Electrochemical Pourbaix diagrams of monolayer MoSSe with different atomic ratios of chalcogens

Li Yan; Ma Xiang-Chao; Huang Xi

doi:10.7498/aps.72.20221567

Abstract

MoSSe material is a very promising photoelectric material, and its application environment is aqueous solution. However, there is no research of the electrochemical stability of MoSSe materials in aqueous solution. In this work, the Pourbaix diagrams of monolayer MoSSe with different atomic ratios of molybdenum, sulfur and selenium are constructed based on density functional theory, and the thermodynamic stabilities and electrochemical corrosion behaviors under different pH values and electrode potentials are studied. The study of the pourbaix diagram of MoSSe shows that part of the corrosion-free region of MoSSe exists within the stable region of water in the Pourbaix diagram, indicating that the MoSSe can exist stably in the water environment. Compared with alkaline solutions, MoSSe has good corrosion resistance in acidic solution and neutral solution. The Pourbaix diagram of Mo₄S₂Se₆, Mo₄S₆Se₂, Mo₄S₇Se and Mo₄SSe₇ show that in the case of high molar fraction of sulfur in monolayer MoSSe with different atomic ratios of molybdenum, sulfur and selenium, the conditions for the stable existence of materials in aqueous solution can have a larger range, and the corrosion resistance becomes better. In the case of high molar fractions of selenium in monolayer MoSSe with different atomic ratios of molybdenum, sulfur and selenium, the range of conditions for the stable existence of materials in aqueous solution becomes smaller, and the corrosion resistance becomes worse. In this work, the stabilities and corrosion behaviors of monolayer MoSSe with different atomic ratios of molybdenum, sulfur and selenium in aqueous solution are predicted, and the degradation behaviors of MoSSe materials are further explored, which can provide theoretical guidance for the application of MoSSe materials in the field of optoelectronics.

Keywords:

Authors and contacts

School of Optoelectronic Engineering, Xidian University, Xi’an 710126, China

Corresponding author: Ma Xiang-Chao, xcma@xidian.edu.cn

Funds: Project supported by the Natural Science Basic Research Program of Shaanxi Province, China (Grant No. 2022JZ-04), the State Key Development Program for the National Natural Science Foundation of China (Grant Nos. 11704298, 61904138 ) .

