The East Harlem facility is currently processing hundreds of children.
Elected officials, faith-based groups and lawyers representing parents of detained children demanded an end to the Trump administration's "zero-tolerance" immigration policy.
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Among the cases highlighted was that of 32-year-old Hector Tejeda Santos, of Honduras.
Santos and his 14-year-old daughter were granted political asylum in January and were living in Galveston, Texas.
When his 30-year-old wife Denise and the couple's two youngest daughters later arrived at the border in June, they were denied entry.
Denise Santos is being held at the Port Isabel Detention Center in Texas, while 5-year-old Serli and 9-year-old Cecia are in foster care at the Cayuga Centers on East 131 Street.
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Lawyers for Tejeda Santos say federal immigration officials denied his request to travel to New York in an attempt to see his children.
"This is unacceptable," attorney Michael Avenatti said. "This is not our America."
The protests come after more than 2,300 families were separated as a result of the Trump administration's zero tolerance immigration policy.
"It is wrong," said state Assemblyman Michael Blake, of the Bronx. "In every possible aspect, it is wrong."
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