Iran has been urged to return with "realistic proposals" to the talks in Vienna aimed at keeping a nuclear weapon out of its hands.
Germany said the drafts put forward so far by Iranian negotiators, coupled with Iran's continued nuclear endeavours at home, were not a promising basis for an agreement.
It said Iran was turning its back on the progress made during an earlier phase of the talks, which resumed last week after being put on hold in June.
France, meanwhile, said on Tuesday that Iran's proposals were "not a reasonable basis" for an accord.
The Foreign Ministry in Paris said it was disappointing that there had not been more progress on restoring the 2015 nuclear deal.
Diplomats in Vienna hope to revive the deal, which imposed limits on Iran's nuclear activity, but they did not reach a breakthrough in five days of resumed talks.
Tehran stopped complying with the 2015 pact, known as the Joint Comprehensive Plan of Action, after the US withdrew from the deal in 2018 and restored sanctions under then president Donald Trump.
Speaking on Monday, German Foreign Ministry spokeswoman Andrea Sasse criticised Iran for pushing ahead with its domestic nuclear activities despite the resumption of talks.
The International Atomic Energy Agency, the UN's nuclear watchdog, has said Iran is continuing to enrich uranium to 20 per cent using advanced centrifuges in an underground site at Fordow. Iran insists it does not seek nuclear weapons.
"On the one hand, Iran keeps on pursuing its nuclear endeavours in a massive way, and on the other hand we’re trying in Vienna to enable Iran’s return to the JCPOA," Ms Sasse said.
"We have thoroughly and very carefully reviewed these text proposals that were presented in the Vienna talks, and have come to the conclusion that Iran is breaking with almost all of the difficult compromises that were previously agreed upon during several months of hard negotiations.
"In our view, this basis, combined with continued development of Iran’s nuclear programme, is not a basis on which the talks can be brought to a promising conclusion."
Ms Sasse said the three European parties to the deal known as the E3, Germany, Britain and France, were prepared to resume without delay.
But "we also have to say quite realistically that the window of opportunity for such a path is closing more and more," she said.
Iran and the E3 countries held five days of talks with Russia and China, the other parties to the pact, while the US took part indirectly.
The talks broke off on Friday with US Secretary of State Antony Blinken saying Iran did not seem to be serious about a deal. No date has been announced for their resumption.
It was the first round of talks since the election of Iranian President Ebrahim Raisi.