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References

[1]	Lu A Y, Zhu H, Xiao J, Chuu C P, Han Y, Chiu M H, Cheng C C, Yang C W, Wei K H, Yang Y, Wang Y, Sokaras D, Nordlund D, Yang P, Muller D A, Chou M Y, Zhang X, Li L J 2017 Nat. Nanotechnol. 12 744 Google Scholar
[2]	Yin W J, Liu Y, Wen B, Li X B, Chai Y F, Wei X L, Ma S, Teobaldi G 2021 Dalton Trans. 50 10252 Google Scholar
[3]	Zhang J, Jia S, Kholmanov I, Dong L, Er D, Chen W B, Guo H, Jin Z H, Shenoy V B, Shi L, Lou J 2017 ACS Nano 11 8192 Google Scholar
[4]	Paez-Ornelas J I, Ponce-Pérez R, Fernández-Escamilla H N, Hoat D M, Murillo-Bracamontes E A, Moreno-Armenta M G, Galván D H, Guerrero-Sánchez J 2021 Sci. Rep. 11 1 Google Scholar
[5]	Guan Z Y, Ni S, Hu S L 2018 J. Phys. Chem. C 122 6209 Google Scholar
[6]	Singh A, Jain M, Bhattacharya S 2021 Nanoscale Adv. 3 2837 Google Scholar
[7]	Teets T S, Nocera D G 2011 Chem. Commun. 47 9268 Google Scholar
[8]	Hansen H A, Rossmeisl J, Nørskov J K 2008 Phys. Chem. Chem. Phys. 10 3722 Google Scholar
[9]	彭少方, 张昭 1992 新疆有色金属 1 28 Peng S F, Zhang Z 1992 Xinjiang Youse Jinshu 1 28
[10]	Beverskog B, Puigdomenech I 1997 Corros. Sci. 39 969 Google Scholar
[11]	Ding R, Shang J X, Wang F H, Chen Y 2018 Comput. Mater. Sci. 143 431 Google Scholar
[12]	Huang L F, Rondinelli J M 2015 Phys. Rev. B 92 245126 Google Scholar
[13]	Dong X X, Wei B, Legut D, Zhang H J, Zhang R F 2021 Phys. Chem. Chem. Phys. 23 19602 Google Scholar
[14]	Perry S C, Gateman S M, Stephens L I, Lacasse R, Schulz R, Mauzaroll J 2019 J. Electrochem. Soc. 166 3186 Google Scholar
[15]	Bajdich M, García-Mota M, Vojvodic A, Nørskov J K, Bell A T 2013 J. Am. Chem. Soc. 135 13521 Google Scholar
[16]	Persson K A, Waldwick B, Lazic P, Ceder G 2012 Phys. Rev. B 85 235438 Google Scholar
[17]	Chen J, Selloni A 2013 J. Phys. Chem. C 117 20002 Google Scholar
[18]	Wang L, Maxisch T, Ceder G 2006 Phys. Rev. B 73 195107 Google Scholar
[19]	Zeng Z H, Chan M K Y, Zhao Z J, Kubal J, Fan D X, Greeley J 2015 J. Phys. Chem. C 119 18177 Google Scholar
[20]	Exner K S 2017 ChemElectroChem 4 3231 Google Scholar
[21]	Perdew J P, Burke K, Ernzerhof M 1998 Phys. Rev. Lett. 80 891 Google Scholar
[22]	林洪斌, 林春, 陈越, 钟克华, 张健敏, 许桂贵, 黄志高 2021 70 138201 Google Scholar Lin H B, Lin C, Chen Y, Zhong K H, Zhang J M, Xu G G, Huang Z G 2021 Acta Phys. Sin. 70 138201 Google Scholar
[23]	Zunger A, Wei S H, Ferreira L G, Bernard J E 1990 Phys. Rev. Lett. 65 353 Google Scholar
[24]	Grau-Crespo R, Hamad S, Catlow C R A, Leeuw N H D 2007 J. Phys. Condens. Matter 19 256201 Google Scholar
[25]	Sen S, Ghosh H 2016 Eur. Phys. J. B 89 277 Google Scholar
[26]	Binder K 1981 Phys. Rev. Lett. 47 693 Google Scholar
[27]	Gale J D 1997 J. Chem. Soc. Faraday Trans. 93 629 Google Scholar
[28]	Huang L F, Rondinelli J M 2015 Physical Review B 92 245126
[29]	Barry T I 1980 ACS Symp. Ser. 133 681
[30]	Lee J B 1981 Corrosion 37 467 Google Scholar
[31]	Muñoz-Portero M J, García-Antón J, Guiñón J L, Pérez-Herranz V 2009 Corros. Sci. 51 807 Google Scholar
[32]	Nikolaychuk P A, Tyurin A G 2011 Mater. Sci. 24 101
[33]	Protopopoff E, Marcus P 2012 Electrochim. Acta 63 22 Google Scholar
[34]	Wagman D D, Evans W H, Parker V B, Schemm R H, Halow I 1982 J. Phys. Chem. Ref. Data 11 2
[35]	Beverskog B, Puigdomenech I 1997 Corrosion Science 39 969
[36]	吴雄伟, 彭穗, 冯必钧, 山村朝雄, 矢野贵, 佐藤伊佐務, 刘素琴, 黄可龙 2011 无机化学学报 26 535 Wu X W, Peng S, Feng B J, Tomoo Y, Yano T, Isamu S, Liu S Q, Huang K L 2011 Chinese J. Inorg. Chem. 26 535
[37]	Gana S J, Egiebor N, Ankumah R O 2011 Mater. Sci. Appl. 2 81
[38]	Nishimoto M, Muto I, Sugawara Y, Hara N 2019 J. Electrochem. Soc. 166 3081
[39]	Choudhary L, Macdonald D D, Alfantazi A 2015 Corrosion 71 1147 Google Scholar
[40]	Alhasan R, Nasim M J, Jacob C, Gaucher C 2019 Curr. Pharmacol. Rep. 5 163 Google Scholar

Cited By

图 1 计算流程图

Figure 1. Calculation flow chart.

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图 2 MoSSe材料的Pourbaix图(图中不同颜色区域对应可能存在的物质参照表5)

Figure 2. Pourbaix diagram of MoSSe material(Refer to Table 5 for the different colored areas in the figure correspond to possible substances).

DownLoad: Full-Size Img PowerPoint

图 3 MoSSe材料在不同pH下吉布斯自由能随电极电位变化图　(a) pH = 0; (b) pH = 7; (c) pH = 14

Figure 3. Diagram of gibbs free energy variation with electrode potential variation of MoSSe material under different conditions: (a) pH = 0; (b) pH = 7; (c) pH = 14.

