Citation: Xu-Hui Yue, Xiang-Wen Zhang, Hui-Min He, Lei Qiao, Zhong-Ming Sun. Synthesis, chemical bonding and reactivity of new medium-sized polyarsenides[J]. Chinese Chemical Letters, ;2024, 35(7): 108907. doi: 10.1016/j.cclet.2023.108907 shu

Synthesis, chemical bonding and reactivity of new medium-sized polyarsenides

Xu-Hui Yue ^a ,
Xiang-Wen Zhang ^a ,
Hui-Min He ^{b, *,} ,
Lei Qiao ^a ,
Zhong-Ming Sun ^{a, *,}

a.
State Key Laboratory of Element-Organic Chemistry, Tianjin Key Lab for Institution Rare Earth Materials and Applications, School of Materials Science and Engineering, Nankai University, Tianjin 300350, China
b.
Department of Physics, Institute of Computational and Applied Physics, Taiyuan Normal University, Jinzhong 030619, China

hehm@tynu.edu.cn

sunlab@nankai.edu.cn

Received Date: 9 July 2023
Revised Date: 29 July 2023
Accepted Date: 7 August 2023
Available Online: 8 August 2023

Figures(8)

Gaining an understanding of the growth mechanism from single atoms to clusters and bulk materials continues to present a challenge. Thus, it is important to explore the evolving trends of clusters in the structure and properties during the size evolution. In this work, we report the synthesis and characterization of two medium-sized chain-like polyarsenic anions. [As₂₁]^3– represents a trimeric example of polyarsenic anion assembled through oxidative coupling of As₇^3– anions. The anion As₁₈^4– included in [As₁₈Mo₂(CO)₈]^4– is regarded as formed by two realgar-type As₈ subunits connected by a dinuclear As-As dumbbell. The As₁₈ cluster was previously predicted by theory, and this is the first time successfully synthesized using wet chemistry method. Besides, small-sized polyarsenides As₂^2– and As₁₀^2– were found in compound [K(18-crown-6)]₃[As₁₀]_0.5[As₄{Mo(CO)₃}₂]_0.5·2en. Among these, the former exhibits coordination with metal atoms. Single-crystal X-ray diffraction combined with quantum chemical calculations revealed the formation of double bonded As₂^2– stabilized by metal carbonyl groups. This work demonstrates a novel synthetic approach for the preparation of new polyarsenides and highlights their intriguing bonding characteristics, laying the foundation for the synthesis of such compounds and paving the way for their potential applications.
- Polyarsenide,
- Zintl anions,
- Chain-like cluster,
- DFT calculations,
- AdNDP
1. [1]
  H.L. Xu, N.V. Tkachenko, D.W. Szczepanik, et al., Nat. Commun. 13 (2022) 2149. doi: 10.1038/s41467-022-29626-5
2. [2]
  X.H. Yue, W.X. Chen, T. Yang, et al., Nat. Synth. 2 (2023) 423–429. doi: 10.1038/s44160-023-00247-0
3. [3]
  M.J. Strumolo, D.B. Eremin, S. Wang, et al., Inorg. Chem. 62 (2023) 6197–6201. doi: 10.1021/acs.inorgchem.3c00370
4. [4]
  F. Guérin, D. Richeson, Inorg. Chem. 34 (1995) 2793–2794. doi: 10.1021/ic00115a002
5. [5]
  R.S.P. Turbervill, J.M. Goicoechea, Chem. Rev. 114 (2014) 10807–10828. doi: 10.1021/cr500387w
6. [6]
