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I've had the same problem lately in that I cannot assign various things from the toolsets tab in the admin section for TinyEditor. This was because I had upgraded the the TinyMCE inside of TinyEditor to the latest version.
For what it's worth, I narrowed the 'problem' down to a specific plugin withing the new TinyMCE. You can upgrade every single folder to the new version of TinyMCE by copying the files over
except for the "\modules\tinyeditor\editor\plugins\advlink" folder. This one is the one that seems to blow up the toolsets tab.
For me, I've simply decided to use the new advlink folder from the latest TinyMCE build anyway and keep the database updated by hand. Remember, the toolsets tab is simply a front end for data that gets stored in the database. If you want, it's fairly simple to just write the strings into the appropriate database fields yourself in order to get it working like you want. The table is 'xoops_tinyeditor_toolsets'. You have a row in this table for each group defined in Xoops. Rows 1 and 2 are associated with Webmasters and Registered Users respectively. You can update the memo fields for the tinyed_row1, tinyed_row2, and tinyed_row3 columns by hand, if necessary, by space separating the names of the plugins you'd like to appear on each row. Remember too that you might also need to include the plugin name in the activeplugs column too in order to get the functionality loaded (and cause the button to actually show up).
But like others here I eagerly anticipate the next release of TinyEditor!