DownLoad: Full-Size Img PowerPoint

图 4 Mo₄S₂Se₆和Mo₄SSe₇材料的Pourbaix图(图中不同颜色区域对应可能存在的物质参照5)　(a) Mo₄S₂Se₆材料; (b) Mo₄SSe₇材料

Figure 4. Pourbaix diagram of Mo₄S₂Se₆ and Mo₄SSe₇ materials (Refer to Table 5 for the different colored areas in the figure correspond to possible substances): (a) Mo₄S₂Se₆ material; (b) Mo₄S₂Se₆ material.

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图 5 Mo₄S₂Se₆(a)和Mo₄SSe₇(b)材料在pH = 7条件下吉布斯自由能随电极电位变化图

Figure 5. Diagram of gibbs free energy variation with electrode potential variation of Mo₄S₂Se₆(a) and Mo₄SSe₇(b) materials at pH = 7

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图 6 Mo₄S₆Se₂(a)和Mo₄S₇Se (b)材料的Pourbaix图(图中不同颜色区域对应可能存在的物质参照5)

Figure 6. Pourbaix diagram of Mo₄S₆Se₂(a) and Mo₄S₇Se (b) materials (Refer to Table 5 for the different colored areas in the figure correspond to possible substances).

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图 7 不同条件下的吉布斯自由能随电极电位变化图　(a) Mo₄S₆Se₂材料在pH = 0时; (b) Mo₄S₆Se₂材料在pH = 7时; (c) Mo₄S₆Se₂材料在pH = 14时; (d) Mo₄S₇Se材料在pH = 0时; (e) Mo₄S₇Se材料在pH = 7时; (f) Mo₄S₇Se材料在pH = 14时

Figure 7. Diagram of Gibbs free energy variation with electrode potential variation under different conditions: (a) Mo₄S₆Se₂ material at pH=0; (b) Mo₄S₆Se₂ material at pH = 7; (c) Mo₄S₆Se₂ material at pH = 14; (d) Mo₄S₇Se material at pH = 0; (e) Mo₄S₇Se material at pH = 7; (f) Mo₄S₇Se material at pH = 14.

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图 8 不同材料的能带结构　(a) Mo₄S₇Se; (b) Mo₄S₆Se₂; (c) Mo₄SSe₇; (d) Mo₄S₂Se₆

Figure 8. Band structure of different materials: (a) Mo₄S₇Se; (b) Mo₄S₆Se₂; (c) Mo₄SSe₇; (d) Mo₄S₂Se₆.

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图 9 Mo₄S₇Se, Mo₄S₆Se₂, Mo₄S₂Se₆和Mo₄SSe₇材料的光吸收系数

Figure 9. Optical absorption coefficients of Mo₄S₇Se, Mo₄S₆Se₂, Mo₄SSe₇ and Mo₄S₂Se₆.

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表 1 不同比例MoSSe材料的标准化学势

Table 1. Standard chemical potential of MoSSe materials with different proportions.

物质	标准化学势 μ⁰/eV
MoSSe	–2.21
Mo₄S₂Se₆	–8.357
Mo₄S₆Se₂	–9.721
Mo₄SSe₇	–7.990
Mo₄S₇Se	–10.038

DownLoad: CSV

表 2 Mo, S和Se元素在水溶液中可能形成的离子状态物质及其标准化学势

Table 2. The possible ionic state substance of Mo, S and Se elements in aqueous solution and their standard chemical potentials.

物质	标准化学势μ⁰/eV	文献
Mo³⁺	–0.60	[30]
MoO₄^2–	–8.02	[31]
MoO₂²⁺	–4.24	[32]
S^2–	0.89	[33]
S₂^2–	0.82	[34]
SO₃^2–	–5.04	[34]
SO₄^2–	–7.72	[33]
HS^–	0.13	[33]
HSO₄^–	–7.84	[33]
HS₂O₄^–	–6.37	[35]
Se^2–	1.34	[34]
SeO₃^2–	–3.83	[34]
SeO₄^2–	–4.57	[34]
HSe^–	0.46	[34]
HSeO₃^–	–4.26	[34]
HSeO₄^–	–4.69	[34]

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表 3 Mo, S和Se元素形成的固态物质的空间群和理论化学势

Table 3. The space group and theoretical chemical potentials of solid substances formed by Mo, S and Se elements.

物质	标准化学势μ⁰/eV	空间群
Mo	0	${Im} \bar 3m$
MoO₂	–5.53	${ {{P} }{4_2}/{{mnm} } }$
MoO₃	–6.92	$P2_1/c$
S	0	$P2/c$
Se	0	$P2/c$
MoSe	–0.23	$P \bar 6 m2$
MoSe₂	–6.92	$P\bar 3 m1$
MoS₂	–2.34	$P6_3/mmc$

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表 4 Mo, S和Se元素在水溶液中可能形成的溶液状态物质及其标准化学势

Table 4. The The possible aqueous state substance of Mo, S and Se elements in aqueous solution and their standard chemical potentials.