  F. Kraus, N. Korber, Inorg. Chem. 45 (2006) 1117–1123. doi: 10.1021/ic0514445
7. [7]
  T. Hanauer, F. Kraus, M. Reil, N. Korber, Monatsh. Chem. 137 (2006) 147–156. doi: 10.1007/s00706-005-0399-3
8. [8]
  F. Kraus, T. Hanauer, N. Korber, Angew. Chem. Int. Ed. 44 (2005) 7200–7204. doi: 10.1002/anie.200502535
9. [9]
  T. Hanauer, M. Grothe, M. Reil, N. Korber, Helv. Chim. Acta 88 (2005) 950–961. doi: 10.1002/hlca.200590088
10. [10]
  A.W. Castleman, S.N. Khanna, A. Sen, et al., Nano. Lett. 7 (2007) 2734–2741. doi: 10.1021/nl071224j
11. [11]
  A. Hinz, J.M. Goicoechea, Angew. Chem. Int. Ed. 55 (2016) 8536–8541. doi: 10.1002/anie.201602310
12. [12]
  C.H.E. Belin, J. Am. Chem. Soc. 102 (1980) 6036–6040. doi: 10.1021/ja00539a010
13. [13]
  T. Hanauer, J.C. Aschenbrenner, N. Korber, Inorg. Chem. 45 (2006) 6723–6727. doi: 10.1021/ic060418j
14. [14]
  R.C. Haushalter, B.W. Eichhorn, A.L. Rheingold, S.J. Geib, J. Chem. Soc. Chem. Commun. (1988) 1027–1028.
15. [15]
  V. Miluykov, A. Kataev, O. Sinyashin, et al., Z. Anorg. Allg. Chem. 632 (2006) 1728–1732. doi: 10.1002/zaac.200600108
16. [16]
  N. Korber, Phosphorus Sulfur Silicon Relat. Elem. 124 (1997) 339–346. doi: 10.1080/10426509708545639
17. [17]
  M. Baudler, D. Düster, Z. Naturforsch. 42b (1987) 335–336. doi: 10.1515/znb-1987-0314
18. [18]
  H.G. von Schnering, V. Manriquez, W. Hönle, Angew. Chem. Int. Ed. 20 (1981) 594–595. doi: 10.1002/anie.198105941
19. [19]
  M. Baudler, D. Düster, K. Langerbeins, et al., Angew. Chem. Int. Ed. 23 (1984) 317–318. doi: 10.1002/anie.198403171
20. [20]
  M. Baudler, R. Heumüller, D. Düster, et al., Z. Anorg. Allg. Chem. 518 (1984) 7–13. doi: 10.1002/zaac.19845181102
21. [21]
  S.S. Du, J.Y. Hu, Z.Q. Chai, et al., Chin. J. Chem. 37 (2019) 71–75. doi: 10.1002/cjoc.201800482
22. [22]
  M. Seidl, G. Balázs, M. Scheer, Chem. Rev. 119 (2019) 8406–8434. doi: 10.1021/acs.chemrev.8b00713
23. [23]
  J.J. Zhao, Phys. Rev. B 73 (2006) 115418. doi: 10.1103/PhysRevB.73.115418
24. [24]
  A.J. Karttunen, M. Linnolahti, T.A. Pakkanen, ChemPhysChem 8 (2007) 2373–2378. doi: 10.1002/cphc.200700376
25. [25]
  H. Thurn, H. Kerbs, Angew. Chem. Int. Ed. 5 (1966) 1047–1048.
26. [26]
  M. Ruck, D. Hoppe, B. Wahl, et al., Angew. Chem. Int. Ed. 44 (2005) 7616–7619. doi: 10.1002/anie.200503017
27. [27]
  M. Häser, U. Schneider, R. Ahlrichs, J. Am. Chem. Soc. 114 (1992) 9559–9568. doi: 10.1021/ja00050a040
28. [28]
  S. Böcker, M. Häser, Z. Anorg. Allg. Chem. 621 (1995) 258–286. doi: 10.1002/zaac.19956210215
29. [29]
  W.Q. Zhang, Z.S. Li, J.E. McGrady, Z.M. Sun, Angew. Chem. Int. Ed. 62 (2023) e202217316. doi: 10.1002/anie.202217316
30. [30]
  W.Q. Zhang, N.V. Tkachenko, L. Qiao, A.I. Boldyrev, Z.M. Sun, Chin. J. Chem. 40 (2022) 65–70. doi: 10.1002/cjoc.202100682
31. [31]
  N.V. Tkachenko, W.X. Chen, H.W.T. Morgan, et al., Chem. Commun. 58 (2022) 6223–6226. doi: 10.1039/d2cc01745h
32. [32]
