Officers carried out new raids Wednesday to root out a possible support network for the men, accused of ploughing vehicles into pedestrians on Barcelona's busy Las Ramblas boulevard last Thursday and a seaside promenade in the resort town of Cambrils just hours later, killing 15 including a young boy and wounding more than 120 people.
Barcelona's mayor, Ada Colau, and the head of the regional government Carles Puigdemont were due to participate in an interfaith ceremony Thursday in memory of the victims.
The scale of the assaults being prepared by the jihadist suspects emerged during a preliminary court hearing Tuesday, when Mohamed Houli Chemlal, 21, told the judge the group was planning "an attack on an even greater scale, targeting monuments" using bombs.
After Chemlal's chilling admission, Barcelona authorities said security was being boosted at key tourist sites including the iconic Sangrada Familia church as well as at major events.
At least 500 litres of acetone, large quantities of nails and detonators as well as gas canisters have been found at a house in the town of Alcanar south of Barcelona, court documents said.
But an accidental blast at the bomb factory in Alcanar on August 16, the eve of the Barcelona van attack, forced the cell to alter its plans and turn to vehicles as killing machines.
After losing their bombs and two cell members in the blast that was so powerful that "the mushroom cloud that was generated was visible several kilometres around", the jihadists put plan B into action.
They rented a van the next day, but again suffered a false start as it got into an accident not far from Cambrils.
After a full day court hearing, Chemlal and another suspect, Driss Oukabir, 28, were Tuesday remanded in custody and charged with terror-related offences.
A third man, Mohamed Aallaa, 27, who owns the car used in the Cambrils attack, was granted conditional release as the judge deemed evidence against him weak.
The judge delayed a decision on the fourth suspect, Salh El Karib, whose shop allows people to make calls abroad and was among targets of police raids late Tuesday.
The men in court Tuesday were the only surviving suspected members of the terror cell, which Spanish police said they had dismantled after gunning down the last man at large and the Barcelona van driver, Younes Abouyaaqoub, on Monday.
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