Organic proton-type ionic liquid, two-dimensional perovskite pure-phase quantum well film, preparation method and use thereof

Patent metadata

Field	Value
Publication number	US-12492161-B2
Application number	US-202117784003-A
Country	US
Kind code	B2
Filing date	Aug 24, 2021
Priority date	Aug 25, 2020
Publication date	Dec 9, 2025
Grant date	Dec 9, 2025

Abstract

Disclosed are an organic proton-type ionic liquid, a film with a two-dimensional perovskite pure-phase quantum well structure, a preparation method and use thereof. The organic proton-type ionic liquid has a chemical formula of RNH 3 + ·CH 3 COO − or RNH 3 + ·RCOO − , where R represents an alkyl group of C4-8 or a phenyl group, preferably, the chemical formula thereof is CH 3 (CH 2 ) 3 NH 3 + ·CH 3 COO − . The organic proton-type ionic liquid can be used to prepare perovskite material, the perovskite film prepared thereby can form a pure-phase single quantum well, with a crystal grain size therein reaching a level of micrometers or even millimeters.

First claim

What is claimed is:

1 . A method for preparing a film with a two-dimensional perovskite pure-phase quantum well structure, the two-dimensional perovskite pure-phase quantum well structure having a chemical formula of A a B b M m X x , where A is a carbon chain organic cation, and a-value ranges from 0 to 2.5; B is an amine group-containing monovalent cation, b-value satisfies 0≤b<m+1, and m is any natural number and satisfies m−1≥0; M is a divalent metal cation; and X is one or more of halogen ion, carboxylate ion and thiocyanate ion, and x-value satisfies 3m−1<x≤3m+1;
the method comprising:
1) Adding BX to a DMSO solution to prepare a DMSO mixture with a BX mass fraction of 1-35%;
2) Adding an organic proton-type ionic liquid to the DMSO mixture prepared in step 1), mixing, stirring at 25° C. for 2 hours, and then adding MX 2 thereto;
3) Then adding 1600 μL of a DMF reagent, heating to 65° C. and stirring until dissolved, and cooling to room temperature to obtain a mixed solution; and
4) Spin-coating the mixed solution prepared in step 3) while heating onto a surface of a glass substrate in air with a humidity of 20%-80%, and maintaining at a temperature of 25° C.-250° C. to obtain the film with the two-dimensional perovskite pure-phase quantum well structure;
wherein a molar ratio of the organic proton-type ionic liquid, the BX, and the MX 2 is 2:m+1:m;
the BX is a compound salt of a monovalent cation;
the MX 2 is a compound formed by a divalent metal cation and an X ion;
the organic proton-type ionic liquid serves as a source of A, and has a chemical formula of RNH 3 + ·CH 3 COO − where R represents an alkyl group of C4-8 or a phenyl group, or a chemical formula of RNH 3 + ·RCOO − where R represents an alkyl group of C4-8 or a phenyl group; and
the A corresponds to RNH 3 + of the organic proton-type ionic liquid.

2 . The method according to claim 1 , wherein the compound salt of the monovalent cation is one or more selected from the group consisting of: a compound salt of methylamine ion, a compound salt of formamidine ion, and a compound salt of guanidine ion.

3 . The method according to claim 1 , wherein an addition amount of the DMF reagent in step 3) is 5-50 times an addition amount of the organic proton-type ionic liquid in volume.

4 . The method according to claim 1 , wherein the spin-coating the mixed solution prepared in step 3) while heating comprises:
heating the glass substrate to a temperature of 80° C.-100° C., setting a spin-coating speed to 500-1000 rpm/min and performing spin-coating for 5-10 s, then setting a spin-coating speed to 2000-6000 rpm/min and performing spin-coating for 5-10 s, continuously heating the substrate between the two spin-coating steps, covering a film obtained after the spin-coating with a petri dish with a diameter of 100 mm, and then subjecting the film to heat-treatment at a temperature of 80° C. to 120° C. for 5-10 minutes.

5 . The method according to claim 1 , comprising:
1) Providing butylamine acetate ionic liquid as the organic proton-type ionic liquid, methyl ammonium iodide as the BX and lead iodide powder as the MX 2 ; 2) Adding the methyl ammonium iodide to the DMSO solution to prepare a DMSO mixture with a mass fraction of the methyl ammonium iodide of 1-35 wt %; 3) Adding the butylamine acetate ionic liquid to the DMSO mixture prepared in step 2), mixing, stirring at 25° C. for 2 hours, and then adding the lead iodide powder thereto; then adding the DMF reagent, heating to 65° C., stirring until dissolved, and cooling to room temperature to obtain a mixed solution; and 4) Spin-coating the mixed solution prepared in step 3) while heating onto a surface of a glass substrate in air with a humidity of 20%-80%, and maintaining the temperature at 25° C. to 250° C., wherein a molar ratio of the butylamine acetate ionic liquid, the methyl ammonium iodide, and the lead iodide powder is 2:4:3.

6 . The method according to claim 1 , wherein the organic proton-type ionic liquid is a butylamine acetate ionic liquid, having a chemical formula of CH 3 (CH 2 ) 3 NH 3 + ·CH 3 COO.

7 . The method according to claim 1 , wherein the two-dimensional perovskite pure-phase quantum well material has the chemical formula of A 2 B 2 M 3 X 10 .

8 . The method according to claim 1 , wherein the A is CH 3 (CH 2 ) 3 NH 3 ± , the B is CH 3 NH 3 + , the M is Pb 2+ , and the X is I, the two-dimensional perovskite pure-phase quantum well material prepared has the chemical formula of [CH 3 (CH 2 ) 3 NH 3 ] 2 (CH 3 NH 3 )Pb 2 I 7 , [CH 3 (CH 2 ) 3 NH 3 ] 2 (CH 3 NH 3 ) 2 Pb 3 I 10 , [CH 3 (CH 2 ) 3 NH 3 ] 2 (CH 3 NH 3 ) 3 Pb 4 I 13 , or [CH 3 (CH 2 ) 3 NH 3 ] 2 (CH 3 NH 3 ) 4 Pb 5 I 16 .

Assignees

• Nanjing University Of Technology

Inventors

• Chen Yonghua
• Gu Hao
• Xia Yingdong
• Huang Wei

Classifications

• B05D3/12

  by mechanical means · CPC title

• B05D3/0218

  Pretreatment, e.g. heating the substrate · CPC title

• B05D1/005

  Spin coating · CPC title

• C09K11/664

  Halogenides (C09K11/661 takes precedence) · CPC title

• C07C211/62

  Quaternary ammonium compounds · CPC title