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Shipments totalled 274,824 tonnes last month, up from 167,257 tonnes a year earlier.
The month-on-month increase from August this year was even higher, up from 146,213 tonnes, the figures showed.
Of total exports in September, 199,746 tonnes went to the USA, up from 132,160 tonnes in September last year and 101,112 tonnes in August this year.
The Netherlands imported 26,419 tonnes, up from 10,782 tonnes and 3,607 tonnes respectively.
Shipments to Chile and Taiwan came next, at 20,901 tonnes and 15,444 tonnes respectively, according to the figures.
In terms of states, Pará and Maranhão, in Brazil’s northern Carajás region, exported the highest volumes in September.
Pará exported 95,805 tonnes, up from 18,417 tonnes year-on-year, while Maranhão shipped 93,764 tonnes, almost unchanged from the 93,385 tonnes of September 2011.
Exports from Minas Gerais, in Brazil’s south-eastern region, reached 72,597 tonnes, up from 48,455 tonnes.
Between January and September, Brazil’s total pig iron exports reached 2.26 million tonnes, down from 2.64 million tonnes in the same period of 2011.