Ning Wang , Hejia Sun , Zhaoqi Guo , Yunfeng Li , Xin Li . Preparation of high-efficient donor-π-acceptor system with crystalline g-C3N4 as charge transfer module for enhanced photocatalytic hydrogen evolution. Chinese Journal of Structural Chemistry, 2024, 43(12): 100463-100463. doi: 10.1016/j.cjsc.2024.100463
15. [15]
  Yan Wang , Jiaqi Zhang , Xiaofeng Wu , Sibo Wang , Masakazu Anpo , Yuanxing Fang . Elucidating oxygen evolution and reduction mechanisms in nitrogen-doped carbon-based photocatalysts. Chinese Chemical Letters, 2025, 36(2): 110439-. doi: 10.1016/j.cclet.2024.110439
16. [16]
  Chunhui Zhang , Jie Wang , Jieyang Zhan , Runmin Yang , Guanggang Gao , Jiayuan Zhang , Linlin Fan , Mengqi Wang , Hong Liu . Highly sensitive hydrazine detection through a novel Raman scattering quenching mechanism enabled by a crystalline and noble metal–free polyoxometalate substrate. Chinese Chemical Letters, 2025, 36(3): 109719-. doi: 10.1016/j.cclet.2024.109719
17. [17]
  Yue Pan , Wenping Si , Yahao Li , Haotian Tan , Ji Liang , Feng Hou . Promoting exciton dissociation by metal ion modification in polymeric carbon nitride for photocatalysis. Chinese Chemical Letters, 2024, 35(12): 109877-. doi: 10.1016/j.cclet.2024.109877
18. [18]
  Jia-Cheng Hou , Wei Cai , Hong-Tao Ji , Li-Juan Ou , Wei-Min He . Recent advances in semi-heterogenous photocatalysis in organic synthesis. Chinese Chemical Letters, 2025, 36(2): 110469-. doi: 10.1016/j.cclet.2024.110469
19. [19]
  Chaoqun Ma , Yuebo Wang , Ning Han , Rongzhen Zhang , Hui Liu , Xiaofeng Sun , Lingbao Xing . Carbon dot-based artificial light-harvesting systems with sequential energy transfer and white light emission for photocatalysis. Chinese Chemical Letters, 2024, 35(4): 108632-. doi: 10.1016/j.cclet.2023.108632
20. [20]
  Jing Wang , Zenghui Li , Xiaoyang Liu , Bochao Su , Honghong Gong , Chao Feng , Guoping Li , Gang He , Bin Rao . Fine-tuning redox ability of arylene-bridged bis(benzimidazolium) for electrochromism and visible-light photocatalysis. Chinese Chemical Letters, 2024, 35(9): 109473-. doi: 10.1016/j.cclet.2023.109473

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(72)
HTML views(7)

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

Iron-doping regulated light absorption and active sites in LiTaO3 single crystal for photocatalytic nitrogen reduction

Metrics

通讯作者: 陈斌, bchen63@163.com

Iron-doping regulated light absorption and active sites in LiTaO₃ single crystal for photocatalytic nitrogen reduction