Santorum swept the southern state of Louisiana with 49 per cent of the vote on Saturday, easily defeating Romney (26.7 per cent), former House speaker Newt Gingrich (15.9 per cent), and Texas congressman Ron Paul (6.1 per cent).
But the comfortable win amounted to a hollow victory as Santorum gained only five more delegates on the day as his main rival Romney, who holds a commanding lead in the race to secure the Republican nomination needed to take on White House incumbent Barack Obama in a November 6 general election.
Santorum, a Catholic and fervent opponent of abortion and gay marriage, has won 11 out of 34 nominating contests so far, largely on the back of strong support from evangelical Christians and the party's most conservative members.
But his stance on hot-button social issues is a worry to the Republican establishment, which thinks such hard-line views could turn-off the independent voters who will ultimately decide the outcome of the general election.
Santorum, however, said the Louisiana win was proof that he is better placed than former Massachusetts governor Romney, labelled a moderate by hard-core elements of the Republican party, to take on Democrat Obama.
"Governor Romney will not be able to pound Barack Obama into the ground with overwhelming negative ads," Santorum told CBS television, alluding to Romney's much better financed campaign team which has spent big on radio and television to overcome rivals in a bitter and tightly fought primary season.
Santorum said Ronald Reagan was the only Republican in the last 100 years who has unseated a Democratic incumbent, Jimmy Carter in 1980, and if the party picked Romney they would be resigning themselves to another defeat.
"We tried before nominating moderates, someone who can appeal to folks in the big cities on the east coast and west coast," Santorum said. "That's not what wins the elections. We're not going to win New York. Him (Romney) doing 10 points better and still losing New York doesn't matter."
The Republican race now exits the South, where Santorum dominated and Romney has so far failed to win a single state, for primaries on April 3 in the more moderate states of Wisconsin and Maryland and the US capital, Washington.
Polls show that Romney has a big lead in Wisconsin, which is bordered by Illinois and Michigan, where he has already won nominating contests.
But Romney has lost big leads before and Santorum has vowed to fight all the way to the Republican convention in August if the frontrunner has not by then won the 1,144 delegates needed to clinch the nomination.
"Barack Obama must be defeated -- period. In the swing states I lead Barack Obama by four points and governor Romney loses by four points," he said.
"We have to have someone who can beat him on the issues and connect with voters," Santorum added, in a dig at Romney's perceived weakness among ordinary Americans, many of whom see the multi-millionaire and former venture capitalist as being out of touch with the concerns of economically hard-pressed families.
Romney, however, currently has an estimated 565 delegates, more than double Santorum's count of 256, according to the leading website Real Clear Politics.
Pressure is high in the Republican Party to rally behind Romney, whose 21 wins include Florida and Ohio -- two key battlegrounds in the general election, but no presidential candidate has yet signalled they intend to drop out.
Veteran Republican Senator Lindsey Graham echoed that mood Sunday, telling CNN that the primary season was all but over.
"Romney will be the nominee," Graham said. "Fiscal and social conservatives will unite and form a bond with libertarians and independents and we'll win the White House if we can run a good fall campaign.
"It won't be easy but I like our chances," he added.
Third-placed candidate Gingrich, who has won two states, has 141 delegates, while Paul, who has not won a single contest, has 66 thanks to the proportional distribution system used in some states.
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