Yea its not about centering the image its more about getting the thumbnail size correct. you can use a hack and do this
in your style sheet find this
.content .portfolio {
background: #fff;
float: left;
margin: 0 2% 40px 0 !important;
overflow: hidden;
padding: 0;
width: 23%;
}
Adjust the width in % to the size that fits (again use firebug to figure this out. Then… add some padding to the left and right to compensate difference shortening the width does. you can do that in % as well.
Otherwise I have read about a plugin or two that will resize your thumbnails.