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Indefinite leave to remain does not expire in the same way that visas do - it's simply means that the person has an indefinite right to live and enter the UK. ILR will be stamped in his passport. His passport can expire and assume this is what has happened.
If his passport has expired it does not mean that his ILR terminates. He can simply apply for a new passport then staple his old passport to his new passport and his ILR will continue. Alternatively he can apply for a Transfer of Conditions once he has his news passport so that they stamp ILR in his new passport but this costs as much as apply for ILR in the first place so people tend not to do that.
Is right to apply for UK citizenship does not need to be supported by you I'm afraid he simply needs to meet the eligibility criteria and show that he has lived in the UK throughout the course of his spouse visa and a further 12 months if he applied for ILR as soon as possible.
I'm afraid that you cannot have him deported now (if this is what you hoped to do) because ILR is permanent and is only revoked where it can be proved that it was obtained fraudulently. It would not be in your interests to claim is was obtained fraudulently because you have supported his application and would be view as complicit. You could face criminal charges in these circumstances.
I'm sorry if this is not what you wanted to hear.
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I will answer your follow up questions you may have.
Settlement for spouses runs in this order:-
1. Application for settlement is made by applicant on the basis of their mariage with a UK national
2. Spouse visa granted to applicatoin for a period of 27 months (ie. it expires 27 months after it was granted).
3. 24 months after the initial visa was granted the applicant can apply for indefinate leave to remain only with the support of his wife, who should state they are still married.
4, After ILR has be granted the applicant can then wait a further 12 months so that their total time in the UK is 3 years and then apply for citizenship.
In summary if your husband has not received ILR yet then you can restrict his ability by doing so by advising the UKBA of the breakdown of your marriage. They will curtail his visa so that his leave to remain ceases. You can then advise them if he does not leave and tell them where he is available to be found to deport. It is up to the UKBA to actually deport him though, ultimately it is their decision.
If you do not comply with his request to support his ILR application with your documents then he will not receive ILR.
If he has already received ILR then there is nothing you can do. He will have the right to apply for citizenship.
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