物质	标准化学势μ⁰/eV	文献
H₂S(aq)	–0.29	[33]
H₂SO₄(aq)	–7.72	[34]
H₂Se(aq)	0.23	[34]
H₂SO₃(aq)	–4.43	[34]

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表 5 编号对照表

Table 5. Numbering reference table.

编号	物质(溶液中)
1	MoO₃ + HSO₄^– + HSeO₄^–
2	MoO₃ + HSO₄^– + SeO₄^2–
3	MoO₃ + SO₄^2– + SeO₄^2–
4	MoO₄^2– + SO₄^2– + SeO₄^2–
5	MoO₄^2– + SO₄^2– + SeO₃^2–
6	MoO₃ + SO₄^2– + SeO₃^2–
7	MoO₃ + SO₄^2– + HSeO₃^–
8	MoO₃ + SO₄^2– + H₂SeO₃
9	MoO₃ + HSO₄^– + H₂SeO₃
10	MoO₃ + HSO₄^– + Se
11	MoO₃ + SO₄^2– + Se
12	MoO₄^2– + SO₄^2– + Se
13	MoO₄^2– + SO₄^2– + HSe^–
14	MoO₄^2– + SO₄^2– + Se^2–
15	MoO₄^2– + S^2– + Se^2–
16	MoO₄^2– + S^2– + HSe^–
17	MoO₄^2– + MoSe₂ + S^2–
18	MoO₄^2– + MoSe₂ + SO₄^2–
19	MoO₃ + MoSe₂ + SO₄^2–
20	MoO₃ + MoSe₂ + HSO₄^–
21	Mo³⁺ + HSO₄^– + Se
22	Mo³⁺ + MoS₂ + Se
23	Mo³⁺ + MoSe₂ + H₂S
24	MoSSe
25	Mo + MoSe₂ + S^2–
26	Mo + MoSe₂ + HS^–
27	Mo + MoSe₂ + H₂S
28	Mo + H₂S + H₂Se
29	Mo + H₂S + HSe^–
30	Mo + HS^– + HSe^–
31	Mo + S^2– + HSe^–
32	Mo + S^2– + Se^2–
33	Mo³⁺ + MoSe₂ + HSO₄^–
34	MoO₄^2– + HSe^– + Mo₄S₅Se₃
35	Mo³⁺ + Se + Mo₄S₅Se₃
36	Mo + HSe^– + Mo₄S₅Se₃
37	Mo³⁺ + Se + Mo₄S₆Se₂
38	MoO₃ + Se + Mo₄S₅Se₃
39	Mo₄S₂Se₆
40	MoO₄^2– + MoSe₂ + HS^–
41	MoO₂ + MoSe₂ + HS^–
42	MoO₃ + MoSe₂ + HS^–
43	Mo₄SSe₇
44	Mo₄S₆Se₂
45	Mo₄S₇Se
46	Mo₄S₅Se₃

