First registration query

My grandparents purchased their home in 1956. An online search with the land registry has confirmed that no title has been registered. I was advised by email to contact the registry by telephone for advice but I am unable to get through. I am the sole attorney on her LPA and want to register the house with the land registry. I have the original deeds in my grandfathers name. He died in 1974. I also have the original will leaving everything to my grandmother. I would be grateful if someone could advise me of the correct method of achieving this.
Also, my grandmother has entered long term care and the house needed renovating before we could rent it out. I funded the renovation (as an interest free loan to my grandmother) and I have been advised to register this as a charge against the property. could someone offer advice on how I would do this?

John - see our online guidance with regards the first registration 
If you wish to take a legal charge over the property then form CH1 is the prescribed form to use.
I would strongly recommend seeking legal advice/assistance although that maybe the 'advice' you have referred to as having already obtained