RadGrid GridDateTimeColumnEditor is unable to process data of type TimeSpan if PickerType is set to TimePicker.
As a workaround, a GridTemplateColumn can be used with a TimePicker inside EditTemplate
<telerik:GridTemplateColumn>
<ItemTemplate>
<%# Eval("Field") %>
</ItemTemplate>
<EditItemTemplate>
<telerik:RadTimePicker ID="RadTimePicker1" runat="server" SelectedTime='<%# Bind("Field") %>'></telerik:RadTimePicker>
</EditItemTemplate>
</telerik:GridTemplateColumn>