  Y.N. Yang, L. Qiao, Z.M. Sun, Chin. Chem. Lett. 34 (2023) 107207. doi: 10.1016/j.cclet.2022.02.013
33. [33]
  Y.S. Huang, D. Chen, J. Zhu, Z.M. Sun, Chin. Chem. Lett. 33 (2022) 2139–2142. doi: 10.1016/j.cclet.2021.08.038
34. [34]
  J.J. Mrowca, T.J. Katz, J. Am. Chem. Soc. 88 (1966) 4012–4015. doi: 10.1021/ja00969a021
35. [35]
  P. Pyykkö, J. Phys. Chem. A 119 (2015) 2326–2337. doi: 10.1021/jp5065819
36. [36]
  S. Mandal, A.C. Reber, M. Qian, et al., Dalton Trans. 41 (2012) 12365–12377. doi: 10.1039/c2dt31286g
37. [37]
  M. Kaas, N. Korber, Z. Anorg. Allg. Chem. 643 (2017) 1331–1334. doi: 10.1002/zaac.201700171
38. [38]
  C. Schoo, S. Bestgen, A. Egeberg, et al., Angew. Chem. Int. Ed. 58 (2019) 1–5. doi: 10.1002/anie.201813481
39. [39]
  C. Schwarzmaier, A.Y. Timoshkin, G. Balázs, M. Scheer, Angew. Chem. Int. Ed. 53 (2014) 9077–9081. doi: 10.1002/anie.201404653
40. [40]
  S. Mandal, M. Qian, A.C. Reber, et al., J. Phys. Chem. C. 115 (2011) 23704–23710. doi: 10.1021/jp207268x
41. [41]
  B.W. Eichhorn, S.P. Mattamana, D.R. Gardner, et al., J. Am. Chem. Soc. 120 (1998) 9708–9709. doi: 10.1021/ja9820700
42. [42]
  H.P. Ruan, L.L. Wang, Z.Y. Li, L. Xu, Dalton Trans. 46 (2017) 7219–7222. doi: 10.1039/C7DT01135K
43. [43]
  P.J. Sullivan, A.L. Rheingold, Organometallics 1 (1982) 1547–1549. doi: 10.1021/om00071a032
44. [44]
  N. Reinfandt, C. Schoo, L. Dütsch, et al., Chem. Eur. J. 27 (2021) 3974–3978. doi: 10.1002/chem.202003905
45. [45]
  L. Qiao, C. Zhang, C.C. Shu, et al., J. Am. Chem. Soc. 142 (2020) 13288–13293. doi: 10.1021/jacs.0c04815
46. [46]
  D.Y. Zubarev, A.I. Boldyrev, Phys. Chem. Chem. Phys. 10 (2008) 5207–5217. doi: 10.1039/b804083d
47. [47]
  T. Lu, F.W.M. Chen, J. Comput. Chem. 33 (2012) 580–592. doi: 10.1002/jcc.22885
1. [1]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
2. [2]
  Yutong Xiong , Ting Meng , Wendi Luo , Bin Tu , Shuai Wang , Qingdao Zeng . Molecular conformational effects on co-assembly systems of low-symmetric carboxylic acids investigated by scanning tunneling microscopy. Chinese Journal of Structural Chemistry, 2025, 44(2): 100511-100511. doi: 10.1016/j.cjsc.2025.100511
3. [3]
  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
4. [4]
  Ronghao Zhao , Yifan Liang , Mengyao Shi , Rongxiu Zhu , Dongju Zhang . Investigation into the Mechanism and Migratory Aptitude of Typical Pinacol Rearrangement Reactions: A Research-Oriented Computational Chemistry Experiment. University Chemistry, 2024, 39(4): 305-313. doi: 10.3866/PKU.DXHX202309101
5. [5]
  Jiabo Huang , Quanxin Li , Zhongyan Cao , Li Dang , Shaofei Ni . Elucidating the Mechanism of Beckmann Rearrangement Reaction Using Quantum Chemical Calculations. University Chemistry, 2025, 40(3): 153-159. doi: 10.12461/PKU.DXHX202405172
6. [6]
  Shaohua Zhang , Liyao Liu , Yingqiao Ma , Chong-an Di . Advances in theoretical calculations of organic thermoelectric materials. Chinese Chemical Letters, 2024, 35(8): 109749-. doi: 10.1016/j.cclet.2024.109749
