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Mayor of London Sadiq Khan should "reflect" on the ULEZ expansion due to the "impact it's having on people", Labour leader Sir Keir Starmer says.
Speaking during a phone-in interview on BBC Radio 5 Live, Sir Keir said he wanted to "see whether there are things that can be done to make it easier for people" who are affected by the scheme.
However, he stressed the law "requires" the mayor to "reduce air pollution".
City Hall has been contacted for comment.
From 29 August, when the ULEZ is set to be expanded to cover the whole of London, drivers of non-compliant vehicles must pay a daily charge of £12.50 to drive within the zone.
Sir Keir's remarks follow Labour's loss in the Uxbridge by-election last week, a result widely seen as being due to the impact of ULEZ.
Answering concerns from a listener called Lorraine, from Hillingdon in west London, Sir Keir said he had spoken to the mayor and his team before and after the Uxbridge by-election and "there are a number of things we discussed".
Sir Keir said the government was refusing to help fund the scrappage scheme - which was recently widened to help more Londoners replace their vehicles - unlike those in other areas of the UK.
"The government has put money behind similar schemes in Birmingham and Bristol but it hasn't put any money into London and I think the government should do that," he said.
"If we make it easier for people to change their car with a proper scrappage scheme, then that massively helps. But the government at the moment won't do it."
Sir Keir also pointed out that the law compelled the mayor to "do something" about cleaner air.
"We can't pretend that this is a simple political decision that you can say 'yes' or 'no' to, and have no regard to the legal content," he said.
"There's a law in place that requires the mayor of London to take measures to reduce air pollution once it gets above a certain level.
"The law is actually driven by the government. If the law requires you to do something, you can't simply do nothing.
"It is not in the gift of the mayor to say 'I'm simply not going to do it'."
A spokesperson for the Department for Transport said: "It's for the mayor of London to justify his decision to expand the ULEZ, and to properly consult to ensure it is not just a tax on the poorest motorists.
"We have provided Transport for London with £6bn to keep public transport moving. Decisions on how to allocate funding to best meet the city's transport priorities are for the mayor of London to make.
"Air quality matters in London are also devolved to the mayor."