I am in my second year of teaching and was appointed unpaid ICT co-ordinator after completing my NQT year in a large primary school. Will I be eligible for teacher and learning responsibility (TLR) repayments?

It depends on how your school carries out its staffing review and the state of its budget. There is nothing to prevent you from receiving a TLR-based salary for an appropriate post. If you are responsible for co-ordinating the work of other teachers, you have a case. Preparing teaching materials and the odd training session is not enough.