Air strikes on parts of Aleppo and areas to the west held by opposition forces killed at least 32 people on Monday, including 12 people in an attack that hit a convoy of aid trucks, the Syrian Observatory for Human Rights reported.
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The attacks were carried out by either Syrian or Russian aircraft, the Syrian Observatory for Human Rights said, adding that there had been 35 strikes in and around Aleppo since the truce ended.
The Observatory said the aid trucks had made a delivery organized by an international organisation to an area west of Aleppo.
"Our outrage at this attack is enormous ... the convoy was the outcome of a long process of permission and preparations to assist isolated civilians," United Nations Special Envoy for Syria, Staffan de Mistura, said in a statement emailed to Reuters by his spokeswoman in Geneva.
A local resident told Reuters by phone that the trucks were hit by around five missile strikes while parked in a center belonging to the Syrian Red Crescent in the town of Urm al-Kubra, near Aleppo. The head of the center and several others were badly injured.
The monitoring group said it was not clear if the jets were Syrian or Russian. Moscow supports Syrian President Bashar Assad with its air force. The Syrian military could not immediately be reached for comment.
The airstrikes appeared particularly heavy in insurgent-held areas west of Aleppo, near the rebel stronghold of Idlib province. In eastern Aleppo, a resident reached by Reuters said there had been dozens of blasts.
"It started with an hour of extremely fierce bombing," said Besher Hawi, the former spokesman for the opposition's Aleppo city council. "Now I can hear the sound of helicopters overhead. The last two were barrel bombs," he said, the sound of an explosion audible in the background.
Abu al-Baraa al-Hamawi, a rebel commander, said the most intense bombardments had taken in place in areas west of Aleppo, the same area where the aid convoy was hit. "The regime and Russians are taking revenge on all the areas," he said.
The raids came as what is likely to be the final attempt by the administration of U.S. President Barack Obama to find a negotiated solution to the five year old civil war appeared close to collapse.
Secretary of State John Kerry scrambled Monday to try to salvage Syria's fractured week-old truce after the Syrian military announced it was over amid numerous violations and apparent Russian unwillingness to press Damascus on the point.
The State Department said it was prepared to extend the cease-fire window in the hopes that if it held, the U.S. and Russia could then turn to their planned military cooperation against the Islamic State militants and al-Qaida-linked groups in Syria.
The latest developments placed added importance on a meeting Tuesday of the International Syria Support Group, or ISSG, which is comprised of countries with a stake in the conflict and endorsed the truce, to be led by Kerry and Russian Foreign Minister Sergey Lavrov.
"Well, the Syrians didn't make the deal," Kerry told reporters in New York.
"The Russians made the agreement. So we need to see what the Russians say; but the point, the important thing is the Russians need to control (Syrian President Bashar) Assad, who evidently is indiscriminately bombing, including of humanitarian convoys. So let's wait and see, collect the facts. We need to see where we are, and then we'll make a judgment. But we don't have all the facts at this point."
Syria's army said the seven day truce period had ended. It accused "terrorist groups", a term the government uses for all insurgents, of exploiting the calm to rearm while violating the cease-fire 300 times, and vowed to "continue fulfilling its national duties in fighting terrorism in order to bring back security and stability".
Asked about the army's statement, Kerry told reporters in New York that the seven days of calm and aid deliveries envisaged in the truce had not yet taken place.
"It would be good if they didn't talk first to the press but if they talked to the people who are actually negotiating this," Kerry said. "We just began today to see real movement of humanitarian goods, and let's see where we are. We're happy to have a conversation with them."
Aid was delivered to the besieged town of Talbiseh in Homs province on Monday, the Red Cross said, for the first time since July. The convoy brought in food, water and hygiene supplies for up to 84,000 people, it said.
But most aid shipments envisioned under the truce have yet to go in, especially a convoy destined for rebel-held eastern parts of Aleppo, where some 275,000 civilians are believed trapped without access to food or medical supplies.
"I am pained and disappointed that a United Nations convoy has yet to cross into Syria from Turkey, and safely reach eastern Aleppo," the UN Under Secretary General for Humanitarian Affairs Stephen O'Brien said in a statement.
The United Nations said it had received government approval to reach nearly all the besieged and hard-to-reach areas where it sought to bring aid, but access to many areas was still constrained by fighting, insecurity and administrative delays.
Already widely violated since it took effect, the cease-fire came under added strain at the weekend when Russia said jets from the U.S.-led coalition against ISIS killed more than 60 Syrian soldiers in eastern Syria.
Assad called that incident "flagrant aggression" while Washington has called it a mistake.