7. [7]
  Bingwei Wang , Yihong Ding , Xiao Tian . Benchmarking model chemistry composite calculations for vertical ionization potential of molecular systems. Chinese Chemical Letters, 2025, 36(2): 109721-. doi: 10.1016/j.cclet.2024.109721
8. [8]
  Lei Shen , Yang Zhang , Linlin Zhang , Chuanwang Liu , Zhixian Ma , Kangjiang Liang , Chengfeng Xia . Phenylhydrazone anions excitation for the photochemical carbonylation of aryl iodides with aldehydes. Chinese Chemical Letters, 2024, 35(4): 108742-. doi: 10.1016/j.cclet.2023.108742
9. [9]
  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
10. [10]
  Yinglian LI , Chengcheng ZHANG , Xinyu ZHANG , Xinyi WANG . Spin crossover in [Co(pytpy)₂]²⁺ complexes modified by organosulfonate anions. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1162-1172. doi: 10.11862/CJIC.20240087
11. [11]
  Rong-Nan Yi , Wei-Min He . Electron donor-acceptor complex enabled arylation of dithiocarbamate anions with thianthrenium salts under aqueous micellar conditions. Chinese Chemical Letters, 2024, 35(11): 110194-. doi: 10.1016/j.cclet.2024.110194
12. [12]
  Qiaojia GUO , Junkai CAI , Chunying DUAN . Effects of anions on the structural regulation of Zn-salen-modified metal-organic cage. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2203-2211. doi: 10.11862/CJIC.20240209
13. [13]
  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
14. [14]
  Tao Ban , Xi-Yang Yu , Hai-Kuo Tian , Zheng-Qing Huang , Chun-Ran Chang . One-step conversion of methane and formaldehyde to ethanol over SA-FLP dual-active-site catalysts: A DFT study. Chinese Chemical Letters, 2024, 35(4): 108549-. doi: 10.1016/j.cclet.2023.108549
15. [15]
  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
16. [16]
  Lumin Zheng , Ying Bai , Chuan Wu . Multi-electron reaction and fast Al ion diffusion of δ-MnO₂ cathode materials in rechargeable aluminum batteries via first-principle calculations. Chinese Chemical Letters, 2024, 35(4): 108589-. doi: 10.1016/j.cclet.2023.108589
17. [17]
  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
18. [18]
  Qihang Wu , Hui Wen , Wenhai Lin , Tingting Sun , Zhigang Xie . Alkyl chain engineering of boron dipyrromethenes for efficient photodynamic antibacterial treatment. Chinese Chemical Letters, 2024, 35(12): 109692-. doi: 10.1016/j.cclet.2024.109692
19. [19]
  Huiju Cao , Lei Shi . sp¹-Hybridized linear and cyclic carbon chain. Chinese Chemical Letters, 2025, 36(4): 110466-. doi: 10.1016/j.cclet.2024.110466
20. [20]
  Xianghe Kong , Xiaoli Liao , Zhenkun Huang , Lei Mei , Hongqing Wang , Kongqiu Hu , Weiqun Shi . Designed assembly of heterometallic cluster organic frameworks based on Th₆ cluster. Chinese Chemical Letters, 2024, 35(11): 109642-. doi: 10.1016/j.cclet.2024.109642

Get Citation

PDF

XML

Metrics

PDF Downloads(2)
Abstract views(265)
HTML views(3)

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