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map

[1]	Lu A Y, Zhu H, Xiao J, Chuu C P, Han Y, Chiu M H, Cheng C C, Yang C W, Wei K H, Yang Y, Wang Y, Sokaras D, Nordlund D, Yang P, Muller D A, Chou M Y, Zhang X, Li L J 2017 Nat. Nanotechnol. 12 744 Google Scholar
[2]	Yin W J, Liu Y, Wen B, Li X B, Chai Y F, Wei X L, Ma S, Teobaldi G 2021 Dalton Trans. 50 10252 Google Scholar
[3]	Zhang J, Jia S, Kholmanov I, Dong L, Er D, Chen W B, Guo H, Jin Z H, Shenoy V B, Shi L, Lou J 2017 ACS Nano 11 8192 Google Scholar
[4]	Paez-Ornelas J I, Ponce-Pérez R, Fernández-Escamilla H N, Hoat D M, Murillo-Bracamontes E A, Moreno-Armenta M G, Galván D H, Guerrero-Sánchez J 2021 Sci. Rep. 11 1 Google Scholar
[5]	Guan Z Y, Ni S, Hu S L 2018 J. Phys. Chem. C 122 6209 Google Scholar
[6]	Singh A, Jain M, Bhattacharya S 2021 Nanoscale Adv. 3 2837 Google Scholar
[7]	Teets T S, Nocera D G 2011 Chem. Commun. 47 9268 Google Scholar
[8]	Hansen H A, Rossmeisl J, Nørskov J K 2008 Phys. Chem. Chem. Phys. 10 3722 Google Scholar
[9]	彭少方, 张昭 1992 新疆有色金属 1 28 Peng S F, Zhang Z 1992 Xinjiang Youse Jinshu 1 28
[10]	Beverskog B, Puigdomenech I 1997 Corros. Sci. 39 969 Google Scholar
[11]	Ding R, Shang J X, Wang F H, Chen Y 2018 Comput. Mater. Sci. 143 431 Google Scholar
[12]	Huang L F, Rondinelli J M 2015 Phys. Rev. B 92 245126 Google Scholar
[13]	Dong X X, Wei B, Legut D, Zhang H J, Zhang R F 2021 Phys. Chem. Chem. Phys. 23 19602 Google Scholar
[14]	Perry S C, Gateman S M, Stephens L I, Lacasse R, Schulz R, Mauzaroll J 2019 J. Electrochem. Soc. 166 3186 Google Scholar
[15]	Bajdich M, García-Mota M, Vojvodic A, Nørskov J K, Bell A T 2013 J. Am. Chem. Soc. 135 13521 Google Scholar
[16]	Persson K A, Waldwick B, Lazic P, Ceder G 2012 Phys. Rev. B 85 235438 Google Scholar
[17]	Chen J, Selloni A 2013 J. Phys. Chem. C 117 20002 Google Scholar
[18]	Wang L, Maxisch T, Ceder G 2006 Phys. Rev. B 73 195107 Google Scholar
[19]	Zeng Z H, Chan M K Y, Zhao Z J, Kubal J, Fan D X, Greeley J 2015 J. Phys. Chem. C 119 18177 Google Scholar
[20]	Exner K S 2017 ChemElectroChem 4 3231 Google Scholar
[21]	Perdew J P, Burke K, Ernzerhof M 1998 Phys. Rev. Lett. 80 891 Google Scholar
[22]	林洪斌, 林春, 陈越, 钟克华, 张健敏, 许桂贵, 黄志高 2021 70 138201 Google Scholar Lin H B, Lin C, Chen Y, Zhong K H, Zhang J M, Xu G G, Huang Z G 2021 Acta Phys. Sin. 70 138201 Google Scholar
[23]	Zunger A, Wei S H, Ferreira L G, Bernard J E 1990 Phys. Rev. Lett. 65 353 Google Scholar
[24]	Grau-Crespo R, Hamad S, Catlow C R A, Leeuw N H D 2007 J. Phys. Condens. Matter 19 256201 Google Scholar
[25]	Sen S, Ghosh H 2016 Eur. Phys. J. B 89 277 Google Scholar
[26]	Binder K 1981 Phys. Rev. Lett. 47 693 Google Scholar
[27]	Gale J D 1997 J. Chem. Soc. Faraday Trans. 93 629 Google Scholar
[28]	Huang L F, Rondinelli J M 2015 Physical Review B 92 245126
[29]	Barry T I 1980 ACS Symp. Ser. 133 681
[30]	Lee J B 1981 Corrosion 37 467 Google Scholar
[31]	Muñoz-Portero M J, García-Antón J, Guiñón J L, Pérez-Herranz V 2009 Corros. Sci. 51 807 Google Scholar
[32]	Nikolaychuk P A, Tyurin A G 2011 Mater. Sci. 24 101
[33]	Protopopoff E, Marcus P 2012 Electrochim. Acta 63 22 Google Scholar
[34]	Wagman D D, Evans W H, Parker V B, Schemm R H, Halow I 1982 J. Phys. Chem. Ref. Data 11 2
[35]	Beverskog B, Puigdomenech I 1997 Corrosion Science 39 969
[36]	吴雄伟, 彭穗, 冯必钧, 山村朝雄, 矢野贵, 佐藤伊佐務, 刘素琴, 黄可龙 2011 无机化学学报 26 535 Wu X W, Peng S, Feng B J, Tomoo Y, Yano T, Isamu S, Liu S Q, Huang K L 2011 Chinese J. Inorg. Chem. 26 535
[37]	Gana S J, Egiebor N, Ankumah R O 2011 Mater. Sci. Appl. 2 81
[38]	Nishimoto M, Muto I, Sugawara Y, Hara N 2019 J. Electrochem. Soc. 166 3081
[39]	Choudhary L, Macdonald D D, Alfantazi A 2015 Corrosion 71 1147 Google Scholar
[40]	Alhasan R, Nasim M J, Jacob C, Gaucher C 2019 Curr. Pharmacol. Rep. 5 163 Google Scholar

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Vol. 72, Issue 4 - 2023-02-20

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