Portuguese police want to seize Madeleine's Cuddle Cat again

Among the items they are said to want to seize is their missing daughter Madeleine's Cuddle Cat toy, which was examined by forensic teams in the summer. They have also demanded Mrs McCann's diary.

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The requests suggest officers remain hopeful of bringing charges against the four-year-old's parents.

Police already have photocopies of the diary but these would not be admissable in court.

A police dossier this week revealed the McCanns remain the chief suspects in the case and that they could be charged with accidental homicide, homicide by negligence, hiding their daughter's body or faking her disappearance to cover up her death.

Police yesterday made a formal request for British police to re-interview the seven friends who were on holiday with the McCanns when Madeleine disappeared. They submitted a catalogue of questions they want answered to the judge in Portugal overseeing the case.

They also included the list of items they would like seized. Leaks have previously suggested these would include the diary kept by Mrs McCann, 39.

She was advised by a trauma counsellor to keep a journal and to include the days before Madeleine vanished from a holiday apartment in Praia da Luz on May 3.

Detectives took the diary and photocopied it, then leaked sections to the Portuguese media in which Mrs McCann allegedly wrote that her eldest daughter was hyperactive and said she could not cope.

Officers used the excerpts to suggest the GP could have been sedating her children. Mrs McCann has always denied the claims.

Police were also said to want to seize clothes and other items - including the pink soft toy Cuddle Cat - on which trained sniffer dogs allegedly picked up the "scent of death".

Detectives have long questioned why Mrs McCann was so attached to Cuddle Cat and why, if it was her last link with Madeleine, she allowed it to be washed.

They have suggested the toy was cleaned to destroy any potential DNA evidence, such as blood. Mrs McCann said it had simply become too grubby.

Other items sought by police are thought to include the couple's laptops and private correspondence, Mrs McCann's Bible, in which a passage related to the death of a child was marked, and their phone records.

The formal "letters of appeal" will now be sent from the court in Portimao to the Portuguese justice minister and then on to Home Secretary Jacqui Smith for her approval.

Once granted police will contact the group to arrange interviews. Detectives in Portugal will then consider whether they need to reinterview the McCanns, of Rothley, Leicestershire, and whether they should be charged.

The spokesman for the McCanns, Clarence Mitchell, said: "Kate and Gerry, and their friends particularly, are very keen to talk to the Portuguese police again because they want to be able to clarify any inconsistencies to do with the timeline of events on May 3, or whenever the police put forward."