You cannot encrypt existing unencrypted tablespaces. In addition, you cannot change encrypted tablespaces so that they do not encrypt.
As an alternative, transfer the tables and indexes to other tablespaces. You can use the following SQL commands for this.
ALTER TABLE table_name SET TABLESPACE new_tablespace; ALTER INDEX index_name SET TABLESPACE new_tablespace; ALTER DATABASE database_name SET TABLESPACE new_tablespace;
See
Refer to "SQL Commands" under "Reference" in the PostgreSQL Documentation for information on SQL commands.