I have encountered the error "Call to Excel Services returned an error" when performing a Scheduled Data Refresh.
This is a rather generic error message. However, we have seen several cases where the Scheduled Data Refresh fails because of Unsupported Features in the workbook.
We have a tool that you can use to remove these Unsupported Features.
Excel Services Compatibility Checker Download Page
First install the "Excel Services Compatibility Checker Add-In". As you can see a tab called "Excel Services" will appear in the ribbon (may need to restart Excel). Now you can remove the Unsupported Features by choosing "Quick Fix". I do suggest creating a copy (back up) of the workbook. After you have removed the Unsupported Features, republish to the PowerPivot Gallery and run a Scheduled Data Refresh.
Excel Services Compatibility Checker Add in - Beta
Other Resources:
Differences between using a workbook in Excel and Excel Services
Excel Services part 12: Unsupported features
Excel Services in SharePoint 2010 Feature Support
Edit a workbook that contains features unsupported by Excel Web App
Again, this is somewhat of a generic message, so this may or may not resolve your issue, but it is definitely worth testing.