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To my knowledge she has not openly refused him and how could she, she is the queen but he is the king and her husband, and in their culture she was not going to be standing up to him regularly.
The one instance that comes to mind of refusal or disobedience is more in Hamlet's conversation with his mother when he urges her to go not to Claudius' bed any longer and to not allow him to get from her the gist of their conversation, no matter how much he is affectionate with her or flatters her.
Perhaps it was this conversation and the resolve she has to move forward thanks to the deep guilt that she felt that would allow her to refuse his order.
Of course it could also be simply that Shakespeare decided she ought to die and this was a ironic a way to do it as any!
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